CP620, Shock Compression of Condensed Matter - 2001 edited by M. D. Furnish, N. N. Thadhani, and Y. Horie © 2002 American Institute of Physics 0-7354-0068-7/02/$ 19.00 TRANSITION FROM EXPANSION TO SHOCK COMPRESSION IN LASER IRRADIATED Si BY MULTIPLE SHOTS Akio Yazaki, Hiroaki Kishimura, Yoichiro Hironaka, Fumikazu Saito, Kazutaka G. Nakamura, and Ken-ichi Kondo Materials and Structures Laboratory, Tokyo Institute of Technology, Nagatsuta, Midori, Yokohama, 226-8503, Japan Abstract Picosecond time-resolved X-ray diffraction measurements have been performed on laser irradiated Si single crystal. Two types of experiments were performed in air. In one set of experiments, single shot irradiation on the silicon (111) crystal was performed at an irradiance range of 1 - 10 GW/cm2. The results of X-ray diffraction measurement showed both thermal expansion and transient elastic shock compression. It is deduced that the ablation threshold falls in the range in irradiance of 1 - 10 GW/cm2. The second set of experiments was performed with multiple shot irradiation in the range in irradiance of GW/cm2. Lattice compression due to the multiple laser irradiation was observed. This result indicates that multiple irradiation causes reduction of the ablation threshold. INTRODUCTION irradiation using picosecond time-resolved X-ray diffraction. Various numbers of multiple laser irradiations and irradiation powers were examined. The mechanism of shock generation was also discussed. In recent years, advances in the development of picosecond sources of hard X-rays have opened the possibility of the direct observation of the changes in material structure in the nanosecond to picosecond time scale. Time resolved X-ray diffraction studies have been reported in recent years l"3. Laser heating was studied and lattice expansion was reported by single laser irradiation on a Si (111) at a few GW/cm 2 . 4 " 6 On the other hand, Hironaka et al 1 studied multiple laser shots on Si(lll) at the same power density (4 GW/cm2) and observed lattce compression up to -1.05%. In the present paper, we investigated transformation from expansion to compression of Si(lll) by laser EXPERIMENTAL Time resolved X-ray diffraction with ultra-short X-ray pulses (1.93 A, 10 ps, 10 Hz) is used to probe structural dynamics in Si pumped by laser pulses (780 nm, 300ps). Details of the experimental setup are shown elsewhere 8. The 300 ps pulsed beam is divided into two beams by a beam splitter. One is used for sample excitation after passing through an optical delay line, and another is compressed to 1375 about 50 fs and irradiated on an iron target at 1017 W/cm2 for X-ray generation. The pulse width of the X-rays was measured to be about 10 ps. The Fe Ka line was used for the diffraction experiment. A 300 ps laser pulse was focused to a spot size of 1 X 4, 2 X 5 and 1 X 3 mm on a target in air with an energy of 60 - 100 mJ/pulse. The axis of irradiation was normal to the surface. Two types of the experiments were performed under varying conditions of laser irradiations. In one set of experiments, single shot irradiations, varying power density, were performed. The other set of experiments was performed with multiple laser shots. The samples used were n-type and non-doped Si (111) wafers with the thickness of 860 and 525 jim, respectively. The X-ray pulse was aimed at the center of the laser focal spot on the Si (111) and the diffracted X-rays were detected with an LN2-cooled CCD area image sensor (512X512 channels of 25 jam X 25 fim size). Data are accumulated for 600 shots. We define the time zero at the arrival of the peak of pump pulse and X-ray producing pulse at the position of sample. RESULTS AND DISCUSSION 35.6 35.8 36.0 362 36.4 36.6 dffractedaTg(e(2B) 36.8 37.0 35.6 35.8 36.0 36.8 37.0 362 36.4 36.6 Diffracted angle (28| FIGURE 1. Scattering spectra for the laser heated Silicon under single laser shot irradiation. The conditions are (a) power density of 5 GW/cm2 and the time delay of 250ps. (b) 10 GW/cm2, 350 ps. The circles are the experimental results, and the solid lines are calculated X-ray diffraction profiles. Single shot experiments Results of single laser shot irradiation experiments