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  • Print publication year: 2009
  • Online publication date: December 2009

6 - Ultrafast-laser interactions with materials



Lasers that can produce coherent photon pulses with durations in the femtosecond regime have opened up new frontiers in materials research with extremely short temporal resolution and high photon intensity. The ultrafast nature of femtosecond lasers has been used to observe, in real time, phenomena including chemical reactions in gases (Zewail, 1994) and electron–lattice energy transfer in solids (Shah, 1996). On the other hand, ultra-short laser pulses impart extremely high intensities and provide precise laser-ablation thresholds at substantially reduced laser energy densities. The increasing availability of intense femtosecond lasers has sparked a growing interest in high-precision materials processing. In contrast to material modification using nanosecond or longer laser pulses, for which standard modes of thermal processes dominate, there is no heat exchange between the pulse and the material during femtosecond-laser–material interactions. As a consequence, femtosecond laser pulses can induce nonthermal structural changes driven directly by electronic excitation and associated nonlinear processes, before the material lattice has equilibrated with the excited carriers. This fast mode of material modification can result in vanishing thermal stress and minimal collateral damage for processing practically any solid-state material. Additionally, damage produced by femtosecond laser pulses is far more regular from shot to shot. These breakdown characteristics make femtosecond lasers ideal tools for precision material processing.

Thorough knowledge of the short-pulse-laser interaction with the target material is essential for controlling the resulting modification of the target's topography.

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Agassi, D., 1984, “Phenomenological Model for Picosecond-Pulse Laser Annealing of Semiconductors,” J. Appl. Phys., 55, 4376–4383.
Anisimov, S. I., Kapeliovich, B. L., and Perel'man, T. L., 1974, “Electron Emission from Metal Surfaces Exposed to Ultrashort Laser Pulses,” Sov. Phys. JETP, 39, 375–377.
Anisimov, S. I., and Rethfeld, B., 1997, “On the Theory of Ultrashort Laser Pulse Interaction with a Metal,” Proc. SPIE, 3093, 192–203.
Arnold, D., and Cartier, E., 1992, “Theory of Laser-Induced Free-Electron Heating and Impact Ionization in Wide-Band-Gap Solids,” Phys. Rev. B, 46, 15102–15115.
Bespalov, V. I., and Talanov, V. I., 1966, “Filamentary Structure of Light Beams in Nonlinear Liquids,” JETP Lett., 3, 307.
Bloembergen, N., 1974, “Laser-Induced Electric Breakdown in Solids,” IEEE J. Quant. Electron., QE-10, 375–386.
Braun, A., Korn, G., Liu, al., 1995, “Self-Channeling of High-Peak-Power Femtosecond Laser Pulses in Air,” Opt. Lett., 20, 73–75.
Brodeur, A., Chien, C. Y., Ilkov, F. al., 1997, “Moving Focus in the Propagation of Ultrashort Laser Pulses in Air,” Opt. Lett., 22, 304–306.
Brorson, S. D., Fujimoto, J. G., and Ippen, E. P., 1987, “Femtosecond Electronic Heat-Transport Dynamics in Thin Gold Films,” Phys. Rev. Lett., 59, 1962–1965.
Brorson, S. D., Kazeroonian, A., Moodera, J. al., 1990, “Femtosecond Room-Temperature Measurement of the Electron–Phonon Coupling Constant l in Metallic Superconductors,” Phys. Rev. Lett., 64, 2172–2175.
Cavalleri, A., Siders, C. W., Brown, F. L. al., 2000, “Anharmonic Lattice Dynamics in Germanium Measured with Ultrafast X-Ray Diffraction,” Phys. Rev. Lett., 85, 586–589.
Cheng, C., and Xu, X., 2005, “Material Decomposition near Critical Temperature during Femtosecond Laser Ablation,” Phys. Rev. B, 72, 165415-1–15.
