Laser-induced Laser -induceddamage damageand andthe the role role of of self-focusing self- focusing M. J. Soileau, FELLOW FELLOW SPIE SPIE M. influence of of selfself-focusing Abstract. We review the influence focusing on the measurement of bulk bulk Florida University of Central Florida in ElectroElectro-Optics Center for Research in Optics and Lasers Orlando, Florida Orlando, Florida 32816 32816 laser-induced-damage optical matematelaserinduced -damage(LID) (LID)thresholds thresholdsinin normally normally transparent optical rials. is experimentally experimentally determined determined by by measuring measuring the the spot spot size size and rials. This role is and polarization dependence of LID LID and and by byobserving observing beam beam distortion distortion in the far field. field. Utilizing these geometry in these techniques, techniques, we we find that by using a tight focusing geometry in which the breakdown breakdown power power is is below below P2, the effects effects of of selfself-focusing focusing can be practically eliminated eliminated ininan anLID LID experiment. experiment.P2 P2isisthe thesoso-called second critical critical called second power for for selfself-focusing, and P2 P2 = 3.77P1, 3.77?^, where P., = cÀ2 cX2 /327T2 n2 , where where cc is is focusing, and where P1 /3272n2, the speed speed of A is the and n2 n2 is the nonlinear of light in vacuum, X the laser wavelength wavelength and accordance with numerical calculations calculations by by J. J. H. H. index of refraction. This is in accordance with numerical Marburger [in Progress Progress in Quantum Quantum Electronics, Electronics, J. J. H. H. Sanders Sanders and and S. S. StenSteneds., Vol. Vol. 4, Part 1, pp. pp. 35-110, Pergamon, Oxford holm, eds., Part 1, 35 -110, Pergamon, Oxford (1975)]. (1975)]. With With this knowledge we determine determine that that damage damage is is only only partially partiallyexplained explainedby by avalanche avalanche and that the initiation initiation of of damage damage is is strongly strongly influenced influencedby by extrinsic extrinsic ionization and processes. LID. processes.We Wetherefore therefore conclude conclude that that we we are measuring extrinsic LID. William E. SPIE William E. Williams, MEMBER SPIE Laser Systems Litton Laser 2787 S. S. Orange Blossom Trail Apopka, Apopka, Florida Florida 32703 32703 Nastaran Mansour Eric MEMBER SPIE SPIE Eric W. W. Van Van Stryland, Stryland, MEMBER University of Central Central Florida Florida Research in in ElectroElectro-Optics Center for Research Optics and Lasers Orlando, Florida Orlando, Florida 32816 Subject terms: terms: laserlaser-induced modification;laserlaser-induced damage; laserSubject induced material material modification; induced damage; induced laser-induced breakdown; avalanche avalanche ionization; breakdown; multiphoton multiphoton absorption; absorption; breakdown; ionization; dielectric breakdown; self-focusing. selffocusing. Optical Engineering 28(10), 28(10), 1133 1133-1144 1989). -1144 (October 1989). CONTENTS 1. Introduction 1. 2. Historical review review 2. Historical 3. 3. Theory 3.1. Self-focusing 3.1. Self -focusing 3.2. Polarization dependence dependence of ofselfself-focusing 3.2. Polarization focusing 4. Experiment Experiment 4. 4.1. Experimental verification verification of Marburger's theory 4.2. Polarization Polarization dependence dependence 4.2. 5. Conclusions from fromthe therole roleofofselfself-focusing inlaserlaser-induced 5. Conclusions focusing in induced damage 5.1. Re-evaluation 5.1. Reevaluation of extrinsic laserinduced damage data laser-induced 5.2. Wavelength, temporal, and spot spot size size dependence dependence 5.2. Wavelength, 6. Controlled defect studies 6. Controlled 7. Conclusion 7. Conclusion 8. Acknowledgments 8. Acknowledgments 9. References 9. References Paper LI LI-112 Invited Paper -112 received received March March 24, 1989; revised manuscript received 1989; revised 1989; accepted June 26, May 5, 1989; accepted for for publication June 26, 1989. 1989. © © 1989 1989Society Societyof ofPhoto-Optical Photo -OpticalInstrumentation Instrumentation Engineers. 1. INTRODUCTION INTRODUCTION 1. In this paper we discuss bulk (as opposed opposed to to surface) surface) laser -inlaser-induced-damage duced- damage (LID) in transparent transparent optical i.e.,i.e., opticalmaterials, materials, materials the input input laser laser wavewavematerials whose whose linear linear absorption absorption at the length is the order of of l0 10~3 or less.1 less. 1 "-3 3 In length is -3 or In anticipation anticipation of our conclusion with few few possible possible exceptions, LID is is influinfluconclusion that, with enced by extrinsic processes, we refer to the damage damage as extrinextrinsic However, sic laser-induced-damage laser- induced -damage(ELID) (ELID) in what follows. However, it is to realize realize that that how how self self-focusing is important important to -focusing affects affects damage damage threshold data data is is independent independent of of the the damage damage mechanism mechanism (i.e., (i.e., intrinsic or extrinsic). By By intrinsic we mean that the threshold is is not not increased by reducing the defect or impurity density. We investigate the the role role of of selfself-focusing focusing in LID LID and how the experimental geometry can alter this role. Misunderstandings Misunderstandings conconcerning self self-focusing -focusing effects effects have have led led researchers researchers to incorrect conclusions concerning the observed parametric parametric dependences of ELID, which in turn affect conclusions of the importance of extrinsic effects of the role of effects in in LID. LID. A clear understanding understanding of self-focusing geomeself -focusingininLID LID allows allows us us to design experimental experimental geometries which such such effects effects can can be be practically practically eliminated. eliminated. tries in which OPTICAL / October 1989 / Vol. 1010 / / 1133 OPTICALENGINEERING ENGINEERING / October 1989 / Vol.2828No. No. Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms SOILEAU, MANSOUR, VAN VAN STRYLAND STRYLAND SOILEAU, WILLIAMS, MANSOUR, DAMAGE IR NO DAMAGE z .x Si02 1.06pm ñX ==1.06ym t p =40ps tp=4Ops x 2234 4 3 IRRADIANCE IRRADIANCE (x1O12 (x1012 W/cm2 W /cm2)) Fig. 1. Method of of LID LID threshold threshold determination. determination.Damage Damage(X (X on on upper Fig. 1. Method line) or no 2. line) no damage damage (X (Xon onlower lower line) line) for for SiO Si02. Parametric Parametric dependencies dependenciesofof ELID ELID thresholds thresholds can can then then be unambiguously unambiguouslycompared comparedwith with predictions predictions of of theory. theory. The The overwhelming overwhelmingevidence evidencefrom fromsuch suchstudies studiespoints points to to the the conconclusion materials isis not clusion that that damage damage in in these these transparent transparent materials not completely explained by avalanche ionizationtheory4,5 theory 4' 5 but avalanche ionization but is is heavily heavily influenced influenced by extrinsic effects. We give evidence supconclusion by porting this this conclusion by presenting presenting ELID ELID data for doped glasses and SiO2 . glasses and gamma-irradiated gamma- irradiated Si02. ELID is is aa threshold threshold-like phenomenon. The The threshold threshold ELID -like phenomenon. 1, which shows behavior is is illustrated illustrated in Fig. 1, shows aa set set of ELID data on aa fused fused silica silica sample sample using using 40 40 ps, data taken on ps, linearly linearly 1.06 /zm size of polarized, 1.06 µm pulses pulses focused focused to a Gaussian spot size approximately 6.8 this paper paper pulsewidths pulsewidths approximately 6.8 ^m. µm. Throughout this and spot spot sizes sizes are are the the HW HW 1l/e2 M in are quoted as FWHM, and /e2M irradiance. The function of of internal internal irradiance. The data data are are plotted plotted as as a function lower line if no damage occurred irradiance with an X on the lower and on the upper line if damage did occur. The threshold is is defined the peak peak-on-axis fluence (J/ (J/cm2 ), irradiance irradiance defined as the -on -axis fluence cm2), (W/cm2), (W /cm2),oror rms rms electric electric field field (V/cm), (V /cm), which which results results in in an irreversible change irreversible change in in the the specimen specimen as as determined determined by one or more of the following: following: an increase in scattering of of aa HeNe HeNe more an increase probe beam (either (either by visual visual observation observation or or photometric photometric probe beam detection), as seen seen in in aa microscope, microscope, detection), a change in morphology as of the sample. sample. In or a permanent change in the transmittance transmittance of most most cases cases this this type type of of damage damage isis obvious obvious and and all all of of the symptoms are are observed. observed. In In addition, addition, ELID in these materials materials symptoms is is usually usually accompanied accompanied by by a visual flash associated with the onset dielectric breakdown (i.e., (i.e., avalanche avalanche ionization). ionization). onset of dielectric These discussed in These data data as as well well as as other other data discussed in this this paper are one-on-one one -on -onemeasurements measurements in inwhich which each each site site isisirradiated irradiated only once once even even ififthe the site site did did not not incur damage. damage. It is observed observed in some preirradiation with with pulses pulses below below the some materials materials that that preirradiation damage threshold threshold as as defined defined can canalter alter the theELID ELID threshold, threshold, the so-called threshold so- calledN-on-one N -on -oneeffect. effect.Note Notethe the very very sharp sharp threshold shown shown in in Fig. Fig. 1, 1, which which isisindicative indicative of ofdamage damage in in transparent transparent thresholdshown shownofofapproximately approximately dielectrics. The threshold 3.33.3XX10 101212 W/cm2 W/ cm2isisabout abouttwo twoorders orders of ofmagnitude magnitude larger than could be expected from the same same sample sample used used as as an an optical optical component component in a system. This isis the the case case since since the failure mode for large in system. This large illuminated areas used in practice is is more likely likely surface damage age where where other other extrinsic extrinsic effects effects cause cause damage. damage. In the experiments ments relevant relevant to to this this paper, surface damage is avoided by Reusing 'ocusing into into the the bulk bulk of of the the material, material, keeping keeping the irradiance itd the damage damage-prone -prone surfaces low. threshold-like The threshold -like behavior behavior illustrated illustrated in Fig. 11 is is indicative extremely nonlinear process. process. Considerable effort tive of an extremely has been spent spent to to monitor monitor subthreshold subthreshold changes in the optical properties of these materials with with little little success. success. A A notable notable properties exception is is the the recent recent work work of Braunlich Bräunlich and coworkers at State University.6 University. 6"-8 8 They Washington State They report report the observation multiphoton absorption absorption of 532 532 nm nm light light inincarefully carefully of multiphoton selected alkali halide samples of as as high high an an order order as as four four prior prior luminescence and to damage using luminescence and the the photoacoustic tech- nique. We comment comment on the the possible possible implications implications of their their nique. We results Sec. 5. 5. No connection connection between between the linear optical optical results in in Sec. properties and the ELID thresholds has has been been found. ExperiExperiments have have also also shown that the transmittance transmittanceof ofaalaser laser pulse pulse is is cut cut off within within aa few few picoseconds picoseconds of of the the initiation of damage damage distortion prior priortotodamage.9 damage. 