are shown in Fig 1. Figure 1. (a) shows scattering spectrum on the condition for laser irradiation with power density of 5 GW/cm2 at time delay 250ps. The X-ray diffraction peak was shifted to lower Bragg angles relative to the spectrum from the unirradiated crystal. Figure 1. (b) shows the result of X-ray diffraction under irradiation with power density of 10 GW/cm2. The new signal appeared at a higher diffracted angle. The strain profile inside the crystal can be estimated from the X-ray diffraction data, (a) In the case of irradiance of 5 GW/cm2, apparent diffraction signal at a lower angle corresponds to lattice expansion, (b) while new signals at higher angles observed in irradiance of 10 GW/cm2 provides evidence that lattice compression had occurred. X-ray diffraction was analyzed by a code based on dynamical diffraction theory and obtained strain distributions are shown in Fig 2. Figure 2. (a) indicates that thermal expansion due to laser heating occurred at this range in irradiance and delay time, and the maximum change in the strain and the surface temperature were estimated to be -0.5% and 1500 K, respectively. It was also suggested that the absorption coefficient of silicon is increasing to 1.2 X 104 cm"1, ten times as large as that to 780 nm light at 300 K. Similar laser-induced lattice expansion has been observed in Si. Larson et al4 studied time resolved X-ray diffraction of 15 ns laser irradiated Si at 0.1 GW/cm2 to find the lattice temperature in Si and observed thermal expansion due to the heating to reach the melting point. On the other hand, at a power density of 10 GW/cm2, the X-ray diffraction shows lattice 1376 Multiple shots experiments 0.5 Figure 3. shows the X-ray diffracted spectrum from the silicon (111) surface under multiple laser irradiations (300 shots) with a power density of 4 GW/cm2. Multiple shot experiments were performed for several sets of shots (20 - 300 shots) with the same power density at delay time 350 ps. In all experiments, the shifts of the diffracted spectrum to higher Bragg angle due to laser shocked compression were observed and strains were estimated to be ~ -1.4 %. The generation of shock compression was observed even at 20-shots as reduction of ablation threshold was induced by the surface damage in laser irradiated area. (a) 0.4 £ •£"0.3 I 02 0.1 0.0 I 1 2 3 4 Depth from the surface (urn) 0 1 2 3 4 0.0 -0.5 (b) £.1.0 2.0 -1.5 -20 11.5 -2.5 •e & 1.0 FIGURE 2. Strain Distributions under the surface of single shot irradiated Silicon. The conditions are (a) with power density of 5 GW/cm2 and the time delay 250ps. (b) 10 GW/cm2, 350 ps. 0.5 0.0 ——— 35.6 35.8 compression. The maximum compression of 2.1 % was estimated from the calculation. To account for the phenomena observed in the present experiments, the absorption coefficient was estimated using the values of laser energy density deposited in the sample, enthalpy changes, and latent heat of silicon. The observed shock compression in this experiment is due to laser ablation. The absorption depth of 780 nm light was estimated to be several hundreds of nanometers (~ 0.4 |xm). The ablation occurred in the thin surface layer (several hundreds of nanometer) at the power density of 10 GW/cm2 (2 J/cm2 for 300 ps pulsed laser). Pronko et al 9 reported that the pulsed laser (780nm, 300ps) induced dielectric breakdown threshold of silicon was ~3 J/cm2, which provides further evidence of laser ablation occurring in this range of laser irradiation. 36.0 36.2 36.4 Diffracted angle (2e) FIGURE 3. Typical X-ray diffraction spectrum on the Si (111) under multiple laser irradiation (300 shots) with power density of 4 GW/cm2. The time delay of the X-ray probe was 350ps. ACKNOWLEDGEMENT We thank Y. Okano, H. Kawano, and M. Hasegawa for their help on experiments and valuable discussions. This work has been supported by CREST (Core Research for Evolutional Science and Technology) program organized by Japan Science and Technology Corporation (JST). REFERENCES 1) Chin, A. H., Schoenlein, R. W., Glover, T. E., Balling, P., Leemans, W. P., and Shank, C. V, Phys. Rev. Lett. 83, 336-339 (1999). 2) Siders, C. 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