Chin, A. H., Schoenlein, R. W., Glover, T. al., 1999, “Ultrafast Structural Dynamics in InSb Probed by Time-Resolved X-Ray Diffraction,” Phys. Rev. Lett., 83, 336–339.
Choi, T.-Y., and Grigoropoulos, C. P., 2002, “Plasma and Ablation Dynamics in Ultrafast Laser Processing of Crystalline Silicon,” J. Appl. Phys., 92, 4918–4925.
Davis, K. M., Miura, K., Sugimoto, N., and Hirao, K., 1996, “Writing Waveguides in Glass with a Femtosecond Laser”, Opt. Lett., 21, 1729–1731.
Day, D., Min, Gu, and Smallridge, A., 1999, “Use of Two-photon Excitation for Erasable–Rewritable Three-Dimensional Bit Optical Data Storage in a Photorefractive Polymer,” Opt. Lett., 24, 948–950.
Diddams, S. A., Eaton, H. K., Zozulya, A. A., and Clement, T. S., 1998, “Characterizing the Nonlinear Propagation of Femtosecond Pulses in Bulk Media,” IEEE J. Sel. Topics Quant. Electron., 4, 306–316.
Downer, M., Fork, R., and Shank, C., 1985, “Femtosecond Imaging of Melting and Evaporation at a Photoexcited Silicon Surface,” J. Opt. Soc. Am. B, 2, 595–599.
Du, D., Liu, X., Korn, G., Squier, J., and Mourou, G., 1994, “Laser-Induced Breakdown by Impact Ionization in SiO2 with Pulse Widths from 7 ns to 150 fs,” Appl. Phys. Lett., 64, 3071–3073.
Elsayed-Ali, H. E., Norris, T. B., Pessot, M. A., and Mourou, G. A., 1987, “Time-Resolved Observation of Electron–Phonon Relaxation in Copper,” Phys. Rev. Lett., 58, 1212–1215.
Fann, W. S., Storz, R., Tom, H. W. K., and Bokor, J., 1992a, “Direct Measurement of Nonequilibrium Electron-Energy Distributions in Subpicosecond Laser-Heated Gold Films,” Phys. Rev. Lett., 68, 2834–2837.
Fann, W. S., Storz, R., Tom, H. W. K., and Bokor, J., 1992b, “Electron Thermalization in Gold,” Phys. Rev. B, 46, 13592–13595.
Fibich, G., and Ilan, B., 2001, “Vectorial and Random Effects in Self-Focusing and in Multiple Filamentation,” Physica D, 157, 112–146.
Fischetti, M. V., DiMaria, D. J., Brorson, S. D., Theis, T. N., and Kirtley, J. R., 1985, “Theory of High-Field Electron Transport in Silicon Dioxide,” Phys. Rev. B, 31, 8124–8142.
Gaeta, A. L., 2000, “Catastrophic Collapse of Ultrashort Pulses,” Phys. Rev. Lett., 84, 3582–3585.
Geindre, J.-P., Audebert, P., Rebibo, S., and Gauthier, J.-C., 2001, “Single-Shot Spectral Interferometry with Chirped Pulses,” Opt. Lett., 26, 1612–1616.
Gibbon, P., and Forster, E., 1996, “Short-Pulse Laser–Plasma Interactions,” Plasma Phys. Contr. Fusion, 38, 769–793.
Glezer, E. N., Milosavljevic, M., Huang, al., 1996, “Three-Dimensional Optical Storage inside Transparent Materials,” Opt. Lett., 21, 2023–2025.
Groeneveld, R. H. M., Sprik, R., Wittebrood, M., and Lagendijk, A., 1992, “Effect of a Nonthermal Electron Distribution on the Electron–Phonon Energy Relaxation Process in Noble Metals,” Phys. Rev. B, 45, 5079–5082.
Guizard, S., Martin, P., Petite, G., D'Oliveira, P., and Meynadier, P., 1996, “Time-Resolved Study of Laser-Induced Colour Centres in SiO2,” J. Phys. – Condens. Matter, 8, 1281–1290.