9This Thishighly highly nonnonwith no pulse distortion linear linear behavior of ELID makes precise determination of the damage mechanism(s) mechanism(s) difficult. fact, we must must infer infer the the damage difficult. In In fact, mechanism(s) mechanism(s) of failure failure from parametric dependences dependences (e.g., (e.g., pulsewidth and wavelength dependence). This has resulted in slow slow progress progress in in developing developing aa complete complete understanding understanding of the physical processes involved in ELID. On On the the other other hand, hand,as as we we shall see see later later in in this this paper, paper, the the first first qualitative qualitative description description of of ELID was was essentially essentially correct) correct. °,) 10 ' 11) 2. HISTORICAL REVIEW 2. HISTORICAL The first first reports reports of of bulk bulk ELID ELIDwere were by The byBruma1° Bruma 10 and and Hercher 11 ininpapers papersatatthe the1964 1964 spring springmeeting meeting of of the the Optical Optical Hercher" Society of America. America. The principal conclusions of these initial reports are as follows: follows: (1) plays no major (1) Linear absorption plays role in this type of of failure. failure. (2) (2) The The damage damage process process isis highly highly nonlinear. (3) Electron avalanche avalanche breakdown breakdown may may be initiated by defects and/or by defects and / or impurities. impurities. (4) (4) The The ELID ELID threshold and morphology depend on on spot spot size. size. While While there there has has been been some some controversy regarding the third statement, data data now now tends to confirm statements made made 25 25 years years ago. ago. Excellent Excellent confirm all all of the statements sources in many many materials materials are are the sources for data on ELID in the proceedproceedings Boulder Damage Damage Conference Conference starting ings of the annual Boulder starting in in 1970 and the references references therein.12 therein. 12 1970 One One can can divide divide much much of the the past results in ELID experiexperiments into two distinct categories. Category Category A A consists consists largely of work conducted at at Harvard HarvardUniversity UniversitybybyBloembergen Bloembergen11 and his his students studentsYablonovitch,13 Yablonovitch, 13-15 " 15 Fradin,16 Fradin, 16 ~-20 20 and and Smith 2' 21 " 23 Smith2,21 -23and andbybytheir theircoworkers. coworkers. The The Category A experiments ments represent a systematic investigation of the breakdown thresholds several alkali halides and fused fused quartz thresholds of several alkali halides quartz over over wavelengths 10.6 jum wavelengths ranging from 10.6 µm to 0.355 ;um µm and for pulse durations ranging ranging from from nanoseconds nanoseconds to totens tensofofpicoseconds. picoseconds. The results were interpreted in in terms terms of of an an intrinsic intrinsic model model of of electron breakdown. 2 The breakdown thresholds thresholds electron avalanche breakdown.2 were sample to to sample sample for for aa given were found found to vary little from sample given material material even if the samples were supplied by different crystal growers. thresholds were were found found to agree agree growers. The The breakdown breakdown thresholds within wavelengths ranging 10.6 µm within ±15% ±15% over wavelengths ranging from from 10.6 jum to to 1.06 jum. that this this agreement agreement in in damage 1.06 µm. It isis important important to note that threshold alkali halides halides was was obtained obtained by by comparing comparing threshold for the alkali damage different focusing focusing conditions damage thresholds thresholds for for different conditions at at the the different pulse durations different wavelengths wavelengths over over aa wide wide range range of pulse durations and focusing conditions. In addition, the Category Category A A workers addition, the found that the frequency dependence of the the breakdown breakdown thresholds of intrinsic intrinsic avalanche olds agreed agreed with with the theory of avalanche ionization ionization over full wavelength wavelength range, although although some some evidence evidence of over the full 22 multiphoton ionization ionization was was observed observed at at 0.355 0.355 µm /xm.22 In part, part, the the agreement agreement of of the the results results of of the the Category Category A A workers with the predicted frequency dependence of of intrinsic electron avalanche breakdown arose from attempts to correct correct the data at 1.064 1.064 µm, Mm, 0.694 µm, jum, 0.532 µm, µm for jum, and 0.355 ^m the presumed effects effects of of self self-focusing. -focusing. For For example, example, Smith Smith et aí.21,22 al. 21 ' 22 scaled scaledthe theresults resultsof of their their picosecond picosecond breakdown work assumption that PI Pj (discussed (discussed in in the next work under under the assumption section) critical power section) was was the the critical power of importance importance for for focused focused Gaussian beams. They observed observed aa slow slow increase increase in in the scaled scaled 1134 / /OPTICAL OPTICALENGINEERING ENGINEERING // October Vol. 28 28 No. No. 10 10 1134 October 1989 1989 // Vol. Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms SELF-FOCUSING OFSELF ROLEOF THEROLE ANDTHE LASER-INDUCED LASER- INDUCED DAMAGE DAMAGE AND -FOCUSING thresholds with increasing frequency, consistent with the prePj is not now know PI We now theory. We dictions of intrinsic avalanche avalanche theory. the critical power of importance importance in those experiments and the conthe coninvalidating the scaled, thus invalidating been scaled, have been should not have data should increasing with increasing decrease with clusions. clusions. The The unsealed unscaled thresholds decrease avaintrinsic avathe intrinsic of the prediction of frequency, opposite frequency, opposite to to the the prediction lanche lanche ionization theory. Category BB workers were of Category results of On the other hand, the results Harvard inconsistent with often found found to to be inconsistent with those those of the Harvard often Olness,24* 25 Yasojima and includeOlness,24,25 workersinclude CategoryBB workers group. Category 28 and Bassand and Barrett Barrett28 and coworkers coworkers at Japan,26' 27 Bass coworkers in Japan,26,27 Manenkov 29 and California, Manenkov29 Southern California, University of Southern the the University Stryland, 32 Van Stryland,32 Soileau, 30' 31 Van Union,Soileau,30,3' Soviet Union, coworkers in the Soviet One of of the the main conclusions conclusions to be drawn from Sparks.4 One and Sparks.4 laser-induced induced breakdown B experiments is that laserthe Category B study is is caused caused by by extrinsic extrinsic properties properties of of the the material. material. In a study Manenkov 29 in reported by Manenkov29 in 1977, 1977,the thebreakdown breakdown irradiance irradiance at NaCl samples varied from sample 100 NaC1 for 100 jum measured for 1.06 1.06 µm in to sample by aa factor factor of 50. 50.The The highest highest thresholds thresholds reported reported in reported previously reported than previously higher than were higher Manenkov's work were Manenkov's work (e.g., three times times those those reported in Ref. Ref. "intrinsic" thresholds (e.g., Soileau 30' 31 and by Soileau3°,31 seen by 13). Similar Similar results results have and in been seen have been 13). no Yasojima. 27 In Olness 25 and earlier studies by Olness25 and Yasojima.27 In addition, no funcas aa functhresholds as systematic variation in the breakdown thresholds systematic variation results of the results observed in was observed bandgap was material bandgap tion of material tion in the A 26' 27 inincontrast Olness24,25 andYasojima Yasojima26,27 contrasttoto the the Category A Olness 24' 25 and measurements. A decrease decrease in in the the breakdown threshold with measurements. A al. 30' 31 in Soileauetetal.3o,31 bySoileau seenby was seen wavelength was decreasing laser wavelength 10.6 /xm halides over wavelengths the alkali halides wavelengths ranging ranging from 10.6 µm to Smith of Smith 1.06 µm, as as was wasobserved observed for for the the unsealed unscaled thresholds of 1.06 /zm, et aí.21,22 Again,this thisisisopposite oppositetoto the the trend trend predicted by al. 21 ' 22 Again, in Cateresults in Finally, results intrinsic avalanche ionization theory. Finally, size spot size gory B B experiments indicate the presence of a strong spot dependence for the the breakdown field in the alkali halides halides and be could not be materials that fused quartz as as well well as as other other materials that could fused quartz self-focusing explained by selffocusingand and isis inconsistent inconsistent with intrinsic damage measured damage Also, the measured avalanche breakdown theory. theory. Also, avalanche breakdown materials in materials even in sample even to sample thresholds differed from sample to from the same manufacturer. Much of the the controversy controversy found found in the literature is due to Much account differences in the differences in the ways ways in in which which various authors account the in the Early in self-focusing. for,self accountfor, attempt totoaccount or attempt for, or -focusing. Early self-focusing ELID, selfof ELID, focusing was recognized as history of studies of irreversible catastrophic, irreversible to catastrophic, contributors to major contributors one one of the major properties. 12 Over the years many studies, changes in material material properties.12 in conducted in been conducted have been experimental, have both theoretical theoretical and experimental, damage self-focusing forself attempts to -focusing effects in bulk damage accountfor to account problem, of the problem, complexity of experiments. However, due to the complexity mixed. been mixed. has been experiment has agreement between theory and experiment agreement between While accurate, accurate, direct measurements of the nonlinear nonlinear index of n2 , have refraction, n2, have been been made made using various techniques (e.g., interferometry33,34), thepower power for for which significant changes 33' 34), the interferometry beams Gaussian beams focused Gaussian offocused propagation of occur occur in the linear propagation estabbeen estabrecently been only recently through nonlinear materials has only nonlinear materials through lished Wepresent presentsome someof of that that work in experimentally. 35' 36 We lished experimentally.35,36 follows. what follows. THEORY 3. THEORY Self-focusing 3.1. Self -focusing results dielectric results transparent dielectric in a highly transparent Nonlinear refraction in by given by refraction given of refraction from a change in the index of (1) (1) n2 <E2> An On = n2 <E2> , field electric field theelectric squareofofthe time-averaged thetime where <E2> -averaged square <E2 >isisthe where assume we assume Here, we n2 isis the and n2 the nonlinear nonlinear index of refraction. Here, less than the much less time much response time has aa response nonlinearity has that the nonlinearity index expressing the index of expressing way of alternative way pulse pulse duration. An alternative 7!, recently isis An come into common use recently change that that has come On == yI, change theirradiance irradiance and and 7 y is aa nonlinear nonlinear index coefficient. coefficient. where II isisthe n2 (esu) with 33 n2 constantwith33 by aa constant related by These coefficients are related (esu) =_ light in vacuum cn /407r7(m2 y(m2/ W),where whereccisisthe the speed speed of light /W), cn/40?r mechaMany mecharefraction. Many of refraction. index of linear index (m/ s) s) and and n is the linear self-focusing focusing effects effects in in solids. solids. For tight nisms can give rise to selffocusing geometries using using nanosecond nanosecond and longer pulse duraelecthe elecself-focusing, thermal self tions, electrostriction, -focusing, and the electrostriction, thermal tions, self-focus. catastrophicselfto aa catastrophic Kerr effect can all contribute contribute to focus. tronic Kerr mechanism in dominant mechanism pulse durations the dominant For picosecond pulse effect. Kerreffect. electronic Kerr the electronic be the to be believed to solids isis believed transparent transparent solids volume of work work has been devoted devoted to the study of large volume A large 12 The self -focusingeffects effectsinin solids. solids.12 The theories theories developed developed to to self-focusing self-focusing thatself indicate that describe describe the process indicate -focusing is dependent critical Two critical material. Two the material. in the laser beam in on the power of the laser for literature for the literature cited in the often cited powers of of importance importance are are often powers by 37 given by37 Pj,isisgiven these,P1, ofthese, first of The first Gaussian beams. The Pl = cA2 cx2 (2) (2) 327r2n2 where X the laser laser wavelength. wavelength. Many theories based on the X isis the cataassumed that have assumed approximation have shape approximation constant that a cataconstant shape strophic collapse of the beam will occur in the material when introduced was first introduced idea was This idea P,. This approachesP1. the beam power approaches by Zverev and Pashkov,38 Pashkov,38 who suggested the following equaself-focusing: duetotoself enhancementdue irradianceenhancement the irradiance for the tion for -focusing: In I0 ISF 1SF (3) ~ I-P/P, I - P/PI self-focuspresenceofofselfthepresence inthe where ISF the peak peak irradiance irradiance in focusISF isis the self-focusing. absenceofofself theabsence in the the peak peak irradiance irradiance in -focusing. I0 isisthe ing and I0 to "scale" researchers to by researchers used by subsequentlyused was subsequently equation was This equation self-focuseffectsofofselftheeffects forthe "correct" for and "correct" damage focusdamage data and give the following 16,21,22 Equation ing.'6.21,22 Equation(3) (3)can canbe be rearranged rearranged to give ing equation: 