Abstract
Ultrafast time-resolved optical spectroscopy has revealed new classes of physical1, chemical2 and biological3 reactions, in which directed, deterministic motions of atoms have a key role. This contrasts with the random, diffusive motion of atoms across activation barriers that typically determines kinetic rates on slower timescales. An example of these new processes is the ultrafast melting of semiconductors, which is believed to arise from a strong modification of the inter-atomic forces owing to laser-induced promotion of a large fraction (10% or more) of the valence electrons to the conduction band1,4,5,6,7,8,9,10,11,12. The atoms immediately begin to move and rapidly gain sufficient kinetic energy to induce melting—much faster than the several picoseconds required to convert the electronic energy into thermal motions13. Here we present measurements of the characteristic melting time of InSb with a recently developed technique of ultrafast time-resolved X-ray diffraction14,15,16,17,18,19 that, in contrast to optical spectroscopy, provides a direct probe of the changing atomic structure. The data establish unambiguously a loss of long-range order up to 900 Å inside the crystal, with time constants as short as 350 femtoseconds. This ability to obtain the quantitative structural characterization of non-thermal processes should find widespread application in the study of ultrafast dynamics in other physical, chemical and biological systems.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Shank, C. V., Yen, R. & Hirlimann, C. Femtosecond time-resolved surface structural dynamics of optically excited silicon. Phys. Rev. Lett. 51, 900–902 (1983).
Zewail, A. H. Femtochemistry: recent progress in studies of dynamics and control of reactions and their transition states. J. Phys. Chem. 100, 12701–12724 (1996).
Vos, M. H. & Martin, J.-L. Femtosecond processes in proteins. Biochim. Biophys. Acta Bioenerget. 1411, 1–20 (1999).
Wood, R. F., White, C. W. & Young, R. T. (eds) in Pulsed Laser Processing of Semiconductors (Academic, Orlando, 1984).
Shank, C. V., Yen, R. & Hirlimann, C. Time-resolved reflectivity of femtosecond-optical-pulse-induced phase transitions in silicon. Phys. Rev. Lett. 50, 454–520 (1983).
Huang, L., Callan, J. P., Glezer, E. N. & Mazur, E. GaAs under intense ultrafast excitation: Response of the dielectric function. Phys. Rev. Lett. 80, 185–188 (1998).
Sokolowski-Tinten, K., Bialkowski, J. & von der Linde, D. Ultrafast laser-induced order–disorder transitions in semiconductors. Phys. Rev. B 51, 14186–14198 (1995).
Sokolowski-Tinten, K., Schulz, H., Bialkowski, J. & von der Linde, D. Two distinct transitions in ultrafast solid-liquid phase transformations of GaAs. Appl. Phys. A 53, 227–234 (1991).
Shumay, I. L. & