The ultrafast-laser-induced solid–liquid phase transition in metals is still not clearly understood and its accurate quantitative description remains a challenge. Here, we systematically investigated, both experimentally and theoretically, the melting of gold by single femto- and picosecond near-infrared laser pulses. Two laser systems with wavelengths of 800 and 1030 nm and pulse durations ranging from 124 fs to 7 ps were used, and the damage and ablation thresholds were determined for each irradiation condition. The theoretical analysis was based on two-temperature modeling. Different expressions for the electron–lattice coupling rate and contribution of ballistic electrons were examined. In addition, the number of free electrons involved in the optical response is suggested to be dependent on the laser intensity and the influence of the fraction of involved electrons on the damage threshold was investigated. Only one combination of modelling parameters was able to describe consistently all the measured damage thresholds. Physical arguments are presented to explain the modeling results.
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J. Wallace, Picosecond and femtosecond fiber lasers serve industry and science. Laser Focus World 56, 27–29 (2020)
R. Stoian, J.-P. Colombier, Advances in ultrafast laser structuring of materials at the nanoscale. Nanophotonics 9, 4665–4688 (2020)
B.C. Stuart, M.D. Feit, S. Herman, A.M. Rubenchik, B.W. Shore, M.D. Perry, Optical ablation by high-power short-pulse lasers. J. Opt. Soc. Am. B 13, 459–468 (1996)
S.-S. Wellershoff, J. Hohlfeld, J. Güdde, E. Matthias, The role of electron–phonon coupling in femtosecond laser damage of metals. Appl. Phys. A 69, S99–S107 (1999)
S.V. Starinskiy, Y.G. Shukhov, A.V. Bulgakov, Laser-induced damage thresholds of gold, silver and their alloys in air and water. Appl. Surf. Sci. 396, 1765–1774 (2017)
P. Balling, Laser coupling and relaxation of the absorbed energy: metals, semiconductors, and dielectrics, in Handbook of Laser Micro- and Nano-Engineering. ed. by K. Sugioka (Springer, Cham, 2021). https://doi.org/10.1007/978-3-319-69537-2_10-1
S.I. Anisimov, B.L. Kapeliovich, T.L. Perel’man, Electron emmision from metal surfaces exposed to ultrashort laser pulses. Sov. Phys. JETP 39, 375–377 (1974)
B. Rethfeld, D.S. Ivanov, M.E. Garcia, S.I. Anisimov, Modelling ultrafast laser ablation. J. Phys. D: Appl. Phys. 50, 193001 (2017)
M.V. Shugaev, M. He, S.A. Lizunov, Y. Levy, T.J.-Y. Derrien, V.P. Zhukov, N.M. Bulgakova, L.V. Zhigilei, Chapter 5, Insights into laser-materials interaction through modeling on atomic and macroscopic Scales, in Advances in the Application of Lasers in Materials Science, Springer Series in Materials Science, vol. 274, ed. by P.M. Ossi (Springer, 2018), pp. 107–148
C. Kittel, Introduction to Solid State Physics, 8th edn. (Wiley, 2004)
B. Rethfeld, A. Kaiser, M. Vicanek, G. Simon, Ultrafast dynamics of nonequilibrium electrons in metals under femtosecond laser irradiation. Phys. Rev. B 65, 214303 (2002)
B.Y. Mueller, B. Rethfeld, Relaxation dynamics in laser-excited metals under nonequilibrium conditions. Phys. Rev. B 87, 035139 (2013)
L. Jiang, H.-L. Tsai, Improved two-temperature model and its application in ultrashort laser heating of metal films. J. Heat Transfer 127, 1167–1173 (2005)
K.P. Migdal, D.K. Il’nitsky, Yu.V. Petrov, N.A. Inogamov, Equations of state, energy transport and two-temperature hydrodynamic simulations for femtosecond laser irradiated copper and gold. J. Phys. Conf. Ser. 653, 012086 (2015)
J. Winter, S. Rapp, M. Schmidt, H.P. Huber, Ultrafast laser processing of copper: A comparative study of experimental and simulated transient optical properties. Appl. Surf. Sci. 417, 2–15 (2017)
G.D. Tsibidis, The influence of dynamical change of optical properties on the thermomechanical response and damage threshold of noble metals under femtosecond laser irradiation. Phys. Rev. B 123, 085903 (2018)
Z. Lin, L.V. Zhigilei, V. Celli, Electron-phonon coupling and electron heat capacity of metals under conditions of strong electron-phonon nonequilibrium Phys. Rev. B 77, 075133 (2008)