1 P 1 (1 1 ID \A + PI (4) self-focusing. absenceofofselftheabsence in the area in where A is is the the focal beam area focusing. inverse area, versus inverse damage, versus for damage, power for inverse power of inverse plot of Thus, aa plot Thus, critical the critical yield both the expected to yield size squared, was expected or spot size self-focusing power for self -focusingPj P1asasthe the intercept intercept and and the damage slope. A critical assumption made in ID from irradiance ID from the slope. indepenirradiance isis independamage irradiance the damage using this this equation is that the using self-focusing. absenceofofself theabsence in the -focusing. We find this area in of focal area dent of 5.2. Sec. 5.2. in Sec. discussed in as discussed assumption invalid as soluexact solustudies, exact self-focusing earlierself theearlier to the contrast to In contrast -focusing studies, Marburger 37 byMarburger37 made by equation made wave equation nonlinear wave tions of the nonlinear devisignificant devigeometries, significant have shown that even for focused geometries, occur until the ations from normal linear propagation do not occur the of the collapse of catastrophic collapse power exceeds beam beam power exceeds P, PI and aa catastrophic beam within the depth of focus does not occur until the beam / Vol. 1989 / October OPTICAL ENGINEERING / October 1989 / Vol.2828No. No.1010/ / 1135 OPTICAL ENGINEERING Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms SOILEAU, WILLIAMS, MANSOUR, MANSOUR, VAN VAN STRYLAND STRYLAND SOILEAU, TABLE I.I. Comparison Comparison of of the the constant constant shape shape approximation approximation (CSA) (CSA) to to numerical solutions37 solutions 37 (NS) focused Gaussian Gaussian beams. beams. numerical (NS) for focused P/P2 P/P2 l/lo In, CSA l/lo Ino 0.27 0.27 0.60 0.60 0.80 0.80 0.90 0.90 0.95 0.95 0.96 0.96 0.97 0.97 0.98 0.98 0.99 1.37 2.50 5.00 5.00 10.00 20.00 20.00 25.00 33.30 33.30 50.00 100.00 1.30 2.08 2.08 3.94 3.94 7.15 16.45 28.60 63.40 100.00 192.00 NS NS power P2 . P2 P2 is defined as power exceeds exceeds the the second second critical power P2. (for Gaussian beams) P2 3.77P, P2 == 3.77P1 . (5) The factor of 3.77 3.77 in Eq. (5) comes from numerical numerical solusolutions of the input beam beam with a the nonlinear nonlinear wave equation equation for an input spatial profile. profile. The The power powerP2 P2 is the least power for a Gaussian spatial singular self self-focus -focusto tooccur occurwithin within the the Rayleigh Rayleigh range, i.e., i.e., the beam confocal parameter, parameter, for both prefocused and unfocused geometries. samples thicker geometries.This Thismeans meansthat that for for samples thicker than than the Rayleigh range is the case case for for most most bulk bulklaserlaser-induced Rayleigh range (as (as is induced damage experiments) a singular singular self self-focus -focus will will occur occur within the sample, and LID LID will occur for an input input power power equal equal to to P2. P2 . Note that for for tightly tightly focused focused beams, beams, i.e., i.e., very very small spot sizes, the breakdown field will will be reached before PP approaches approachesP2. P2 . 1f If breakdown field that is the case, case, then then LID LID results can be be nearly nearly independent of self-focusing size needed needed will will self -focusingeffects. effects.The Thesmall smallfocal focal spot spot size depend material, P2, P2 , and the the material material breakdown breakdown depend on on the the material, threshold. Marburger 37 found Marburger37 found that that the the irradiance irradiance enhancement within the nonlinear material was given approximately by by Indeed, Eq. (5) can be be "verified" (i.e., we we show that P2 P2 is is the critical power of importance) as as shown shown in in Sec. Sec. 4. Additional evidence for high P2 P2 materials materials is given by by measurements measurements of the polarization dependence of the breakdown powers powers and meameasurements distortions in in the the transmitted, transmitted,time time-intesurements of beam distortions -intespatial beam beam profile profile discussed discussed in in Sec. Sec. 4. 4. grated spatial Polarizationdependence dependenceofofself self-focusing 3.2. Polarization -focusing The use of short pulses presents presents us us with the advantage advantage that that we we need only consider the fast fast electronic electronic Kerr Kerr nonlinearity nonlinearity in need in analysis. This This nonlinearity nonlinearity isis polarization polarization dependent, data analysis. dependent, polarization dependence dependence presents presents us us with with aa simple simple and this polarization way of determining whether whether or ornot notself self-focusing effects are -focusing effects measurements. present in LID measurements. Early papers in the the literature literature have shown shown that that the the nonlinear nonlinear isotropic materials materials (such (such as as fused refractive index for isotropic fused quartz) quartz) is given givenbyby39-41 39~41 is n2 n2 (L.P.) (L.P.) = n2 (C.P.) n2 (C.P.) = II~P/P2 - P0P2 (6) which P2 /4. which isis only only valid valid for for PP < < P2/ 4. Note Note that this is identical to Eq. (3) with with P1 Pj replaced replaced by P2 . When power is is Eq. (3) by P2. When the the input power significantly /4 one significantlygreater greaterthan than P2 P2/4 one must must use use the the more more comcomplete plete numerical numerical solution solution to compute the enhanced irradiance due self-focusing. due to self -focusing.Table TableI Iisisaacomparison comparison of of the the approxiapproximation exact numerical numerical solution solution mation given given by by Eq. Eq. (6) (6) and and the exact given while the given by by Marburger Marburger (see (see Ref. Ref. 37, 37, p. p. 66). 66). Note Note that while enhancement cannot cannot be be calculated calculated accurately accuratelyby by Eq. Eq. (6) (6) for P > P2/4, P2 /4, itit still still correctly predicts breakdown breakdown at at aa power power of of P2. P2 . In 1977 1977 Smith et aí.22 al. 22 also in using using P1 Pj alsofound found some problem problem in for correcting their 532 nm and 355 nm picosecond damage thresholds for selfself-focusing. focusing.In Inmost mostcases, cases,their their 355 355nm nmthreshthresholds were were higher higher than than Pj. P1. A A scaling scaling factor factor was was proposed proposed such that the critical power varied between between P1 P l and P2 depending on the value value of of PP at at damage. damage. However, However, since sincethe theexact exactfunctional functional dependence time, dependence for for the the intensification intensification was was unknown at the time, the thresholds thresholds reported in Ref. 22 22 included included the breakdown breakdown power power and and the the uncorrected uncorrected focal focal area area so so that that future workers workers could could re-examine re- examinethe thedata data in in the the light light of new new measurements. measurements. We We re-examine re- examinethat that data data in Sec. 5.1. We evidence showing We previously previously presented presented experimental evidence that, as predicted predicted by Marburger, the important important power power for for that, as by Marburger, focused geometries geometries is is the thesecond secondcritical criticalpower, power, P2 . 35' 37 focused /32.35,37 n ,(3) Xiiii Xi31 i1 (7) (7) 247T 247 3 v (3) X1122 122 X1) for linearly polarized and circularly circularly polarized polarized light, light, respecrespectively, where the the X(32¡ x^Vi are arethird-order third -ordernonlinear nonlinear susceptibility tensor elements. A symmetry symmetry relation relation exists exists for for isotropic isotropic tensor elements. materials such that (3) _ > ) (3) Xllll ~= Z XH22 + X1221 X1(311)1 2X1(3122 (8) Measured values values for these tensor elements elements indicate that for for Measured fused quartz quartzX1(3122 Xm2 ls isapproximately equaltotoX1221.41 Xi22i-41 Thus, fused approximately equal Thus, we we can express n2 n2 (C.P.) in in terms terms of ofthe thesame samex(3) x^ tensor tensor element element as n2 n2 (L.P.), giving giving Io ISF 127T 12 7r n2 (C.P.) = 87T X1 (9) We see of n2 n2 for circular polarization to to n2 n2 for We see that that the ratio of linear polarization is 2/3. This This implies implies that the the 9ratio 9ratio of the critical powers for for self self-focusing two cases cases isis 1.5. 1.5. -focusing for the two slightly more more complicated complicatedanalysis analysisfor forNaC1 NaCl A similar but slightly gives the critical critical powers powers that thatvaries variesbetween between 1.37 1.37 gives aa ratio for the 1.46 depending and 1.46 depending on on the propagation direction in the cubic orientationof ofthe the large large grain size crystal. We do not know the orientation crystalline samples and, therefore, expect expect aa ratio ratio between between the the above values near 1.4. 1.4. If we we extend extend this this concept to measurements of bulk optical breakdown and ifif self self-focusing breakdown breakdown -focusing dominates dominates the breakdown process, then, in both the isotropic isotropic and and cubic cubic cases, cases, the ratios the breakdown breakdown powers powers for the the two two polarization polarization states states of the should be equal to the ratio ratio of of the the critical critical powers powers (i.e., (i.e., 1.5 1.5 for SiO2 and-1.4 forNaC1). NaCl). Si02 and =1.4 for The polarization polarization dependence dependenceof ofself self-focusing -focusing has already been well well established established experimentally. experimentally. For example, Moran et al. 34 measured aí.34 measured n2 n2for forvarious variouslaser laserglasses glasses(isotropic (isotropic materials) materials) using time-resolved and found foundthat thatn2 n2 (L.P.) (L.P.) --time -resolved interferometry interferometry and 1.5n2 al. 42 measured 1.5n2(C.P.). (C.P.). Feldman Feldman et aí.42 measured the the breakdown breakdown powers function of polarization for fused fused quartz and other ers as as a function glasses at 1.06 1.06 µm. jum. He used glasses using using nanosecond nanosecond pulse durations durations at used the observed observed polarization dependence in an attempt attempt to to sepasepa- 1136 OPTICALENGINEERING ENGINEERING // October Vol. 28 No. No. 10 1136 / /OPTICAL October 1989 1989 // Vol. Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms SELF-FOCUSING OFSELF ROLEOF THEROLE ANDTHE LASER-INDUCED LASERINDUCED DAMAGE DAMAGE AND -FOCUSING beam using beam measured using as measured n2 as indexn2 refractiveindex TABLE II. The nonlinear refractive 43 compared distortion distortion43 comparedwith with other methods. MATERIAL MATERIAL 10" esu) (x 1013 n2 (Others) 10" esu) (x 1013 1.06 0.53 0.53 128130 128 ±30 + 30*5 125 125 ± 3045 NaCI 1.06 0.53 0.30 1.37 +±0.30 1.37 + 0.30 1.38 1.38±0.30 33 1.22 1.22 ±0.21 ±0.2133 1.5957 1.5957 Si02 Si02 1.06 0.53 0.62 0.62±+ 0.15 + 0.15 0.60 0.60±0.15 0.95 + 0.10 33 0.95±0.1033 BK-7 BK-7 1.06 0.53 0.53 1.45 + 0.30 1.45± 1.01+0.25 1.01 ±0.25 1.46 1.46 + ± 0.10« 0.1046 1.3047 1.3047 CS2 CS2 N a CI WAVELENGTH ^m µm n2 other P2 with using P2 method using LID method Comparison of TABLE TABLE III. Ill. Comparison of the the LID with other CS2 . in CS2. n2 in measuring n2 methods of measuring METHOD METHOD Equation 55 Equation Equation 5 Equation Beam Beam Distortion Distortion Beam Beam Distortion Interferometry 123 + 30 123±30 \0irn) x(um) 10" esu) n2 n2 (x (x 1011 1.06 1.06 0.53 0.53 1.06 1.06 0.53 1.32 0.3 48 1.3 +±0.34a 1.3 48 1.210.3 1.2 ±0.346 0.3 43 1.5 +±0.343 1.5 0.343 1.5 1.5±+ 0.343 1.3 + 0.345 1.3±0.345 -H- 0.8547 0.8547 1.5 T X =0.53µm 1.4r r -30 ps 'BC n2 and was the first to point to n2 rate the various various contributions to self-focusing -focusingininbreakdown breakdown out that the presence or absence of self measurements measurements could could be be determined determined by by measuring measuring the the breakbreakWe use down threshold threshold power power as as aa function of polarization. We conthe condetermine the to determine this concept in our own measurements to self-focusing. of selftribution of focusing. The The data data presented in Sec. 4.2 on NaCI clearly fused quartz and NaC1 fused clearly show show the the transition transition from from an self-focusing which self in which experimental geometry in -focusing dominates dominates the be can be self-focusing whichselfgeometryininwhich damage process to aa geometry focusing can neglected. neglected. In In the the next next section section we wefirst firstverify verifyMarburger's Marburger's theory theory by by monitoring monitoring breakdown breakdown in CS2 CS2 at at 1.06 1.06 p,m um and 0.53 0.53 /zm. µm. EXPERIMENT 4. EXPERIMENT Experimental verification of Marburger's theory 4.1. Experimental 4.1. 