Practical generation of femtosecond pulses of 267 nm ultraviolet light Daniel D. Hickstein∗ University of Colorado (Dated: April 15, 2009) Nonlinear crystals are a simple and effective method of generating short pulses in the near UV but cannot provide light shorter than about 200 nm. Previous studies have indicated that combining the fundamental (800 nm) and the second harmonic (400 nm) of a femtosecond Ti:sapphire laser in a hollow fiber waveguide filled with either air, argon, or xenon is an effective way to produce ultrafast pulses of third (267 nm), fourth (200 mn), and fifth (160 nm) harmonic light [1–3]. However, this method has only been used to study a handful of chemical systems, suggesting that it is more difficult to implement than its apparent simplicity would suggest. In this study a 5 cm long 150 µm ID argonfilled fiber waveguide is used to generate 200 nJ pulses of 267 nm light at 1 kHz. The dependence of the third harmonic intensity is found to vary significantly with argon pressure featuring a broad peak near atmospheric pressure. Suggestions are given for improving the conversion efficiency. I. INTRODUCTION A. Motivation The desire to observe ultrafast reaction dynamics of molecules means that there is a need for sources capable of producing femtosecond pulses of deep and vacuum ultraviolet light (VUV is light shorter than 200 nm). UV light can be used to excite electronic transitions in molecules which can rapidly induce changes in molecular geometry and cause chemical bonds to be made or broken. Such processes are relevant to all manners of new technologies, including solar energy conversion and chemical synthesis, and, since they occur extremely rapidly, lend themselves to study on a femtosecond timescale. However, as of this writing, a system for the creation of intense femtosecond pulses in the VUV range is not commercially available. Several companies currently provide reliable systems for generating 20 fs pulses of infrared light at 800 nm using a Ti:sapphire laser. This output can then be frequency doubled or tripled using nonlinear crystals to create light at 400 and 266 nm. However, the absorption of nonlinear crystals such as BBO at short wavelengths prevents their use in the creation of light less than about 200 nm [4]. Since many interesting absorption bands in molecules and materials are below 200 nm, it is important to develop practical, inexpensive, and reliable methods for generating ultrafast pulses in the vacuum ultraviolet. B. Competing methods In 1993, Ringling and coworkers published an article describing their system for the generation of 180 fs ultraviolet pulses that could be tunes from 189 to 200 nm[5]. This system utilized a series of BBO crystals and, conse- ∗ Electronic address: [email protected] quently, was able to achieve reasonably high power (4 µJ per pulse at 200 nm and 1 KHz repetition rate). Since then, various research groups have been attempting to match this level of efficiency with methods that will extend into the vacuum ultraviolet. 1. Gas cells The technique of focusing 800 nm light into a small (about 10 mm) cell filled with argon gas is the most experimentally simple of all the methods discussed here. Though the pulses generated are generally low intensity [6], the technique has recently been used for an ultrafast study of exited ethylene [7] and to measure a time constant of 1.8 fs for the dissociation of water [8]. However, the short interaction length of a simple focused beam means that the intensity of the light produced by such methods will likely be lower than that produced using other techniques. For example, the argon cell in Ref 6 produces 5 nJ of fifth harmonic light while a modern fiber waveguide has produced 160 nJ per pulse [1]. 2. Filamentation One way of increasing the interaction length of the light with the noble gas is to utilize the phenomenon of filamentation, whereby intense light creates a plasma and self-focuses into a long, narrow filament. A group in Japan has generated 20 µJ, 12 fs pulses of 260 nm light by filamentation through 15 cm of neon gas in a glass cell [9]. These results are quite promising, but this method does not seem to be in common use for generating higher harmonics. The main disadvantage is that each gas has a critical power for self-focusing, so the power cannot be adjusted as freely as it can be in the other methods. 