Guo, C., Rodriguez, G., and Taylor, A. J., 2001, “Ultrafast Dynamics of Electron Thermalization in Gold,” Phys. Rev. Lett., 86, 1638–1641.
Haglund, R. F. Jr., and Itoh, N., 1994, “Electronic Processes in Laser Ablation of Semiconductors and Insulators,” in Laser Ablation. Principles and Applications, edited by Miller, J. C., Berlin, Springer-Verlag, pp. 11–52.
Hwang, D., Choi, T., and Grigoropoulos, C. P., 2004, “Liquid-Assisted Femtosecond Laser Drilling of Straight and Three-Dimensional Microchannels in Glass,” Appl. Phys. A, 79, 605–612.
Hwang, D. J., Choi, T.-Y., and Grigoropoulos, C. P., 2006, “Efficiency of Silicon Micromachining by Femtosecond Laser Pulses in Ambient Air,” J. Appl. Phys., 99, 083101–083106.
Iaconis, C., andWalmsley, I. A., 1998, “Spectral Phase Interferometry for Direct Electric-Field Reconstruction of Ultrashort Optical Pulses, Opt. Lett., 23, 792–796.
Kawata, S., and Sun, H. B., 2003, “Two-Photon Photopolymerization as a Tool for Making Micro-devices”, Appl. Surf. Sci., 208, 153–158.
Kawata, Y., Ueki, H., Hastimoto, Y., and Kawata, S., 1995, Three-Dimensional Optical Memory with a Photorefractive Crystal,” Appl. Opt., 34, 4105–4110.
Kelley, P. L., 1965, “Self-Focusing of Optical Beams,” Phys. Rev. Lett., 15, 1005–1008.
Keldysh, L. V., 1965, “Ionization in Field of a Strong Electromagnetic Wave,” Sov. Phys. JETP, 20, 1307.
Kelly, R., and Miotello, A., 1996, “Comments on Explosive Mechanisms of Laser Sputtering,” Appl. Surf. Sci., 96–98, 205–215.
Korte, F., Nolte, S., Chichkov, B. al., 1999, “Far-Field and Near-Field Material Processing with Femtosecond Laser Pulses,” Appl. Phys. A, 69, S7–S11.
Larsson, J., Heimann, P. A., Lindenberg, A. al., 1998, “Ultrafast Structural Changes Measured by Time-Resolved X-Ray Diffraction,” Appl. Phys. A, 66, 587–591.
Lenzner, M., 1999, “Femtosecond Laser-Induced Damage of Dielectrics,” Int. J. Mod. Phys. B, 13, 1559–1578.
Lenzner, M., Krüger, J., Santania, al., 1998, “Femtosecond Optical Breakdown in Dielectrics,” Phys. Rev. Lett., 80, 4076–4079.
Li, M., Menon, S., Nibarger, J. P., and Gibson, G. N., 1999, “Ultrafast Electron Dynamics in Femtosecond Optical Breakdown of Dielectrics,” Phys. Rev. Lett., 82, 2394–2397.
Li, Y., Itoh, K., Watanabe, al., 2001, “Three-Dimensional Hole Drilling of Silica Glass from the Rear Surface with Femtosecond Laser Pulses,” Opt. Lett., 26, 1912–1914.
Lindenberg, A. M., Kang, J., Johnson, S. L., 2000, “Time-Resolved X-Ray Diffraction from Coherent Phonons during a Laser-Induced Phase Transition,” Phys. Rev. Lett., 84, 111–116.
Liu, X., Du, D., and Mourou, G., 1997, “Laser Ablation and Micromachining with Ultrashort Laser Pulses,” IEEE J. Quant. Electron., 33, 1706–1716.
Mao, X. L., Mao, S. S., and Russo, R. E., 2003, “Imaging Femtosecond Laser-Induced Electronic Excitation in Glass,” Appl. Phys. Lett., 82, 697–699.
Mao, S.S., Quéré, F., Guizard, al., 2004, “Dynamics of Femtosecond Laser Interactions with Dielectrics,” Appl. Phys. A, 79, 1695–1709.
Marcinkevicius, A., Juodkazis, S., Watanabe, al., 2001, “Femtosecond Laser-Assisted Three-Dimensional Microfabrication in Silica,” Opt. Lett., 26, 277–279.
Martin, P., Guizard, S., Daguzan, al., 1997, “Subpicosecond Study of Carrier Trapping Dynamics in Wide-Band-Gap Crystals,” Phys. Rev. B, 55, 5799–5810.
Milchberg, H. M., Freeman, R. R., and Davey, S. C., 1988, “Behavior of a Simple Metal under Utrashort Pulse High Intensity Laser Illumination,” Proc. SPIE, 913, 159–163.
Momma, C., Nolte, S., Kamlage, G., Alvensleben, F., and Tunnermann, A., 1998, “Beam Delivery of Femtosecond Laser Radiation by Diffractive Optical Elements,” Appl. Phys. A, 67, 517–520.
Perry, M. D., Stuart, B. C., Banks, P. al., 1999, “Ultrashort-Pulse Laser Machining of Dielectric Materials,” J. Appl. Phys., 85, 6803–6810.
Petite, G., Guizard, S., Martin, P., and Quéré, F., 1999, “Comment on ‘Ultrafast Electron Dynamics in Femtosecond Optical Breakdown of Dielectrics,’”Phys. Rev. Lett., 83, 5182.
Pronko, P., Dutta, S., Squier, al., 1995, “Machining of Sub-micron Holes using a Femtosecond Laser at 800 nm,” Opt. Commun., 114, 106–110.
Pronko, P. P., VanRompay, P.A, Horvath, al., 1998, “Avalanche Ionization and Dielectric Breakdown in Silicon with Ultrafast Laser Pulses,” Phys. Rev. B, 58, 2387–239.
Qiu, T. Q., and Tien, C.-L., 1993, “Heat Transfer Mechanisms During Short-Pulse Laser Heating of Metals,” J. Heat Transfer, 115, 835–841.
Quéré, F., Guizard, S., and Martin, P., 2001, “Time-Resolved Study of Laser-Breakdown in Dielectrics,” Europhys. Lett., 56, 138–144.
Quéré, F., Itatani, J., Yudin, G. L., and Corkum, R. B., 2003, “Attosecond Spectral Shearing Interferometry, Phys. Rev. Lett., 90, 073902-1–6.
Ranka, J. K., and Gaeta, A. L., 1998, “Breakdown of the Slowly Varying Envelope Approximation in the Self-Focusing of Ultrashort Pulses,” Opt. Lett., 23, 534–536.
Rethfeld, B., Kaiser, A., Vicanek, M., and Simon, G., 1999, “Femtosecond Laser-Induced Heating of Electron Gas in Aluminum,” Appl. Phys. A, 69, 109–112.
Rethfeld, B., Kaiser, A., Vicanek, M., and Simon, G., 2002, “Ultrafast Dynamics of Nonequilibrium Electrons in Metals under Femtosecond Laser Irradiation,” Phys. Rev. B, 65, 214303-11.
Rose-Petruck, C., Jimenez, R., Guo, al., 1999, “Picosecond–Milliångström Lattice Dynamics Measured by Ultrafast X-Ray Diffraction,” Nature, 398, 310–312.
Schaffer, C. B., Brodeur, A., Garcia, J. F., and Mazur, E., 2001, “Micromachining Bulk Glass by Use of Femtosecond Laser Pulses with Nanojoule Energy,” Opt. Lett., 26, 93–95.
Seideman, T., Ivanov, M. Yu, and Corkum, P. B., 1995, “Role of Electron Localization in Intense-Field Molecular Ionization,” Phys. Rev. Lett., 75, 2819–2822.