37 that Marburger's Marburger's prediction prediction37 that breakdown breakdown will will occur occur at at an P2 given input power P2 given by by Eq. Eq. (5) (5) in a tight focusing geometry which the experiment in verified by can can be be verified by arranging arranging an an experiment in which the P2 is very low. A classic threshold isis very high and P2 breakdown threshold CS2 . This material is example example of such such aa material material is the liquid CS2. nonsince its nonstudies since system studies excellent choice an an excellent choice for for model system is relatively well for years and is well linear behavior has been studied for understood. The nonlinearity isis due dueto tononresonant nonresonant reorientareorientaCS2 molecules, tion of the CS2 molecules, which which relaxes relaxes with with aa time time constant constant n2 in measure n2 of of approximately approximately 22 ps. ps. The The first first step step is is to measure in aa meamanner independent induced breakdown mealaser-induced the laserindependent of the manner surements. surements. Table Table IIII isis aa summary summary of such such measurements measurements for for CS2and andother othermaterials materials of of interest interest using usingthe the beam beamdistortion distortion CS2 other obtained by other Values obtained technique described technique described in in Ref. Ref. 43. 43. Values comparifor comparilisted for workers using workers using various various techniques techniques are are listed \yith son.33,44-47 son.33,44-47 Withthe thepossible possibleexception exceptionof of SiO2 Si02 (a (a 30% 30% differdifferIt isis excellent. It is excellent. methods is agreement with ence) the ence) the agreement with other methods important to note note that the observation of beam beam distortion in in the far far field field as asreported reported in in Ref. Ref. 43 43 isisperformed performedatat irradiance irradiance levels levelsnot not far far below below damage, damage, and and the the agreement agreement with with other other powers. input powers. high input for high analysis for data confirms the propagation propagation analysis CS2 , i.e., in CS2, experiment in We We next next set set up up aa bulk bulk breakdown breakdown experiment arranged the sample length to be much longer than the confopower.48 breakdownpower.48 the breakdown measured the cal cal beam beam parameter, and measured 0.53 and 0.53 ^m and 1.06 pm n2 at both 1.06 We We then then used used Eq. Eq. (5) (5) to to calculate n2 /zm pm and compared this with values obtained by beam distorinterferometry.45 time-integrated measurements 44 and time tion measurements44 -integrated interferometry.45 The results of this this comparison comparison are shown in Table III. In this experiment laser-induced laser- inducedbreakdown breakdown isistotally totally dominated dominated by by self-focusing self -focusingand andthe thebreakdown breakdown power power was experimentally conditions. focusing conditions. the focusing of the independent of determined to determined to be independent n2 determined between the n2 Note the excellent agreement between determined from assumes measurements using Eq. (5), which assumes the the breakdown measurements pB 1.3 11 1.1 1.1 1.0 _ 10 i 15 20 2s 30 W6I/ rol PB for to PB light to polarized light circularlypolarized for circularly PB for ofPB ratioof theratio ofthe plotof Fig. 2. Fig. 2. AA plot for (sample SiO 2(sample size inin Si02 spotsize of spot as a function of polarized light as linearly polarized self-FQ-7940-1). 7979 -F0.7940 -1). The Thedashed dashed line linerepresents represents the the expected expected ratio when when self focusing dominates. beam by beam determined by those determined that P2 is is the critical power, and those 3.77 of 3.77 factor of the factor verifies that the This verifies measurements. This distortion measurements. predicted by the theory in Ref. 37 is is correct correct to within the error error bars shown. self-focuswhenselfdeterminedwhen experimentally determined We We have also experimentally focusobserving by observing experiments by ing isis present present in bulk breakdown experiments ing discussed in the as discussed dependence of damage as the the polarization dependence following section. 4.2. Polarization dependence 4.2. for power for breakdown power the breakdown of the ratio of Figure Figure 22 isis aa plot of the ratio linear polarfor linear power for breakdownpower the breakdown to the circular polarization polarization to in measured in radius measured spot radius focal spot the focal of the function of ization ization as as a function is wavelength is laser wavelength 35 ' 36 The air. air.35,36 Thematerial materialisisfused fusedquartz, quartz, the laser regions of ps. Three regions 30 ps. 0.53 0.53 jum, µm, and and the pulse duration isis 30 small and small small focal radii and evident. For small clearly evident. interest are clearly interest is approxiPBcirCuiar/ pBiinear ratio PBcircular/ breakdown breakdown powers powers the the ratio PBlinear iS self-focusing electronicself lackofofelectronic thelack indicatingthe mately unity, indicating -focusing as as 23 jum discussed discussed in in Sec. Sec. 3.2. 3.2. For For focal focal radii radii greater greater than 23 µm and levels off to near the theoratio levels large breakdown powers the ratio self-focusing. dominanceofofself the dominance indicating the 1.5 indicating retical value of 1.5 -focusing. increasing from unity to data increasing The transition regime regime shows the data Thejransition elecof eleconset of the onset showing the clearly showing maximum, clearly the theoretical maximum, self-focusing tronic self -focusing in in fused fused quartz. quartz. critical powers the critical of the ratioof the ratio at the looking at than looking Now, rather than we we examine examine the the behavior behavior of the breakdown breakdown powers directly in power in megawatts is plotted as Fig. 3. 3. Here, the breakdown power as repretriangles repreThe triangles air. The in air. radius in a function of the focal spot radius the sent the breakdown powers for linear polarization, and the sent polarization. powers for circular polarization. circles circles are are the the breakdown powers P2 for the critical power P2 represents the line represents dashed line The horizontal horizontal dashed n2 values for measuredn2 ourmeasured fromour calculatedfrom linear polarization polarization calculated sample. 43 As this sample.43 Ascan canbe beseen, seen,the thebreakdown breakdown power for linear then focal radius and then increases with increasing focal polarization increases the where the region where the region In the radii. In focal radii. larger focal P2 for reaches P2 for larger OPTICAL ENGINEERING OPTICAL ENGINEERING/ /October October1989 1989// Vol. Vol. 28 28 No. No. 10 10 // 1137 1 137 Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms STRYLAND SOILEAU, WILLIAMS, WILLIAMS, MANSOUR, VAN VAN STRYLAND SOILEAU, 3.0 3 '-PBc 2.5 2.5 PB r T I i 1 T * ' PBL L P. --P2 for for L.P. -P2 i /urn A- 0.53 0.53pm 2.0 20 IMWI |MW| I rri_______ I t P~ 1.5 1.5 -P2 _____ ________I P *• |s PB PB IMWI NW! 1.5 P2 - 1.5 1.00 l r LhWM Polarization Polarization Linear 66 I-- L 2" I—— PB Pg 1MW] IMW) 44 P2 P2 I 22 J I 05 05 00 I * À = 1.06µm r =42ps 68 I 10 1.0 I-" I- IU 10 2.5 2.5 2.0 20 r- 30 ps PS r-30 PB 30 3.0 I 05 0.5 00 I 11 _r 1 1 I 1I I1 5 10 15 20 25 Wolµml 1 T 00 *A * 0 1 50 | 1 100 150 ioof 200 200 Zp=L 30 OJol/im) Wolµml ZR t 71: t versus spot breakdown power versus the breakdown plot of the spot size size for for the the Fig. 3. A plot circular polarization, circles -circular sampleof of Fig. Fig. 22 (triangleslinear polarization, (triangles linear sample meapolarization). The The dashed dashed line line gives gives P2 P2 as ascalculated calculated from from the meapolarization). ru ofn2.43 "2- ~ value of sured value in. foraa22 in. NaCIfor sizeininNaCI spotsize functionofofspot as aa function Fig. 4. Breakdown poweras Breakdown power (X). The horizontal sample (X). thick sample and aa 11 in. thick (triangles) and thick sample (triangles) thick sample dotted n2 , 43 and fromn2,43 P2 as dashed line gives P2 as calculated from and the the vertical vertical dotted focused the focused of the range of Rayleigh range the Rayleigh size at which the line gives the spot size sample. in. sample. beam equals the the sample sample thickness thickness for for the 2 in. beam equals breakdown power becomes becomes constant, constant, the polarization ratio is seen for fused quartz at are seen results are Similar results approximately 1.5. Similar approximately 1.5. self-focusing thatself indicate that 1.06 nm. pm. Both Both of the these trends indicate -focusing 1.06 breakdown the breakdown when the process when breakdown process dominates the breakdown dominates the P2 . approaches P2. power approaches for observed for are observed SiO2 are seen for Si02 those seen Results similar to to those Results similar NaCl. 0.53 i^m pm for 30 30 ps ps pulses pulses and and small small focal focal radii and NaCI. At 0.53 approxitherefore, small breakdown breakdown powers, powers, the the ratio isis approxitherefore, small self-focuselectronicselfofelectronic lack of the lack mately unity. This indicates the focuspowers ing, whereas whereas for for large large focal focal radii radii and and large breakdown breakdown powers levels off the ratio levels off near near the the mean mean theoretical theoretical value of approxapproxself-focusing imately 1.4. focusing dominates dominates the break1.4. In this region selfbreakdown the breakdown where the region where down process. process. Again, Again, in in the region down powers remain constant with increasing spot size, the ratio of powers remain Similar 1.4. Similar reaches approximately 1.4. powers reaches the breakdown powers discuss We discuss pm. We 1.06 pm. sample at 1.06 seen for this sample results are also also seen results are below. significance below. their significance some those measurements and their some of those this point we we remind remind the the reader reader of the definition of the At this Mar-of Mar more of self-focusing critical power power for selffocusing and and discuss discuss more critical 37 P2P2isisthe burger's results. results.37 theleast leastpower power for for which which aa cataburger's unfocused strophic collapse collapse will will occur occur for for both focused and unfocused does on-axis maximum on geometries. The The point of maximum -axis irradiance does geometries. waist; it occurs "downstream" "downstream" of the occur at the beam waist; not occur waist at at aa distance distance comparable comparable to the Rayleigh range in beam waist P2.. If If the the sample sample thickness thickness isisthinner thinner than than the material for P = P2 range, insufficient insufficient nonlinear nonlinear material material exists exists for for Rayleigh range, the Rayleigh selffocusingtotocause causeaacatastrophic catastrophic collapse collapse of of the the beam beam to self-focusing self-byself dominatedby damage dominated For damage P2 . For occur in the material at P2. occur in focusing, this this means meansthat that the the material material will will not not fail fail until until the focusing, seen in be seen can be P2.. This This type of behavior behavior can beam power exceeds P2 the data presented in Fig. 4. Here we have plotted the breakspot focal spot down power power in in megawatts megawattsasas aa function function of of the the focal down 1.06 wavelengthisis 1.06 laser wavelength NaCI sample. The laser radius in air for the NaC1 is 42 pm, 42 ps. ps. The The horizontal dashed line jum, and the pulsewidth is n2 measured n2 P2 calculated from measured represents the critical power P2 represents line II). 43 The this sample (see Table Table II).43 The vertical vertical dotted line values of this divides the the data data for which which the the sample sample thickness is is less less than than the the divides which the Rayleigh range (region (regiontoto the the right) right) from from that in which Rayleigh range left). the left). to the sample isis thicker thicker than than the Rayleigh range (region to Let us first first examine examineonly onlythe thetriangular triangular data data points that are for sample thickness thickness of 22 in. in. If Ifwe weexamine examinethe thedata data for for the the a NaCI sample left, we we see seethat that the the breakdown breakdown power increases region to the left, However, P2 . However, with increasing increasing focal focal radius radius to to approximately P2. with focus of focus depth of when the sample becomes shorter shorter than than the depth sample becomes when the to continues to power continues breakdown power the breakdown (region to the right), right), the (region to increase. If we we now now rotate rotate the sample so so that that the beam propapropadramatic in., aa dramatic gates through through 11 in. in. of material instead of 2 in., gates by seen by This isis seen observed. This powerisis observed. breakdown power increase in the breakdown The size. The spot size. ^tm spot 150 pm examiningthe the data data points points for for the 150 examining for a sample thickness of 22 in., point isis for triangular point in., and and the the point point triangular other No other material. No of material. in. of for 11 in. is for representedby by the the XX is represented the change in the that the show that To show have been changed. To parameters have parameters effect a orientation effect breakdown power power was was not not due due to to an orientation breakdown in which the sample was case in for aa case was performed for similar test was for 11 in. of material. range for Rayleigh range the Rayleigh with the thick compared with when the observed when was observed power was No change change in in the breakdown power No effects was rotated. rotated. This simple test clearly shows the effects sample was self -focusingininbreakdown breakdown measurements. of self-focusing SELF-OFSELF ROLEOF THEROLE FROM THE 5. CONCLUSIONS CONCLUSIONS FROM 5. FOCUSING IN LID Re-evaluation 5.1. evaluation of of ELID ELID data 5.1. Resignificance of of this this work work should should be be emphasized. emphasized. Much Much of of The significance scaling self-focusing onself work on -focusing used the scaling experimental work the early experimental self-forself datafor the data correct the al. 38 to correct et al.38 Zverev et by Zverev law proposed by law was critical power of importance was focusing. In In that work the critical focusing. laser-induced of the laserP,.. Spot be PI Spot size dependencies of induced assumed to be reflection of of damage thresholds were assumed to be merely a reflection in were in powers were self -focusing since since the the breakdown breakdown powers the effect of self-focusing self-focustheselfsincethe However,since of P l. . However, focusmost cases a fair fraction UPI critical the critical confirms that the ing theory theory predicts predicts and and this work confirms ing size dependencies are in spot size fact P2 P2and and not not Pj, PI, the spot power is in fact possibly material, possibly the material, in the mechanisms in cases due to other mechanisms most cases defects to the LID thresholds. Work that the contribution of defects re-examined. beretobe needs to al. needs et al. Zverev et used the method of examined. of Zverev used and Zverev and the Zverev using the work using Unfortunately, much much of the work Unfortunately, since literature since Pashkov38 scaling isis not not recoverable recoverable from the literature 38 scaling Pashkov be cannot be and cannot the uncorrected thresholds are are not reported and uncorrected thresholds the et Fradin et However, Fradin extracted due to insufficient information. However, Zverev and a1.19 anticipationofofsome some problem problem with with the the Zverev and 19 ininanticipation al. 1973 for in 1973 reported in data reported scale the data Pashkov method did not scale self -focusing,and and in inretrospect retrospect they were correct in not scaling self-focusing, NaCI powerininNaC1 damagingpower thedamaging that the observed that They observed the data. They used for lenses used the lenses of the length of focal length scaled as as the square of the focal scaled 1977 Smith et in 1977 earlier, in noted earlier, As noted the picosecond pulsewidths. As 532 their 532 Pj to correct their aí.22 alsofound found some some problem problem in using P1 al. 22 also self-focusforselfthresholdsfor damagethresholds focuspicosecond damage nm and 355 nm picosecond ing. They They included included the thebreakdown breakdown power and and the the uncorrected uncorrected ing. recould reworkers could future workers that future so that report so focal area in their report focal area 10 No. 10 28 No. Vol. 28 ENGINEERING // October OPTICALENGINEERING 1138 October 1989 1989 // Vol. 1138 / /OPTICAL Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms LASER-INDUCED ANDTHE THEROLE ROLEOF OFSELF SELF-FOCUSING LASER- INDUCED DAMAGE DAMAGE AND -FOCUSING TABLE IV. scaled for TABLE IV. Breakdown Breakdown thresholds thresholdsat at0.53 0.53 urn µm of of Ref. Ref. 22 scaled for self-focusing self- focusing using using P1 Pt (column 7) and P2 P2(column (column 8). 8). PPstands standsfor forthe the breakdown PB , E0 breakdown power PB, E0isisthe the breakdown breakdown field, field, and A is the focal area area calculated calculated using using linear linear optics. Material Material PB PB (KW) (Kw) AA G»m)» (µm)= P/Pi P/P, P/P2 P/P= (unsealed) )unsealed) E. Eo (MV/cm) (MVrcm) (unsealed) (unsealed) EPi Ep, EP2 (scaled) (scaled) (scaled) (scaled) EP2 KH2P04 KH2PO4 151.0 151.0 16.0 16.0 0.57 0.57 0.15 0.15 15.3 15.3 23.4 23.4 (53o/a) (53%) 16.6 (8%) (8%) 16.6 Si02 Si02 129.0 129.0 15.9 15.9 0.46 0.46 0.12 0.12 14.5 14.5 19.0(31%) 19.0 (31o/a) 15.4(6%) 15.4 (6%) NaCI NaCI 38.4 38.4 15.1 15.1 0.60 0.60 0.05 0.05 7.9 7.9 12.4(57%) 12.4 (57%) 8.1 (3%) 8.1 (3%) CaF2 CaF2 146.0 146.0 15.9 15.9 0.62 0.62 0.09 0.09 15.5 15.5 25.2 (63%) (63%) 25.2 16.3 (5%) (5%) 16.3 NaF NaF 126.0 126.0 15.8 15.8 0.45 0.45 0.05 0.05 15.0 15.0 19.4 (30%) 19.4(30%) 15.4 (3%) (3%) 15.4 LiF LiF 171.0 171.0 16.1 16.1 0.59 0.59 0.06 0.06 16.9 16.9 26.5 (57%) (57%) 26.5 17.5(4%) 17.5 (4%) examine light of of new new measurements. measurements. examine the the data in the light We We can can now now use use Eq. (5) to reexamine the the 532 532 nm nm breakbreakre-examine down al. 22 In work, the breakdown breakdown down data data of Smith et al.22 In that that work, powers powers are are all all below below P,, P1, so so the the irradiance increase predicted by Eq. Eq. (5) (5)should should be bevalid. valid.Six Sixmaterials materials were were studied, studied, includincluding fused NaCI, as fused quartz quartz and NaC1, as shown in Table IV. IV. In examining we find that that the the breakdown breakdown threshold threshold fields ing the the data we fields increased These increased increased increased as as much much as as 50% 50% to to 60% 60% using usingP,. P. These thresholds However, when the thresholds are thresholds were were reported. reported. However, properly corrected using using the the second second critical critical power powerP2 P2 we we find on average only only a 5% 5% increase. increase. This is on the average is well well within the ±15% absolute uncertainty in the measurements. Smith et al. 22 also at 355 355 al.22 alsoreported reported breakdown breakdown thresholds at nm for three three of the the materials materials listed in Table Table IV. IV. The The results results for for near-UV this near -UVstudy studyindicate indicatethat, that, in in most cases, cases, the breakwere substantially down threshold powers for these materials were than the the P1 Pj critical powers at this wavelength. higher than wavelength. The The only only exception was CaF2 CaF2 where PB PB was be 0.7P1. 0.7Pj. In an was found found to be to correct correct their theirdata datafor forthe thepresence presenceofofself attempt to -focusing self-focusing they scaled scaled their breakdown breakdown threshold threshold irradiance they irradiance levels levels in in KH2 PO4 , LiF, KH2PO4, LiF, and SiO2 Si02 using Eq. (5) but with a critical power Pj and and P2. P2 . somewhere between P1 While While they theywere wereon onthe theright righttrack, track, meaningful meaningful comparison comparison of the the 355 355nm nmdata data with with results results at other wavelengths wavelengths is is difficult poor spatial spatial quality quality of due to the reported poor ofthe the 355 355 nm nm beam beam used in the the measurements. measurements. The The uncertainty uncertainty in the used the energy energy distributionwithin withinthe thefocal focalarea arealead leadSmith Smithetetal.22 al. 22 to assign a distribution factor of two range for the scaled breakdown threshold threshold fields fields at this wavelength. wavelength. The The actual actual breakdown thresholds may or may not be within may within this this range. range. A A further complicating factor 355 nm work is the recent result that the the for interpreting the 355 effective n2 effective n2for foraamaterial materialmay maynot notbe beconstant constant as as aafunction function of of wavelength energies approaching wavelengthfor for photon photon energies approaching aa substantial substantial fraction of the band band-gap -gap energy. energy. Based Based on our measurements measurements using the technique of Ref. Ref. 43 43 in in BK BK-7 technique of -7(see (seeTable Table II II comparing comparing n2 at jum) and and those thoseofofWhite Whiteetetal. BK-10 n2 at 11 jumandO.5 µm and 0.5 µm) al.4949ininBK -10 at at 355 355 nm, nm, the the n2 n2 values valuesfor for the the three three materials materials studied studied at at the third harmonic wavelength wavelength may well well be substantially substantially lower lower than the values values at 1064 nm. the need need for for than the at 1064 nm. This This points points to to the accurate measurements of of n2 n2 in these materials in in the the regime regime where effects may play. It may where multiphoton effects may be be coming into play. also necessary to measure nonlinear refraction refraction at at near near-also be necessary to measure damaging levels as damaging irradiance levels as isis done done in in the beam distortion method.43 This method.43 This being beingthe the case, case, we wewill willnot notattempt attempt at this time to reexamine the 355 355 nm nm thresholds. In our our rere-evaluation breakdown results results of other other evaluation of of the breakdown workers, we have concentrated onthe thework workof ofRef. Ref. 22 22 for for two concentrated on reasons. The first reason is that the breakdown measurements breakdown measurements in that work were were conducted conducted for pulse pulse durations comparable to our our own. own. Therefore, Therefore,the theselfself-focusing mechanisms in the focusing mechanisms the test materials will will be second reason is be the same. same. The second is that, of the experimenters who scaled scaled their breakdown thresholds for the presumed presumedpresence presenceofofselfself-focusing, Smithetetal.22 al. 22 compose compose focusing, Smith one of few fewgroups groups whose whosework workcontains contains sufficient sufficient information information and experimental parameters determine the true true breakbreakand experimental parameters to determine down workers merely merely reported reported the the scaled scaled down thresholds. Other workers breakdown threshold irradiance irradiance levels levels without including including the focal used in in the the measurements. measurements. This This makes makes itit focal spot spot radii used impossible thresholds. In In addiimpossible to to recalculate the breakdown thresholds. addition, the incorrectly incorrectly scaled scaled data dataofofSmith Smithetetal.22 al. 22 was was used used in in support of the intrinsic intrinsic avalanche ionization ionization model. model. studies have Several other breakdown studies have been been conducted in these materials in in which which no noselfself-focusing corrections were were these focusing corrections For example, example, Manenkov29 made. For Manenkov 29 reported breakdown breakdown meameasurements in the alkali alkali halides halides (including (including NaC1) NaCI) for nanonanosurements at 10.6, 10.6, 1.06, 1.06, 0.69, 0.69, and 0.53 0.53 µm pm laser laser second pulse pulse durations at wavelengths. wavelengths.There There isis some some uncertainty uncertainty in in the focal focal spot spot radius used in the measurements measurements since since two values are reported without specifying specifying which which correspond correspond to the breakdown irradiance levels levels listed in Manenkov's Manenkov'swork.29 work. 29 Feldman Feldmanetetal.42 al.42 electrostriction isis of relatively minor importance estimate that electrostriction for the nanosecond nanosecond pulses pulses used used in in these these experiments. experiments. HowHowever, we will use the the larger largervalue valueofofn2n2==4 4X 10~13 X 10 -13 esu calculated from nanosecond nanosecondthree three-wave lated from -wave mixing mixingexperiments.50 experiments. 50 With this in in mind mind we we find findthat thatPB PBininNaC1 NaCI isis 0.5P2 0.5P2 at 532 532 nm and PB isis 0.14P2 0. I4P2at at 1064 1064nm nm ififwe weuse usethe the larger larger of the the two focal radii cited in Ref. 29. If we use use the small focal radius we find find that PB PB for NaCI is 0.07P2 0.07P2 at 532 nm and 0.02P2 for 1064 nm. 1064 nm. Thus, self self-focusing -focusing effects effects in in Manenkov's Manenkov's29 are 29 work for NaC1 NaCI are negligible negligible except except perhaps perhaps for for the the combination of the largest spot size size and and shortest wavelength and, therefore, should should not not be scaled. scaled. The The wavelength wavelength dependence dependence reported reported by by Manenkov Manenkov from 10.6 10.6 /xm 0.69 µm µm to 0.69 /zm was an increase in threshold much stronger stronger than than that that reported reported by by Fradin 1717 (a factor of of three). three). However, 0.53 )um net drop However, the the threshold threshold dropped dropped at 0.53 µm for a net going from from 11 /im to 0.5 0.5 pm µm consistent with our measurements. In a similar similar nanosecond nanosecondstudy, study,Merkle Merkleetetaí.51 al. 5I-53 ~ 53 reported single for Corning Corning 7940 7940 fused quartz single shot shot damage thresholds for for laser wavelengths wavelengths ranging from 1064 1064 nm to 355 355 nm. In In fused quartz as well as in NaCl, NaCI, for for the the tight tight focusing focusing geomegeometry used, electrostriction has been been shown shown to to play play aa small role in electrostriction has self-focusing around30 30ns.42 ns.42 We We self- focusingeffects effectsfor for pulse pulse durations durations around use n2 value of of 0.95 0.95X10" 13 esu use the n2 X 10 -13 esureported reportedby by Feldman Feldman et et al. 42 for al.42 fornanosecond nanosecondpulse pulsedurations durations in SiO2 Si02.. We We find find that that the the breakdown powers powers reported by by Merkle Merkle et et al.51 al. 51 for for Corning Corning 7940 1064 nm and equal to 0.07P2 7940 were were less less than than 0.08P2 0.08P2 at at 1064 0.07P2 at 532 self-focusing 532 nm. nm. Therefore, Therefore, self -focusing effects in the work of Merkle et al. 51 are of two al.51 arenegligible. negligible.They Theyreport report a decrease by a factor of in threshold in in going going from from 1.06 1.06 pm /im to to0.53 0.53 µm.51 /xm. 51 We re-examined We have have also reexamined our our own own results published published in Refs. Refs. 33 and and 32. 32. In Ref. Ref. 33 we we used used beam beam distortion distortion and polarization dependence to verify verify that that self self-focusing zation dependence -focusing was was not not the dominant breakdown breakdowneffect. effect. However, However, these these tests tests (i.e., (i.e., polardominant ization dependence dependence and beam distortion) were not conducted conducted condition used. used. For for each experimental condition For the the most part, little few percent) of the (a few percent) or no adjustment of the originally originally published published numbers is is needed. needed. For For the ultra-short ultra -short pulse data (pulsewidth (pulsewidth OPTICAL ENGINEERING / October 1989 / Vol. 1139 OPTICAL ENGINEERING / October 1989 / Vol.2828No. No.1010/ / 1139 Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms STRYLAND VAN STRYLAND MANSOUR, VAN SOILEAU, WILLIAMS, MANSOUR, 1054 at 1454 SiO2 at jum for Si02 14 µm size of 14 less ps) and largest spot size less than 55 ps) nm, adjustments as high as a factor of two were needed. These adjustments as observed or trends observed corrections do not not change change any any of the trends corrections do discussed in conclusions drawnfrom from that that data as discussed in the next conclusions drawn section.3,32 addition,we weshould should note note that that we have studied section. 3' 32 InInaddition, techniques many samples of these materials grown by various techniques over the past past 15 15years. years.While Whilethe thethresholds thresholds vary from sample different from different even from and even boule, and boule to boule, from boule sample, from to sample, is here is presented here samples taken from the same boule, the data presented optical "good" optical similar "good" consistent with consistent with data data obtained from similar sample exceptional sample quality material. We We have have not found an exceptional quality material. samples the samples of the behavior of that behaved from the behavior differently from behaved differently here. reported here. dependence size dependence spot size 5.2. Wavelength, Wavelength, temporal, and spot 5.2. self-focusing ofselfeffects of theeffects for the account for focusing Given that we now can account we can can unambiguously unambiguously determine determine the in an LID experiment, we as such as dependence of of the the threshold threshold on various parameters such dependence pulsewidth, spot size, size, and and wavelength. wavelength. The The conclusion conclusion reported reported dependence wavelength dependence observed wavelength al. 22 that by by Smith et aí.22 that the observed theory ionization theory avalanche ionization predictions of avalanche agreed with with the predictions agreed P l as the critical depended on the scaling using Eq. (3) with P1 depended decrease in shows a decrease Ref. 22 shows , the power. Using Using P2 P2, the data data of Ref. power. threshold with decreasing wavelength, which isis not not consistent consistent We find with intrinsic intrinsic avalanche avalanche breakdown. breakdown. We find similar similar results results with wavelength this wavelength While this dependence. While wavelength dependence. the wavelength for for the multi-intrinsic multi by intrinsic predicted by dependence isis in in the direction predicted dependence damage,54 the photon- induced damage,54 the dependence dependence is is much much too weak. photon-induced process is As the the order order m m of the the multiphoton absorption process As increased, the the irradiance irradiance needed needed to to obtain obtain the same same absorpabsorpincreased, inverse ratio of the nonincreases approximately approximately as the inverse tance increases by linear absorption coefficients.55 This ratio ratio is is estimated by coefficients. 55 This linear ExperiI, where 55 to Wherrett Wherrett55 to be be = 10~4 10 -4I, whereII isis the the irradiance. Experi10~3 ments indicate indicate that that this ratio is =10 -3II (Refs. (Refs. 56 56 and and 58). 58). For For ments CdS at coefficient of CdS two-photon example, the the two -photon absorption absorption coefficient example, three-photon its three cm/GW, 5.5 cm reported 56 as is reported56 nm is 0.53 µm 0.53 as 5.5 /GW, and its -photon 0.01 as 0.01 reported 58 as coefficient at 1.06 absorption 1.06 pm µm isis reported58 absorption coefficient . Thus, cm3 cm3/GW2 /GW2. Thus,totoobtain obtainthe the same same absorptance absorptance at the two 550 different wavelengthswould wouldrequire requirean an irradiance irradiance of =550 different wavelengths GW/cm2 GW /cm2(or (ormore, more, theoretically). theoretically). Four-photon Four -photon absorption 10 would require would require a correspondingly higher irradiance. From 10 µm to 0.5 0.5 jum µmthe theexperimentally experimentally measured measured irradiance irradiance threshjum olds olds change change but but only only by by factors factors of of two two to to four. four. The The reported observation of of four-photon four -photonabsorption absorptionatat 532 532 nm nm prior prior to to observation damage by the the group group at at Washington Washington State University is interesting and and may mayindicate indicatethat that intrinsic intrinsic multiphoton multiphoton absorption the damage in the responsible or or partially partially responsible responsible for for damage isis responsible note, We note, selected samples samplesof of NaCl NaC1studied studiedby by that that group. group. We selected however, that the high high irradiance used by by the WSU WSU group group of however, that 550 GW /cm2for forpicosecond picosecondpulses pulsesisis 5.5 =5.5 times times the the damage damage 550 GW/cm2 by reported by samples reported "best" samples threshold observedfor for the the "best" threshold observed pulses. 29 The Manenkov using nanosecond The absorptance due nanosecond pulses.29 be of the order of then be to direct four-photon four -photon absorption absorption would then It , lower 5.5 -3,, which which isis = 66XX10~3 10 -3, lowerfor forthe thenanosecond nanosecond pulses. It 5.5~3 is caused pulses is seems unlikely unlikelythat that if if damage damage for picosecond pulses seems same mechanism the same that the by intrinsic intrinsic multiphoton multiphoton absorption absorption that Manenkov. 29 dataofofManenkov.29 nanosecond data is for the the nanosecond responsible for is responsible inconsistencies with Gorshkov also found found inconsistencies with the avaal. 59 also Gorshkov et aí.59 of the damage of of damage dependence of lanche model in the the temperature temperature dependence Ref. 88 of Ref. authors of 0.53 jum. µm. We agree with the authors alkali halides at 0.53 in and contradictory contradictory data data exist exist for for m m = 4 in "insufficient and that "insufficient assign unequivocally assign eV) to unequivocally 2.33 eV) NaCI (E (Eg== 8.6 8.6 eV, eV, hv by = 2.33 NaCl NsCI 150 + 15 150515 105±15 105315 m=7.2Nm 36 + 4 3634 5 EO(MVIcm) EB(MV/cm) 0.5 1.06 150315 105315 3634 5 10 15 20 EB(MV/cm) EgOMVkm) several forseveral SiO2 for and Si02 NaCl and forNaCI E B for ofEB dependenceof Fig. 5. Wavelength Wavelengthdependence Fig. scaled beenscaled havebeen thresholdshave Thesethresholds /urn.These 0.53µm. and0.53 1.06and at1.06 pulsewidths pulsewidths at values measured values and measured P2 and usingP2 self-focusing forselfpercent for by by a few percent focusing using n2 . 43 of of n2.43 since the However, since mechanism." However, avalanche mechanism." damage damage to the avalanche the sample to sample, from sample considerably from damage threshold varies considerably present and effects are we we must must still still conclude conclude that extrinsic effects are present and Additionally, samples. Additionally, thresholdsamples. lower threshold dominant for the the lower dominant may contribute carriers for intrinsic multiphoton absorption may intrinsic was evidence for an eventual although no evidence for this was avalanche, although eventual avalanche, an jum in 0.5 µm 8. At 0.5 Ref. 8. observed observed in in the the photoacoustic photoacoustic data data of Ref. these wide-gap wide -gapmaterials materialsthe the question question of the role of intrinsic these However, it is remains. However, LID remains. multiphoton multiphoton absorption absorption in in LID jum and longer intrinsic unlikely unlikely that that for the wavelengths wavelengths of of 11µm is playing a role. multiphoton absorption is NaCl at of NaC1 samples of 13 samples on 13 We reported damage on at 11 /zm µm and We from varied from thresholds varied field thresholds thefield While the Ref. 3.3. While in Ref. nm in 0.5 µm 0.5 we saw no of four, we sample to to sample sample by by as as much much as a factor of sample dependencies of the systematic differences differences in in the the parametric parametric dependencies the systematic were perexperiments were all experiments thresholds, although ELID ELID thresholds, although not all formed for all samples. samples. Figure 55 shows aa bar bar graph graph of damage damage size in air of spot size focal spot for aa focal SiO2 (lower) for NaCl (upper) (upper) and Si02 in NaCl 1.06 /zm 7.2 )um µm for various pulsewidths as indicated, for both 1.06 µm small corrections (unshaded) and 0.53 (shaded). The small corrections for ^m (shaded). 0.53 ,um self- focusinghave havebeen beenincluded included in in this this figure. figure. Except for the self-focusing ELID the ELID samples, the SiO2 samples, NaCl and Si02 shortest shortest pulses pulses in in both NaCI to 0.5 1 ^m to in going from a wavelength of 1µm threshold isis reduced in threshold µm, which is inconsistent inconsistent with an intrinsic avalanche model. which is /im, Refs. 44 and In the avalanche breakdown model model of Refs. and 55 the avalanche breakdown In (i.e., limit (i.e., field limit highfield thehigh E2ininthe proportionaltotoE2 ionization rateisis proportional ionization rate by given by carriers isis given ofcarriers buildup of short pulse limit). Then, the buildup N0 exp(aE2t) , N N == Noexp(aE2t) (10) (10) N0 is where N is is the carrier density, No is the the initial carrier density, and a is is aa material material dependent dependent constant. This limit corresponds electrons the electrons of the energy of in energy increasein theincrease which the in which situationin to the situation simply proportional in the conduction proportional to to the input conduction band is simply says that the negligible. This says are negligible. losses are all losses that all irradiance and that light input light the input which the at which rate at ionization rate is is limited by the rate electrons. It is band electrons. beam can supply energy to the conduction conduction band carrier the carrier when the occurs when damage occurs commonly assumed commonly assumed that that damage can be solved (10) can Eq. (10) Thus, Eq. Nc . Thus, value Nc. critical value reaches aa critical density reaches dependence: t^°-5 showing aa tp field showing .5 dependence: breakdown field for the breakdown EB = 1 1 /at! atp Nr N ln' /2 (11) (11) No pulsewidth this pulsewidth NaCl this forNaC1 pulses for shortpulses very short for very We find that for We constant, is constant, fluence is breakdown fluence dependence dependence is is valid valid and the breakdown t^° 3 dependence. weakert-13-3 somewhatweaker while for Si02 see aasomewhat we see SiO2 we while No. 10 Vol. 28 No. ENGINEERING // October OPTICALENGINEERING 1140 1140 / /OPTICAL October 1989 1989 // Vol. Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms LASER-INDUCED DAMAGE AND ANDTHE THEROLE ROLEOF OFSELF SELF-FOCUSING LASERINDUCED DAMAGE -FOCUSING IUU 100 24 E 20 14µm IB .. 1 06m 16 4 Ó 12 10 ó ff B s Ips 10ps 10ps lOOps Ins 100ps Ins PULSE DURATION, ttp p PULSE DURATION, 10ns IOns For the low field field limit, limit, i.e., i.e., longer longer pulses, pulses, the the ionization ionization rate is is exponentially exponentially dependent dependent on on E and the the resulting resulting pulsewidth pulsewidth dependence dependence isis relatively relatively weak.4 weak.4In In Fig. Fig. 6,6, we we reproduced reproduced the the theoretical curves curves derived derived by Sparks et al.4 al.4 showing the predicted dicted dependence dependence of of the the breakdown field EB EB on pulsewidth and have have extended extended the the pulsewidth pulsewidth scale scaleto to longer longerand and shorter shorter pulses. of the the data data for pulses. The overall dependence dependence of foraa given given spot spot size size is is in in remarkably remarkably good good agreement agreement with with this this theory using using no adjustable intrinsic avalanche adjustable parameters. However, intrinsic avalanche ionizaionizapredict aa spot spotsize size dependence, dependence, which tion does not predict which isis clearly clearly seen seen in in the the data. This relatively relatively large spot size size dependence dependence may may well well be be due due to extrinsic materials materials parameters parameters such such as as multiphoton ionization of impurities impurities or defects defects that provide the starter starter electrons electronsfor forthe theavalanche avalancheN0.3,32 N0 . 3' 32 While While the the observed observed temporal temporal dependence is consistent with spot size an intrinsic avalanche, the wavelength and spot size dependdependence strongly phenomena is ence strongly indicate indicate that that the phenomena is an an extrinsic extrinsic of materials. In In addition, addition,the thestrong strongsampleproperty of to -samsample-to-samin thresholds thresholdssupport supportthis thisconclusion.12,29 ple variations in conclusion. 12' 29 The extrinsic nature damage makes makes quantitative, quantitative, first extrinsic nature of bulk damage first principle descriptions damage process process very principle descriptions of the damage very difficult. difficult. One problem is is that that the good optical materials of of interest have very low low levels levelsof ofdefects defectsand and impurities. impurities. One One solution to this problem do experiments experiments with with samples samples prepared with problem isis to do with known type and densities of defects and impurities. This is the approach we take below. below. 6. CONTROLLED DEFECT STUDIES 6. CONTROLLED The (which produces, produces, among other The effects effects of of y irradiation (which defects, 60 on defects, E' centers) centers)60 onthe the ELID ELID thresholds of fused silica, were were investigated. investigated. Samples Samples were were sliced slicedinto into four four quadrants. One was kept as One quadrant was as aa control control (i.e., (i.e., no no irradiation), irradiation), and the remaining three quadrants quadrantswere weresubjected subjectedtoto106, 107,, and 106 ,107 10 8 rad 108 rad of of cobalt cobalt y irradiation irradiation from from the the Naval Naval Research Research Laboratory source. Unfortunately, Unfortunately, the density of Laboratory cobalt cobalt source. the density defects defects cannot cannot be determined,60 determined,ó0 although although their effects effects on linlinear absorption and ELID ELID can can be be measured. measured. Single Single specimens specimens of three types types of fused fused silica silica were were tested: tested: Spectrasil A, B, and WF performedwith with1818nsns(F(FWHM) W F(water (water free). free). Damage Damage was performed W H M) pulses at 1.06 1.06 p,m Amand and0.53 0.53/zm µmfocused focused into into the bulk of three 3 mm thick samples using a 40 40 mm focal length lens. Each site was was irradiated irradiated only only once. once. The The ELID ELID thresholds thresholds were were found found to to be at the be independent independent of of y irradiation at the1.06 1.06 µm jumwavelength. wavelength. However, However, significant significant reduction reduction in in damage damage thresholds thresholds (up to 40%) 40 %)was wasmeasured measuredfor forthe the irradiated irradiated samples samples at at 0.53 0.53 µm.61,62 jum. 61 ' 62 effects of selfself-focusing Again, the effects focusing were weredetermined determined to be negligible by ligible by performing performing polarization dependent dependent damage damage meamea- V (a) I 266 532 266 532 100ns 100ns Fig. 6. Pulsewidth dependence dependence of Fig. 6. Pulsewidth of the the rms rms breakdown field E8 for breakdown field EB for NaCI at /urn for different spot spot sizes. sizes. Data Data are are scaled scaled for NaCI at 1.06 .em for three different self-focusing . 43 The self- focusing using using P2 P243 Thesolid solidline linewas wasobtained obtained from from the electron avalanche avalanche ionization of Sparks Sparks et et al.4 al. 4 ionization theory of i /^'N' — WF --- A ..... B 0Q 0 __...—-*.._„ "^ #= a—*" 90 90 80 80 70 70 60 60 50 50 40 40 30 30 20 20 10 10 5.0µm 7.2µm 22 J 1064 1064 r* IUU 100 90 90 80 80 70 70 60 60 50 50 40 40 30 30 20 10 n e=> ST -A f^ / V v' — WF -—A .......... B i ! (b) 1 266 532 266 532 1064 \|nm) X Inml Alnml X Inml Fig. Fig. 7.7. Transmission Transmissionas asaafunction function of of wavelength wavelength AX for for the the three three samples of (a) unirradiated samples of SiO2 Si02 (a) unirradiated and and (b) (b) yy irradiated irradiated with with 108 10 8 rad. of the the various various fluorozirconate f luorozirconateglasses glasses studied. TABLE V. V. Composition Composition of studied. Sample Sample A A BB CC DD EE FF Color Color Clear Clear Green Green Green Green Green Green Violet Violet Yellow Yellow ZrF4 ZrF4 (mol°/o) (mot %) BaF2 BaF, (mol%) (mol %) 57 57 34.5 34.5 34.25 34.25 34 34 34 34 33.75 33.75 34.25 34.25 56.75 56.75 56.5 56.5 56.5 56.5 55.75 55.75 56.75 56.75 LaF3 LaF, AIF3 AIF, CrF, CrF3 MnF2 MnF, (mol %) (mol"/o) (mol°/o) (moth) (mol%) (mol %) (mol%) (mol %) 4.5 4.5 44 44 44 44 44 44 4.5 4.5 4.5 4.5 4.5 4.5 4.5 4.5 4.5 4.5 NiF, NiF2 (mol°/o) (mol %) NdF3 NdF, (mol°/o) (mol %) 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 0.5 11 1 1 0.5 0.5 surements. jum are substantially surements. The ELID thresholds at 0.53 µm lower than those at 1.06 1.06 µm /zm even for the unirradiated witness witness samples. samples. Avalanche ionization predicts an an increase increase in threshold reduced wavelength. wavelength. Thus, the ELID ELID process old for reduced process is is not not simply even for for the the witness witness sample. simply avalanche breakdown even sample. spectra of Figure 7 shows shows the linear transmission spectra of the unirradiated and and irradiated irradiated(108 (108rad) rad)samples.61.62 samples.61 ' 62 Note that this this figure figure shows shows no no observable change in transmission at either either 1.06 show a substantial substantial change 1.06 urn µm or or 0.53 0.53 jitm µm but does show change at 0.266 jum irradiated samples. 0.266 µm for the irradiated samples. This This suggests suggests that the the decrease in at 0.53 µm jum may be associated with in ELID ELID threshold threshold at with the change in transmission at the the harmonic harmonic0.266 transmission at 0.266µm. ^m. We We will will examine examine this this relation relation after after presenting presenting data data that that shows shows aa similar linear absorption absorption at similar dependence dependenceofofELID ELID on on linear at aa harmonic. We also performed series of LID performed a series LID experiments on fluorozirconate (FZ) glasses, glasses, undoped undoped and and doped with Cr, Mn, Ni, Ni, and and Nd. 63 Table Nd.ó3 Table VVshows showsthe theglass glasscompositions. compositions. The linear absorpabsorption spectra are given given in in Ref. Ref. 63. 63. The The doped doped and undoped FZ glasses were were studied studied at 1.06 jum µm using 45 ps and 18 ns pulses pulses and and a calculated 5.3 5.3 jum Measurementsatat0.53 µm focused spot size. Measurements 0.53 Am jum were performed 18 ns pulses performed using 18 pulses and and a calculated focused spot size, size, assuming assuming negligible negligible aberrations, aberrations, equal Polarequal to to 2.7 2.7 µm.63 jum. 63 Polarization dependent studies studies confirmed confirmedthe theabsence focusabsenceofofselfself-focusing effects. effects.The The breakdown breakdown fields decreased significantly at both wavelengths FZ glasses glasses when when compared wavelengthsfor for all all of of the doped FZ compared with the undoped sample sample A. A. We present below below aa two two-photon assisted electron We present -photon assisted electron avaavalanche breakdown model as as given given in in Refs. Refs. 62 62 and and 63 63 that breakdown model that we we justify primarily on on the the basis basis of of its its surprisingly good fit of the data. experimental results results for both the irradiated irradiated silica data. Our experimental silica and FZ glass materials were found to be be in in good good agreement agreement with this very simplified simplified model in which two-photon two -photon absorption by impurities or defects provides the starter electrons for an avalanche. avalanche. In In this this model modelwe weassume assumethat thatlaserlaser-induced induced breakdown occurs occurs when when the the density density of breakdown offree free carriers carriers generated generated combination of oftwo two-photon and avalanche by aa combination -photon and avalanche processes processes OPTICAL / October 1989 / Vol. OPTICALENGINEERING ENGINEERING / October 1989 / Vol.2828No. No.1010 / / 1141 1141 Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms SOILEAU, MANSOUR, VAN VAN STRYLAND STRYLAND SOILEAU, WILLIAMS, WILLIAMS, MANSOUR, 500 1BU 180 i5 S Nl_ • Spectrasil A Spectrasil A 160 160 • tp tp == 15ns 1 5ns 140 \ff O i jWm 120 100 Fluorozirconate Glass Gbss Fharozirconate X-1064nm a= 1084 nm J-' • À \ == 532nm 532nm 400 - tp tp « 45 ps =45ps A c /f ; CO o 300 S 300 O 200 - >X •1 > W loo «n 80 0 2 1 33 4 -In (of | at 266m 266nm In krPI 012345 o 3 2 4 Fig. Square of nm versus versus the Fig. 8. 8. Square of the the damaging damaging electric electric field field at 532 nm the negative negative natural natural logarithm logarithm of of the the linear linear absorption absorption at 266 266 nm for the irradiated irradiated and and unirradiated unirradiated Spectrasil Spectrasil A Si02 SiO2 samples. samples. reaches some reaches some critical critical value value Nc Ne.. In In the avalanche process the buildup of free carrier density density is is given given by Eq. Eq. (10), (10), where where we we assumed assumed the the high high field field limit limit with with an an ionization ionization rate rate proportional to El. E|. The The model model assumes assumes that that the the initial initial free free carriers carriers are generated generated by by two-photon two -photonabsorption absorption from from impurity states states within the bandgap. Therefore, Therefore, No N0 can can be be written writtenasasNo N0 cc oc n, where is the density density of of two two-photon allowed impurity where nn is -photon allowed impurity or defect logarithm of ofEq. defect states. states. Taking Taking the natural logarithm Eq. (10) (10) yields yields ln(n) ++ constant constant aEB == -ln(n) . (12) The final assumption assumption is that the the density density ofoftwo The final is that -photon two-photon allowed wavelength (X) allowed states states at at the fundamental wavelength is propor(A) is tional to the linear absorption at the thesecond second harmonic harmonic(X (X/2). absorption at /2). For that assumption assumption Eq. Eq. (12) (12) gives gives EBla[ X a -1n(aPi)Iat lat X/2 A/2 (13) (13) where the linear linear absorption absorption coefficient coefficient at the where aa is the the second second harmonic harmonic wavelength wavelength and and It is the sample length. Figure 8 isis aa plot field at 532 plot of ofthe the square square of the the breakdown breakdown field nm \n(at) atat266 266 nm nm for forthe theSpectasil Spectasil A nm as as aa function function of of -1n(at) A sample. increasing irradiation dosage dosage goes goes from sample. Note Note that increasing from right to left left in in this this figure. figure. A A linear linear relation relation is is also also seen seen for for the the other samples (B and WF), although althoughsample sampleBB shows shows aa signifisignificant increase increase in in absorption absorption for only the highest highest y irradiation level. level. Figure Figure 99 isisaaplot plotof ofthe thesquare square of ofthe the breakdown breakdown field at 1.06 ln(a£) at at 0.53 0.53 µm p,m using using picosecond picosecond pulses 1.06 /zm µm versus versus -ln(a2) pulses for updoped and doped doped FZ FZ glasses. glasses. A similar for the updoped similar plot for for nanosecond nanosecond pulses pulses also also yields yieldsaa linear linear relation. relation. Plotting Plotting the breakdown ln(a:£) at breakdown field fieldsquared squaredatat0.532 0.532jum µmversus versusthe the -1n(at) 0.266 gives a linear rela0.266 fjLm µm using using nanosecond pulses again gives tion. Similar plots of damage versus linear linear losses losses at the damaging aging wavelength wavelength show show no no systematic systematic trends. trends. The The agreement agreement with with the the prediction of Eq. (13) is quite good considering the extreme extreme simplicity simplicity of of the the model model and and the the assumptions made. Note that even in cases cases in in which which nanosecond nanosecond pulses were used where is expected from the where the the ionization ionization rate rate is expected to depart from the EB E| dependence what pulsewidth pulsewidth or dependencegood goodfits fits are are obtained. obtained. At what irradiance from an anEB E| dependence dependence becomes becomes irradiance the the deviation from large isis not not well wellestablished. established. However, However, we we found found that that for all of the FZ glasses glasses where picosecond data where both both nanosecond nanosecond and picosecond were were taken, taken, the the reduction reduction in in ELID ELID threshold threshold for for the the doped doped samples samples was was nearly nearlyaa factor factor of of two two larger larger for the picosecond picosecond irradiation. expected in this model model where where the irradiation. This This trend trend is expected starter avalanche are created created by by nonlinear nonlinear starter electrons electrons for for an avalanche -In 532nm -In Joff) Iarl at 532nm Fig. Fig. 9. 9. Square of the damaging damaging electric electric field field at 1064 nm versus the of the the linear linear absorption absorption at at 532 532 nm nm for negative natural logarithm logarithm of for the the Fluorozirconate glass samples listed in Table V. absorption since since the breakdown breakdown field field isis substantially substantially larger larger for picosecond pulses. pulses. In spite spite of of the thecomplexity complexityassociated associatedwith withlaserlaser-induced induced damage mechanisms for dielectric materials, our our experimenexperimenare consistent consistent with with aatwo two-photon-assisted tal results are -photon- assisted electron avalanche process. this model model is is corprocess. We We should should note that ifif this implication is is that that the the witness witness samples samples at at 0.53 0.53 µm, jitm, in in rect, the implication the case of the fused fused silica silica samples, samples, and the the undoped undoped glass glass (sample A) in the glass samples are the case case of ofthe the fluorozirconate fluorozirconate glass also dominated by by extrinsic extrinsic defect defect (or (or impurity) impurity) initiated initiated also dominated This conclusion conclusion comes comes from from the the fact fact that thatthese these samples samples ELID. This are included in in the the curves curvesof ofELID ELIDversus versus In -ln absorption, and they fit. how far we we can can take take this this simple simple model model is not they fit. Just how in presenting presenting itit is that the data clear. The primary justification justification in fits the prediction. One conclusion, conclusion, however, however, is is certainly true; these materials materials is is dependent dependent on on defects defects and and the damage in these impurities. CONCLUSION 7. CONCLUSION clarified the therole roleofofself self-focusing laser-inducedWe have clarified -focusing ininlaserinduceddamage experiments experiments and and can can readily readily account accountfor forits its effects effects on With this this knowledge knowledge we we have carefully measured thresholds. With examined both our data and and the the data data of ofothers others to to determine determine examined that intrinsic avalanche ionization theory cannot account for the parametric parametricdependencies dependenciesobserved. observed.Sample Sample-to-sample -to- sample variations, wavelength wavelength dependence, dependence, and and spot spotsize size dependence suggest that damage to transof damage thresholds strongly suggest dielectric materials materials isis an an extrinsic extrinsic process. process. In In aa sense, sense, parent dielectric is good this is good news news in in that that the implication is that ELID thresholds increased as progress is is made made in the materials materials olds can can be be increased as progress areas. growth and preparation areas. 8. ACKNOWLEDGMENTS 8 ACKNOWLEDGMENTS We of the Office of Naval We gratefully gratefully acknowledge acknowledge the support support of Naval Research, Research, the the Florida High Technology and Industry Council, cil, and and the the Defense Defense Advanced Advanced Research Projects Agency, and we wish we wish to to thank thank D. Griscom of the Naval Research Laborairradiating samples. samples. tory for irradiating 9. 9. REFERENCES 1.1. N. N. Boembergen, Boembergen, "Laser induced electric electric breakdown in solids," solids," IEEE J. Quantum Electron. Electron. QE QE-10, 375 (1974). (1974). Quantum -l0, 375 2. W. L. L. Smith, Smith, "Laser "Laser induced induced breakdown breakdown ininoptical optical materials," materials," Opt. Eng. Eng. 2. 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Instrum. ionizing radiation radiation on laserinduced damage damage in in Si02," Methods Phys. Phys. Res. Res. B:32, 6:32,311-314(1988). 311 -314 (1988). 62. M. M. J.J.Soileau, Soileau, N. N. Mansour, Mansour,E.E.Canto, Canto,and andD.D.L.L.Griscom, Griscom,"Effects "Effects of 62. of radiation induced induced defects defects on laserlaser-induced ," Natl. induced breakdown breakdown in in SiO2 Si02," Natl. Bureau of Standards Special Pub. 746,486^496, Print-Standards Special Pub. 746, 486 -496, U.S. Government Print ing (1985). ing Office, Office, Washington, Washington, D.C. (1985). OPTICAL ENGINEERING OPTICAL ENGINEERING/October / October1989/Vol. 1989 / Vol. 28 28 No. No. 10 10 // 1143 1 143 Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms STRYLAND VAN STRYLAND MANSOUR, VAN SOILEAU, SOILEAU, WILLIAMS, WILLIAMS, MANSOUR, Martin, D. Martin, Bendow, and B. Bendow, Soileau, B. J. Soileau, M. J. Guha, M. S. Guha, Mansour, S. N. Mansour, 63. N. 63. and D. glass," "Laser-induced "Laser- induceddamage damageinin doped doped and and undoped fluorozirconate glass," Natl. Bureau Bureau of of Standards Standards Special Special Pub. Pub. 746,108-119, 746,108-119, U.S. U.S. Government S (1985). Printing Office, Office, Washington, Washington, D.C. (1985). Printing received He received 1944. He in 1944. born in was born Soileau was M. J. Soileau the Ph.D. degree in in quantum quantum electronics in electronics in Ph.D. degree the Cali Southern Caliof Southern University of 1979 1979 from from the University fornia, Los Angeles, where where he worked worked at the Los Angeles, fornia, laser-induced onlaserCenter for Laser induced Studies on Laser Studies Center to wide-bandgap wide -bandgap optical optical materials. He He damage to and Force and Air Force U.S. Air the U.S. spent spent six six years years in in the worked for seven years at the Navy Michelson for seven ^m^Mmjm: •of the faculty of Laboratory. Dr. Soileau joined the faculty Texas State North Texas Physics of North Department Department of Physics founding member and was a founding 1 980 and University in 1980 became the he became 1987 he In 1987 Center for for Applied Applied Quantum Quantum Electronics. In of the Center Electro-Optics in ElectroResearch in for Research Center for Optics first director of the newly formed Center is a professor he is where he and Lasers Lasers at atthe the University University of Central Central Florida, where professor of and interests research interests Soileau's research Dr. Soileau's electrical engineering engineering and and physics. physics. Dr. electrical induced damage damageto tooptical optical materials, materials, nonlinear nonlinear absorption absorption laser-induced include laserand and refraction, refraction, and and optical optical limiting. degree BS degree hisBS received his Williamsreceived E. Williams William E. Texas, in Beaumont, Texas, University, Beaumont, Lamar University, from from Lamar 1978. He He then then attended school at graduate school attended graduate 1978. North Texas Texas State State University, University, Denton, Denton, where where North and his he received his MS MS degree degree in in 1981 1981 and his received his he Ph.D. degree degree in in 1984, 1984, both both in physics. physics. His His dis disPh.D. sertation, "Parametric studies picosecond of picosecond studies of sertation, laserinduced breakdown breakdown in in fused quartz and laser-induced self-focusing of selfwith the influence focusing influence of NaCI," dealt with In liquids. In and liquids. solids and damage in on optical in solids optical damage on 984 Dr. 11984 Dr. Williams Williams joined joined the the technical technical staff staff of of Texas Instruments, Instruments, Inc. Inc. (Tl), (TI), Defense Defense Systems Systems and and Electronics Electronics Group. Group. Texas While at evaluated aa number number of of optical optical limiting limiting technologies for he evaluated Tl he at TI system level level applications applications and was was cofounder of aa dedicated dedicated laboratory laboratory at at system TI for development development of of optical optical lirniters. limiters. Since Litton at Litton been at has been he has 1987 he Since 1987 Tl for Laser Systems, Systems, Orlando, Orlando, as aa member member of of the the research research staff. staff. His research Laser interests include laserinduced damage, damage, optical optical lirniters, limiters, optical phase phase laser-induced processes. optical processes. nonlinear optical by nonlinear conjugation, and frequency conversion by Dr. Williams Williams is currently and Laser and IEEE Laser the IEEE OSA, the the OSA, of the member of currently aa member Dr. Electro- OpticsSociety, Society,SPIE, SPIE,and andthe theAssociation Association of of Old Old Crows. Crows. Electro-Optics (first class honors) in physics from BS (first receivedaa BS Mansourreceived Nastaran Nastaran Mansour from the the from physics from in physics (honors) in MS (honors) an MS National National University, University, Tehran, Tehran, Iran, Iran, an physics in physics Ph.D. in and aa Ph.D. Texas, and Dallas, Texas, University, Dallas, Methodist University, Southern Southern Methodist Texas, DenNorth Texas, of North Universityof the University from the 1988 from (quantum (quantum electronics) in 1988 DenResearch Center for Research ton. ton. She She then then worked as aa research research scientist at the Center Florida, Central Florida, of Central University of Electro-Optics in in ElectroOpticsand and Lasers Lasers at at the the University physics at the of physics professor of assistant professor Orlando. Orlando. Dr. Dr. Mansour Mansour is currently currently assistant also on ran. She id Baheshti), National National University University (Shah (Shahid Baheshti), Teh Tehran. She isis also on the Laser Division, in Energy, Laser Atomic Energy, of Atomic research research staff of the Organization of dielec in dielecTehran. Her Tehran. Her research research interests interests include optical nonlinearities in optical to optical damage to laser-induced materials,lasersemiconductor materials, and semiconductor tric and induced damage is a member Mansour is Dr. Mansour physics. Dr. laser physics. and laser limiting, and materials, optical limiting, member APS. and APS. IEEE, and OSA, IEEE, the OSA, of the He 1947. He in 1947. born in was born Stryland was Van Stryland W. Van E. W. E. Ph.D. degree received received the Ph.D. degree in in physics physics in in 1976 of Arizona, Tucson, University of from the University Tucson, where where on Center on Sciences Center Optical Sciences the Optical he worked at the he He worked optical optical coherent transients. He worked in in the the multi-production, multi areas of femtosecond pulse production, laser-induced and lasersolids, and in solids, photon absorption in induced Laser Studies at the damage damage at at the Center for Laser Los Angeles. University of Southern California, Los Angeles. depart physics departthe physics Stryland joined the Dr. Dr. Van Van Stryland n 1978 n ivers ity iin Texas State Nortih Texas ment at North State UUniversity Elec Center for Applied Quantum Electhe Center informing and and was was instrumental instrumental in forming the in Research in forResearch Centerfor formedCenter newlyformed the newly joined the he joined 1987 he In 1987 tronics there. In Orlando, Florida, Orlando, Central Florida, of Central Electro-Optics Electro- Optics and and Lasers Lasers at at the the University of where he is aa professor professor of ofphysics physicsand andelectrical electricalengineering, engineering, working working in in the area area of of nonlinear optics. No. 10 Vol. 28 No. ENGINEERING /October 1144 / /OPTICAL OPTICAL ENGINEERING / October 1989 1989 // Vol. 1144 Downloaded From: http://proceedings.spiedigitallibrary.org/ on 01/30/2015 Terms of Use: http://spiedl.org/terms
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