2 3. Fiber waveguides “This alternative technology will make DUV pulses accessible for a broad range of scientific applications” –Babushkin and Herrmann [10] !" !" Hollow-core glass waveguides have been shown to generate high intensity femtosecond pulses of UV light [2, 3, 11, 12] and offer a great deal of control over the phase matching parameters. The fiber length, fiber diameter, and gas pressure can all be varied in order to achieve better phase matching for the desired process. Fiber waveguides have been used to generate UV pulses as short as 8 fs [2] and a recent study generated third harmonic light with 2 percent efficiency [3]. A theoretical study [10] found that generation of 160 nm pulses in hollow waveguides can occur with up to 30 percent efficiency and that it should be possible to generate “sub10-fs pulses in the spectral range from 90 to 140 nm”, making it clear that the there is great potential in UV generation from hollow-core fiber waveguides. C. Theory The UV light generated by these fiber waveguides is a result of a difference-frequency four wave mixing (FWM) process that involves the the combination of the fundamental and the second harmonic as shown in Figure 1. As the diagram suggests, the intensity of the second harmonic light is much more important to the efficiency of third and fourth harmonic generation than is the intensity of the fundamental. Indeed, in an unpublished report [13] to the National Science Foundation, a group at KM-Labs finds the following relationships between the harmonic intensities: 2 I3ω ∝ Iω I2ω 2 3 I4ω ∝ Iω I2ω 4 I4ω ∝ Iω3 I2ω (1) (2) (3) Thus, it is essential to maximize the amount of second harmonic in the fiber, with the fundamental playing a much smaller role. Jailaubekov and Bradforth [11] estimate the dependence of the third harmonic power (P3ω ) on the fiber length (L) and diameter (a): P3ω ∝ L2 a4 (4) suggesting that a very narrow fiber should be used. However, in practice, the difficulty of coupling light into a very small fiber creates a lower limit to the inner diameter of the fiber. An advantage of producing harmonics in a fiber waveguide is that the phase matching condition can be controlled by varying the fiber length and width as well as the pressure of the gas. Durfee and coworkers have authored several papers [14–16] regarding phase matching !!" !!" #!" "!" !!" "!" FIG. 1: The fourwave mixing process for the generation of third (left) and fourth (right) harmonic light. processes in fiber waveguides. The following equation [16] connects the wave vector for light (k) at a wavelength (λ) to the pressure in the waveguide (P ) and the diameter of the waveguide (a): k(λ) = 2π 2πP δ(λ) u2nm λ + − λ λ 4πa2 (5) where δ is related to n, the refractive index of the gas, as δ(λ) = n−1 P . Thus, the phase mismatch can often be minimized through the appropriate selection of gas and pressure[4]. II. EXPERIMENTAL The experimental work described here was completed in the laboratories of the Kapteyn–Murnane group at JILA at the University of Colorado between early February and mid-April 2009. A. Apparatus The experimental apparatus is shown in Figure 2. The idea is to pass the 800 nm output from a Ti:Sapphire laser through a BBO crystal to generate the second harmonic (400 nm); split the 400 nm light from the 800 nm; pass the 800 nm light through a half-waveplate, polarizer, and delay stage; then recombine the beams before coupling them into an argon-filled fiber waveguide. The half-waveplate in necessary because the type I BBO crystal causes the polarization of the two different harmonics to be 90 degrees offset. The delay stage is required because the group velocity dispersion (GVD) in the BBO crystal causes some pulse walk-off between the blue and the red. While there are schemes [17] to synchronize the timing and polarization without splitting the beam into 3 the two harmonics, the desire to ultimately substitute the 800 nm light with tunable infrared light from an optical parametric amplifier (OPA) dictated the use of a separate path for each harmonic. 1. Laser The 800 nm input beam was generated by a two-stage amplified, mode-locked Ti:sapphire laser operating at a repetition rate of 1 kHz. The output power of the laser (as measured at the end of the second-stage amplifier) was varied between 0.5 and 2.0 watts for alignment and, for the final experiment, measured 1.51 watts just before the UV-OPA setup. The power was not increased beyond this due to fear of burning the fiber, but with better coupling efficiency (see §II A 5), the power could be increased to the full capacity of the laser system: in excess of 4 watts. In a previous experiment, Robynne Lock (of the Kapteyn–Murnane group) found the temporal pulse width of this laser to be between 24 and 27 