Shah, J., 1996, Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures, Berlin, Springer-Verlag.
Shank, C. V., Yen, R., and Hirlimann, C., 1983, “Time-Resolved Reflectivity Measurements of Femtosecond-Optical-Pulse-Induced Phase Transitions in Silicon,” Phys. Rev. Lett., 50, 454–457.
Shen, Y. R., 1984, The Principles of Nonlinear Optics, New York, Wiley.
Shibata, T., Iwai, S., Tokisaki, al., 1994, “Femtosecond Spectroscopic Studies of the Lattice-Relaxation Initiated by Interacting Electron–Hole Pairs under Relaxation in Alkali-Halides,” Phys. Rev. B, 49, 13255–13258.
Siders, C. W., Cavalleri, A., Sokolowski-Tinten, al., 1999, “Detection of Nonthermal Melting by Ultrafast X-Ray Diffraction,” Science, 286, 1340–1342.
Silvestrelli, P. L., Alavi, A., Parrinello, M., and Frenkel, D., 1996, “Ab Initio Molecular Dynamics Simulation of Laser Melting of Silicon,” Phys. Rev. Lett., 77, 3149–3152.
Skripov, V. P., and Skripov, A. V., 1979, “Spinodal Decomposition (Phase-Transition via Unstable States),” Usp. Fiz. Nauk, 128, 193–231.
Sokolowski-Tinten, K., Bialkowski, J., and der Linde, D., 1995, “Ultrafast Laser-Induced Order–Disorder Transitions in Semiconductors,” Phys. Rev. B, 51, 14186–14198.
Sokolowski-Tinten, K., Cavalleri, A., and der Linde, D., 1999, “Single-Pulse Time- and Fluence-Resolved Optical Measurements at Femtosecond Excited Surfaces,” Appl. Phys. A, 69, 577–579.
Sokolowski-Tinten, K., and der Linde, D., 2000, “Generation of Dense Electron–Hole Plasmas in Silicon,” Phys. Rev. B, 61, 2643–2650.
Song, K. H., and Xu, X., 1998, “Explosive Phase Transformation in Excimer Laser Ablation,” Appl. Surf. Sci., 127, 111–116.
Song, K. S., and Williams, R. T., 1993, Self-Trapped Excitons, Berlin, Springer-Verlag.
Stampfli, P., and Bennemann, K. H., 1990, “Theory for the Instability of the Diamond Structure of Si, Ge, and C Induced by a Dense Electron–Hole Plasma,” Phys. Rev. B, 42, 7163–7173.
Stampfli, P., and Bennemann, K. H., 1992, “Dynamical Theory of the Laser-Induced Lattice Instability of Silicon,” Phys. Rev. B, 46, 10686–10692.
Stuart, B. C., Feit, M. D., Herman, al., 1995, “Laser-Induced Damage in Dielectrics with Nanosecond to Subpicosecond Pulses,” Phys. Rev. Lett., 74, 2248–2251.
Stuart, B. C., Feit, M. D., Herman, al., 1996, “Nanosecond-to-Femtosecond Laser-Induced Breakdown in Dielectrics,” Phys. Rev. B, 53, 1749–1761.
Sun, H.-B., Xu, Y., Juodkazis, al., 2001, “Arbitrary-Lattice Photonic Crystals Created by Multiphoton Microfabrication,” Opt. Lett., 26, 325–327.
Sundaram, S. K., and Mazur, E., 2002, “Inducing and Probing Non-thermal Transitions in Semiconductors using Femtosecond Laser Pulses,” Nature Mater., 1, 217–224.
Thoma, E. D., Yochum, H. M., and William, R. T., 1997, “Subpicosecond Spectroscopy of Hole and Exciton Self-Trapping in Alkali-Halide Crystals,” Phys. Rev. B, 56, 8001–8011.
Tien, An-Chun, Backus, S., Kapteyn, H., Murnane, M., and Mourou, G., 1999, “Short-Pulse Laser Damage in Transparent Materials as a Function of Pulse Duration,” Phys. Rev. Lett., 82, 3883–3886.
Toyozawa, Y., 1980, Relaxation of Elementary Excitations, edited by Kubo, R. and Hanamura, E., Berlin, Springer-Verlag, pp. 3–18.
Trukhin, A. N., 1992, “Excitons in SiO2: A Review,” J. Non-Cryst. Solids, 149, 32–45.
Tzortzakis, S., Sudrie, L., Franco, al., 2001, Self-Guided Propagation of Ultrashort IR Laser Pulses in Fused Silica,” Phys. Rev. Lett., 87, 213902/1–4
Ueta, M., Kanzaki, H., Kobayashi, K., Toyozawa, Y., and Hanamura, E., eds., 1986, Excitonic Processes in Solids, Berlin, Springer-Verlag.
Driel, H. M., 1987, “Kinetics of High-Density Plasmas Generated in Si by 1.06- and 0.53-μm Picosecond Laser Pulses,” Phys. Rev. B, 35, 8166–8176.
Stryland, E. W., Vanherzeele, H., Woodall, M. al., 1985, “Two Photon Absorption, Nonlinear Refraction, and Optical Limiting in Semiconductors,” Opt. Eng., 24, 613–623.
Vechten, J., Tsu, R., and Saris, F., 1979, “Nonthermal Pulsed Laser Annealing of Si, Plasma Annealing,” Phys. Lett. A, 74, 422–426.
Vasil'ev, A. N., Fang, Y., and Mikhailin, V. V. 1999, “Impact Production of Secondary Electronic Excitations in Insulators: Multiple-Parabolic-Branch Band Model,” Phys. Rev. B, 60, 5340–5347.
der Linde, D., Sokolowski-Tinten, K., Blome, al., 2001, “Generation and Application of Ultrashort X-Ray Pulses,” Laser Part. Beams, 19, 15–22.
Will, M., Nolte, S., Chichkov, B. N., and Tünnermann, A., 2002, “Optical Properties of Waveguides Fabricated in Fused Silica by Femtosecond Laser Pulses,” Appl. Opt., 41, 4360–4364.
Williams, R. T., Craig, B. B., and Faust, W. L., 1984, “F-Center Formation in NaCl – Picosecond Spectroscopic Evidence for Halogen Diffusion on the Lowest Excitonic Potential Surface,” Phys. Rev. Lett., 52, 1709–1712.
Wu, M., 1997, “Micromachining for Optical and Optoelectronic Systems,” Proc. IEEE, 85, 1833–1856.
Xu, X., 2001, “Heat Transfer and Phase Change during High Power Pulsed Laser Ablation of Metal,” in Annual Review of Heat Transfer, edited by Tien, C.-L., Prasad, V., and Incropera, F. P., 12, New York, Begell House, 79.
Ye, M., and Grigoropoulos, C. P., 2001, “Time-of-Flight and Emission Spectroscopy Study of Femtosecond Laser Ablation of Titanium,” J. Appl. Phys., 89, 5183–5190.
Yoo, K. M.Zhao, X. M., Siddique, al., 1990, “Femtosecond Thermal Modulation Measurements of Electron–Phonon Relaxation in Niobium,” Appl. Phys. Lett., 56, 1908–1910.
Zewail, A. H., 1994, Femtochemistry: Ultrafast Dynamics of the Chemical Bond, Singapore, World Scientific.
Ziman, J. M., 1964, Principles of the Theory of Solids, Cambridge, Cambridge University Press.
Zozulya, A. A., Diddams, S. A., Engen, A. G., and Clement, T. S., 1999, “Propagation Dynamics of Intense Femtosecond Pulses: Multiple Splittings, Coalescence, and Continuum Generation,” Phys. Rev. Lett., 82, 1430–1433.