M.Z. Mo, Z. Chen, R.K. Li, M. Dunning, B.B.L. Witte, J.K. Baldwin, L.B. Fletcher, J.B. Kim, A. Ng, R. Redmer, A.H. Reid, P. Shekhar, X.Z. Shen, M. Shen, K. Sokolowski-Tinten, Y.Y. Tsui, Y.Q. Wang, Q. Zheng, X.J. Wang, S.H. Glenzer, Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction. Science 360, 1451–1455 (2018)
N.A. Inogamov, Y.V. Petrov, Thermal conductivity of metals with hot electrons. JETP 110, 446–468 (2010)
S.D. Brorson, J.G. Fujimoto, E.P. Ippen, Femtosecond electronic heat-transport dynamics in thin gold films. Phys. Rev. Lett. 59, 1962–1965 (1987)
J. Güdde, J. Hohlfeld, J.G. Müller, E. Mattias, Damage threshold dependence on electron-phonon coupling in Au and Ni films. Appl. Surf. Sci. 127–129, 40–45 (1998)
X. Ni, C. Wang, L. Yang, J. Li, L. Chai, W. Jia, R. Zhang, Z. Zhang, Parametric study on femtosecond laser pulse ablation of Au films. Appl. Surf. Sci. 253, 1616–1619 (2006)
M.E. Shaheen, J.E. Gagnon, B.J. Fryer, Femtosecond laser ablation behaviour of gold, crystalline silicon, and fused silica: a comparative study. Laser Phys. 24, 106102 (2014)
A.A. Ionin, S.I. Kudryashov, S.V. Makarov, A.O. Levchenko, A.A. Rudenko, I.N. Saraeva, D.A. Zayarny, C.R. Nathala, W. Husinsky, Nanoscale surface boiling in sub-threshold damage and above-threshold spallation of bulk aluminium and gold by single femtosecond laser pulses. Laser Phys. Lett. 13, 025603 (2016)
Y.J. Li, X.L. Liu, B.B. Sun, Measurement of ultrafast laser damage threshold on optical materials. Proc. SPIE 11562, 115620T (2020)
G. de Haan, J. Hernandez-Rueda, P.C.M. Planken, Femtosecond time-resolved pump-probe measurements on percolated gold in the ablation regime. Opt. Express 28, 12093–12107 (2020)
H.E. Bennett, J.O. Porteus, Relation between surface roughness and specular reflectance at normal incidence. J. Opt. Soc. Am. 51, 123–129 (1961)
C.-D. Wen, I. Mudawar, Modeling the effects of surface roughness on the emissivity of aluminum alloys. Int. J. Heat Mass Transf. 49, 4279–4289 (2006)
E.D. Palik, Handbook of Optical Constants of Solids (Academic Press, 1985)
A.V. Bulgakov, I. Mirza, N.M. Bulgakova, V.P. Zhukov, R. Machulka, O. Haderka, E.E.B. Campbell, T. Mocek, Initiation of air ionization by ultrashort laser pulses: evidence for a role of metastable–state air molecules. J. Phys. D: Appl. Phys. 51, 25LT02 (2018)
N.M. Bulgakova, V.P. Zhukov, A.Y. Vorobyev, C. Guo, Modeling of residual thermal effect in femtosecond laser ablation of metals: role of a gas environment. Appl. Phys. A 92, 883–889 (2008)
J.M. Liu, Simple technique for measurements of pulsed Gaussian-beam spot sizes. Opt. Lett. 7, 196–198 (1982)
S.V. Starinskiy, A.A. Rodionov, Y.G. Shukhov, E.A. Maximovskiy, A.V. Bulgakov, Dynamics of nanosecond-laser-induced melting of tin in vacuum, air, and water. Appl. Phys. A 125, 734 (2019)
S. Preuss, A. Demchuk, M. Stuke, Sub-picosecond UV laser ablation of metals. Appl. Phys. A 61, 33–37 (1995)
M.I. Kaganov, I.M. Lifshitz, M.V. Tanatarov, Relaxation between electrons and the crystalline lattice. Sov. Phys. JETP 4, 173–178 (1957)
R.H.M. Groeneveld, R. Sprik, A. Lagendijk, Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au. Phys. Rev. B 51, 11433 (1995)
C. Suárez, W.E. Bron, T. Juhasz, Dynamics and transport of electronic carriers in thin gold films. Phys. Rev. Lett. 75, 4536–4539 (1995)
J. Hohlfeld, S.-S. Wellershoff, J. Güdde, U. Conrad, V. Jähnke, E. Matthias, Electron and lattice dynamics following optical excitation of metals. Chem. Phys. 251, 237–258 (2000)
J.K. Chen, J.E. Beraun, C.L. Tham, Investigation of thermal response caused by pulsed laser heating. Numer. Heat Transf. A 44, 705–722 (2003)
The authors thank Dr. J. Bonse for providing the bulk gold target. This work was supported by the European Regional Development Fund and the state budget of the Czech Republic (Project BIATRI: No. CZ.02.1.01/0.0/0.0/15_003/0000445). S. A. L. and A. V. B. also acknowledge financial support from the Russian Foundation for Basic Research (Project No. 19-38-90203).
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Lizunov, S.A., Bulgakov, A.V., Campbell, E.E.B. et al. Melting of gold by ultrashort laser pulses: advanced two-temperature modeling and comparison with surface damage experiments. Appl. Phys. A 128, 602 (2022). https://doi.org/10.1007/s00339-022-05733-4