fs. 2. Second harmonic generation crystal Second harmonic light (400 nm) was generated from the 800 nm fundamental using a 10 mm diameter 100 µm thick beta barium borate (BBO) crystal. BBO was selected for this experiment over other second harmonic generation (SHG) materials because its high second harmonic generation coefficient allows a very thin crystal to generate significant quantities of second harmonic light. The thickness of the crystal was chosen to be 100 µm in order to limit the temporal broadening of the pulse. The desire to create UV light that could ultimately be used to study molecular dynamics means that, in this study, generating temporally short pulses takes priority over producing high laser intensity. The 10 mm crystal was smaller than the 15 mm beam, presenting the choice to either clip part of the beam, focus the beam through the crystal, or to down-collimate. Since the light would later need to be coupled into a capillary, it was decided that the better quality beam-mode resulting from simply clipping the beam would allow for more light to be coupled into the fiber. In the future, a 15 mm 200 µm crystal would greatly improve second harmonic intensity. 3. Beamsplitters The two optics that separate and, later, recombine the two harmonics have the potential to cause significant temporal pulse broadening and were therefore carefully selected. The 400/800 nm beamsplitters are 1 inch diameter 1 mm thickness “High Energy Harmonic Separators” custom coated by CVI Laser Corporation. These thin optics were chosen in order to minimize the amount of material that the red light must pass through, thereby reducing the temporal broadening of the pulses. The manufacturer claims that these separators transmit in excess of 90 percent of incident light and reflect more than 99.5 percent. The 45 degree angle of the second beamsplitter (see Figure 2) to the red beam leaves the effective diameter of the beamsplitter only slightly larger than the diameter of the beam, it proved very difficult to align this optic with both beams. The situation was further complicated by the manner in which most optical mounts extend beyond the face of the optic, resulting in further clipping of the red beam. Ultimately, the beamsplitter was glued to a mount, eliminating any additional material at the level of the beams. Further implementations of such a setup should probably incorporate a larger diameter optic in this position in order to minimize alignment difficulties. 4. Mirrors The 400 nm and 800 nm mirrors used in this experiment are standard anti-relection coated glass mirrors from the supplies of the Kapteyn–Murnane Laboratory at the University of Colorado. The original plan was to have the beam exit the UV-OPA traveling back towards the source. However, this was modified to make better use of table space by having the light pass through the apparatus and emerge traveling in the same direction as before. This would have required that more mirrors be added to the apparatus, but instead a retro-reflector was placed on a translation stage to act as the two mirrors in the delay line. The retro-reflector minimizes the changes in beam pointing caused by adjustment of the translation stage. Originally, the retroreflector was placed after the two mirrors in the red beamline, however, this made recombining the beams very difficult, as the retroreflector is difficult to finely adjust. Thus, in the final design, the retroreflector was placed before the two mirrors which allowed for easy recombination of the red and the blue beams. 5. Fiber waveguide The four-wave mixing process takes place in the center of a hollow glass fiber which keeps the light tightly focused for many centimeters. Though short fibers, from about 1 cm to 5 cm in length, are frequently used for high harmonic generation, several studies [1, 2, 10] have found that longer fibers, of about 20 to 50 cm, provide better efficiency for four-wave mixing experiments. Though Ref 2 used a 100 µm inner diameter (ID) fiber, the reported difficulty of coupling light efficiently into such a fiber convinced me that the 150 µm fiber would be the best choice for the amateur. Consequently, I prepared several 20 cm long, 150 µm ID fibers and mounted one of them into a 20 cm “V-goove” mount provided by KM-Labs Inc. 4 FIG. 2: Schematic of the experimental setup. This sketch is not to scale: in the actual setup the blue and the red beam-paths are exactly equal. FIG. 3: The 5 cm fiber (top) connected to argon and the vacuum system and the 20 cm fiber (bottom) wishing that it could be of some use to the world. The preparation of a fiber involves using a specialty computer-controlled focused laser to burn two holes into the side of the fiber about 5 mm from each end. The ends of the fiber are then sanded flat and the fiber is cleaned using an ultrasonic bath followed by a rinse with methanol. The mount features a V-shaped groove that greatly improves light transmission through the fiber by keeping it perfectly straight. The mount provides connections so that gas can pass in through the large holes in the side of the fiber and out through the ends of the fiber, where vacuum is applied. In this experiment, the vacuum at the ends of the fiber FIG. 4: The 5 cm 150 µm ID fiber waveguide during the experiment. was approximately 0.1 torr and the argon pressure at the side-holes was varied between 30 and 1100 torr. Since the holes on the side of the fiber are larger than the holes at the end, the pressure inside of the fiber is hopefully similar to the pressure measures at the side holes. In reality, the pressure inside the fiber will be somewhat less than the measured pressure of argon and is probably not constant over the length of the fiber. Thus, all “waveguide pressure” measurements in this study are approximate and will overestimate the true pressure inside the waveguide. Since it is more difficult to couple light into a longer fiber, I decided to start with a 5 cm fiber. Unfortunately, the difficulties involved in coupling the light into this fiber 5 meant that there was not enough time to also try to 20 cm fiber. It is likely that better four-wave mixing efficiency would be observed using the 20 cm fiber. Figure 3 shows both fibers in their V-groove mounts as well as the vacuum and argon gas system used to connect the 5 cm fiber. 6. Detection A simple fused silica prism was used to split the beam that emerged from the fiber into its 800, 400, and 267 nm components. Due to the overwhelming brightness of the second harmonic, a 400 nm mirror was used to reflect the majority of the 400 nm light into a beamstop, allowing all three wavelengths to be seen on a paper notecard. This was photographed with a simple point-and-shoot camera (Figure 5). Also, the power was estimated using a common laboratory power-meter and the spectrum of the 267 nm light was analyzed using an ocean optics 200–1000 nm spectrometer. I encountered some difficulty using the spectrometer because the lens that helps to couple the light into the spectrometer’s optical fiber is apparently coated with something that completely blocks 267 nm light! Once this was removed, the measurements could be made easily. B. Modifications from previous studies Originally, this experiment sought to merely replicate the results from a study conducted by KM-Labs [3] where third and fourth harmonic light was generated with a fiber waveguide. However, several significant modifications distinguish this study from Ref 3 and other previously published studies. Most of these modifications stem from the desire of this study to produce extremely short pulses that would be useful in molecular dissociation studies. This is in contrast to Ref 3 which sought only to produce high intensities of ultraviolet light for applications such as defect inspection in lithography where temporal pulse length is of little concern. The main modification of this experiment that allows for the generation of shorter pulses is the use of a 100 µm BBO crystal instead of the 1 mm crystal used in Ref 3. The increased laser power in this experiment (1.5 versus 0.2 mJ per pulse) will hopefully compensate for the decreased SHG efficiency of the thinner crystal. Still the relative intensity of the blue light will likely be less than in previous studies, so priority is given to maximizing the intensity of the blue light that is ultimately coupled into the fiber at the cost of more loss of the red light. To wit, this setup uses harmonic separators that reflect the blue and pass the red light, transferring the 10 percent transmission loss to the red beam. Similar to the apparatus in Ref 3, this setup places the delay stage in the red beam to ensure that there are fewer optics and fewer opportunities for misalignment in the blue beam than in FIG. 5: The fundamental (left), second harmonic (center), and third harmonic (right) as seen on a 3-by-5 inch notecard after passing through a prism. The intensities are not to scale because most of the second harmonic has been removed with a mirror and the light has been cropped with an aperture. The spots seen above the black line are caused by imperfect coupling into the fiber and are not part of the main beam. the red. Another important difference is that this study uses argon gas in the waveguide instead of xenon as it is much less expensive. III. RESULTS AND DISCUSSION When the light was properly coupled into the fiber, the generation of the third harmonic was observed visually by using a prism to spatially spread the three harmonics onto a paper index card. A 400 nm mirror was needed to reflect most of the 400 nm light onto a beamstop so that the bright 400 nm light would not overshadow the third harmonic. Though 266 is past the edge of the visible (380 nm), it creates a blue fluorescence on a paper index card. Interestingly, if the card is moved, a pale yellow trail appears behind the 266 nm spot, indicating some, probably phosphorescent, transition with a lifetime of several hundred milliseconds. The fourth harmonic was not observed. A. Optimization of third harmonic After first observing the third harmonic at atmospheric pressure of argon, several parameters were adjusted to optimize the intensity of the third harmonic: the dis- Integrated intensity of 266 nm peak (arbitraty units) 6 8000 7000 Intensity (arbitrary units) 6000 With 400 nm 6000 4000 5000 2000 4000 400 nm blocked 0 240 3000 250 260 270 280 290 2000 1000 200 400 600 800 1000 50000 40000 30000 20000 10000 0 20 40 Wavelength (nm) FIG. 6: Spectrum of the light emitted from the fiber with either just 800 nm or both 800 and 400 nm light passing through the fiber. After the fiber, the light was spatially filtered with a prism to remove most of the 800 and 400 nm light. Intensity (arbitrary units and positions) 66.7 fs 50 fs 41.7 fs 0 25 fs 16.7 fs -20000 0 fs -40000 240 250 260 270 80 100 120 FIG. 8: The integrated intensity of the third harmonic signal verses the delay of the red pulse. Shorter times imply that the red pulse arrived sooner than the blue. The zero point of the delay is arbitrary and does not correspond to “zero delay.” 1. 40000 20000 60 Delay (fs) of 800 nm pulse 280 290 Wavelength (nm) FIG. 7: Spectrum of the third harmonic region at different delays of the red pulse. Shorter times imply that the red pulse arrived sooner than the blue. The zero point of the delay is arbitrary and does not correspond to “zero delay.” tance of the lens to the fiber, the timing of the red pulse (by adjusting the delay stage), and the pressure of argon in the fiber. Since the lens was already positioned so that the focus was near the entrance to the fiber, the intensity of the third harmonic was already optimized with regard to the position of the lens. Furthermore, the lens had a focal length of 500 mm, so the intensity of the third harmonic was quite insensitive to the position of this lens. In contrast, the timing of the red pulse and the pressure of argon had large effects on the efficiency of third harmonic generation. Timing dependence Since the third harmonic is generated by a combination of second harmonic and the fundamental, it should be quite sensitive to the timing of the pulses. The timing of the red pulse was scanned by adjusting the position of the retroreflector using a translation stage. For this scan the pressure of argon in the fiber was fixed at 650 torr. Figure 7 shows that there is range of about 40 fs where the third harmonic is generated, a result we expect given the ∼30 fs temporal pulse width from the laser. In addition to governing the intensity of the third harmonic, the timing of the pulses also appears to affect the spectral shape of the pulse, with the peak shifting by about 5 nm over the course of about 25 fs. Since the spectrometer did not average over the entire spatial extent of the 267 nm beam, it is possible that this effect is merely due to changes in the beam profile, but it is also possible that the exact timing of the two pulses truly affects the resulting spectrum of the third harmonic light that is generated. Figure 8 presents the change in the overall intensity of the third harmonic light with changes in timing. Since the spectrometer is only capturing a small portion of the 266 nm beam, some of the effects that are seen could be due to changes in the spatial profile of the beam, but the plot nevertheless demonstrates that the third harmonic intensity is strongly dependent on the timing. Though it might simply be noise, the plot suggests that there are, possibly, two peaks of high third harmonic intensity. This result, combined with the two peaks in the spectral profile of the third harmonic suggests that perhaps the 400 nm pulses have a two-peaked shape which results in a similar profile of the third harmonic. 7 Since a previous study [13] reported some success with generating harmonics in a fiber waveguide filled with air, I tried disconnecting the argon and filling the waveguide with atmospheric pressure air. Upon doing so, the third harmonic light dropped to about one tenth of its previous intensity. Varying the pressure of air had a similar affect as with argon: the best intensity was observed around 700 torr and the third harmonic was barely visible below about 300 torr. Though the power of the third harmonic signal generated by air was too small to be measured, it is clear that using argon provides a significant increase in third harmonic intensity. Intensity (arbitrary units and positions) 40000 900 torr 30000 20000 700 torr 10000 600 torr 300 torr 100 torr 240 260 280 300 Wavelength (nm) B. Integrated intensity 255–270 nm (arbitrary units) FIG. 9: Spectrum of the third harmonic region at different pressures of argon in the capillary. 100000 80000 60000 40000 20000 0 200 400 600 800 1000 Argon pressure (torr) FIG. 10: The integrated intensity of the third harmonic signal verses the pressure of argon in the fiber. 2. Gas and pressure dependence Figure 9 shows that the pressure of argon has a similar effect on the spectrum of the third harmonic as the timing of the red pulse: there appear to be two overlapping peaks and the relative intensities change depending on the pressure of argon. The intensity is optimized at pressures between 600 and 800 torr and decreases to almost nothing a low pressures. The pressure regulator only provides pressures up to 1100 torr, but at this point the third harmonic signal has decreased substantially. Figure 10 shows how the integrated area of the spectral peak of the third harmonic changes with argon pressure. Here, we again see that there appear to be two peaks, one around 200 nm and the other around 750 nm. Refs 4, 14 discuss how different phase matching conditions generate different spatial modes depending on the pressure. Ref 14 found that the peak at lower pressure correspondes to the EH13 mode and the peak at higher pressure to the EH14 mode. Intensity and efficiency Though the 267 nm light was quite weak, it was possible to measure it using a simple laboratory power meter. After emerging from the fiber, passing through a fused silica mirror to filter out the 400 nm light, and traveling through approximately 2 cm of fused silica prism, the power of the 267 nm signal was still measured to be 0.2 mW. This corresponds to 200 nJ per pulse, an energy that would certainly be sufficient for many chemical dynamics applications. However, since higher harmonics will have several orders of magnitude smaller energies, it is unlikely that this experiment produces useful quantities of fourth or fifth harmonic light. The power of the 800 nm light immediately before this setup was measured to be 1.45 watts. After the second beamsplitter (shortly before the fiber waveguide) the power of the 800 nm light was 460 mW and the blue was 112 mW. After the fiber, the intensities for the blue/red were 9.2/31.3 watts, for a coupling efficiency of 8.2 percent for the blue and 6.2 percent for the red. In respect to the blue light coupled into the fiber, the generation of third harmonic could be considered to be 2 percent efficient. However, in terms of watts of 800 nm input into the apparatus, the third harmonic generation was only 0.01 percent efficient, a far cry from the 2 percent efficiency attained by Zhang and coworkers [3]. C. Suggested improvements to apparatus The better four wave mixing efficiency achieved by other groups [3, 11] and the optimistic theoretical predictions [10] suggest that the apparatus described in this study could be dramatically improved. Since the intensities of the third and higher harmonics are dependent on high powers of the second harmonic intensity, better coupling efficiency of the 400 nm light into the fiber could provide order of magnitude improvements in the intensity of the third harmonic signal. Durfee and coworkers [2] achieved a coupling efficiency of 20 percent for the 400 nm light and values are high as 70 percent have been reported [3]. If good coupling could be achieved, using the 20 cm fiber instead of the 5 cm could 8 also provide a significant increase in interaction length and consequent increase in conversion efficiency. Also, if fifth harmonic can be generated, the sapphire windows used at the ends of the fiber mount would have to be exchanged for windows made from a material that is more transmissive in the VUV such as calcium fluoride. D. Possibilities for future experiments This study has shown that it is reasonably simple to generate the third harmonic of a Ti:sapphire laser using an argon filled fiber waveguide. However, there are still a number of experiments that should take place in order to further characterize the resulting pulses as well as to explore the mechanisms of how they are generated. The dependence of the intensity of the third harmonic on pressure (Figure 10) and the pulse timing (Figure 8) suggest that the temporal and spectral shape of the third harmonic pulse is not a simple Gaussian, and instead may be better described as being composed of two peaks. Future experiments would probably want to use a technique like frequency resolved optical gating (FROG) to characterize the temporal shape of the pulses. If they are indeed not simple Gaussian-like peaks, then this would pose interesting questions regarding the origin of their shape. Also, it would be good to understand what parameters of this apparatus can be controlled in order to generate the shortest pulses possible, as it would be convenient if the pulses generated using this method were short enough to use directly for chemical dynamics studies without compression. [1] Tzankov, P.; Steinkellner, O.; Zheng, J.; Mero, M.; Freyer, W.; Husakou, A.; Babushkin, I.; Herrmann, J.; Noack, F. Opt. Express 2007, 15, 6389–6395. [2] Durfee,; Backus, S.; Kapteyn, H. C.; Murnane, M. M. Opt. Lett. 1999, 24, 697–699. [3] Zhang, X.; Liu, H.-H.; Müller, D.; Backus, S. Simple and Practical 157nm and 193nm Coherent Light Source. Conference on Lasers and Electro-Optics, 2008; pp CWI5+. [4] Misoguti, L.; Backus, S.; Durfee, C. G.; Bartels, R.; Murnane, M. M.; Kapteyn, H. C. Physical Review Letters 2001, 87, 013601+. [5] Ringling, J.; Kittelmann, O.; Noack, F.; Korn, G.; Squier, J. A. Opt. Lett. 1993, 18, 2035+. [6] Kosma, K.; Trushin, S. A.; Schmid, W. E.; Fuß, W. Opt. Lett. 2008, 33, 723–725. [7] Kosma, K.; Trushin, S. A.; Fuss, W.; Schmid, W. E. The Journal of Physical Chemistry A 2008, 112, 7514–7529. [8] Trushin, S. A.; Schmid, W. E.; Fuß, W. Chemical Physics Letters 2009, 468, 9–13. [9] Fuji, T.; Horio, T.; Suzuki, T. Opt. Lett. 2007, 32, 2481– 2483. IV. SUMMARY AND CONCLUSION This study demonstrated a practical setup to create femtosecond pulses of third harmonic light from the difference-frequency four wave mixing of the second harmonic and the fundamental of a Ti:sapphire laser. The final conversion efficiency of the 800 nm input beam into 267 nm was 0.01 percent and no fourth harmonic was observed. The experiment took approximately one month of graduate student time. However, many of the key components of the fiber waveguide, as well as the custom machine for making the fibers were readily available at JILA. Furthermore, experts in such systems provides much valuable advice and assistance. In a laboratory without these tools, the construction of such a fiber waveguide system would probably take much longer. Also, the fiber waveguide is difficult to align and can require re-alignment on a day-to-day basis. Consequently, if large amounts of intensity are not needed, other techniques for creation of ultrafast UV light, such as focusing through an argon cell, may be more appealing. V. ACKNOWLEDGEMENTS I would like to thank Margaret Murnane and Henry Kapteyn for providing the inspiration, funding, and lab space for this project. Chan La-o-vorakiat and Ariel Paul shared valuable advice regarding the fabrication and mounting of the fiber waveguides. Robynne Lock and Xibin Zhou provided lots of help in the lab and answered hundreds of stupid questions. [10] Babushkin, I.; Herrmann, J. Opt. Express 2008, 16, 17774–17779. [11] Jailaubekov, A. E.; Bradforth, S. E. Applied Physics Letters 2005, 87, 021107+. [12] Durfee,; Backus, S.; Murnane, M. M.; Kapteyn, H. C. Opt. Lett. 1997, 22, 1565–1567. [13] Zhang, X.; Backus, S. A simple and practical 157 nm and 193 nm coherent light source; Technical Report, 2008. [14] Durfee, C. G.; Rundquist, A.; Backus, S.; Chang, Z.; Herne, C.; Kapteyn, H. C.; Murnane, M. M. Journal of Nonlinear Optical Physics and Materials 1999, 8, 211– 234. [15] Durfee, C. G.; Misoguti, L.; Backus, S.; Kapteyn, H. C.; Murnane, M. M. J. Opt. Soc. Am. B 2002, 19, 822–831. [16] Misoguti, L.; Backus, S.; Murnane, M. M.; Kapteyn, H. C.; Durfee, C. G.; Li, T. Generation and measurement of ultrafast tunable VUV light. Ultrafast Phenomenon Conference, 2000; pp TuC5+. [17] Enqvist, H. M.Sc. thesis, Lund, 2004.
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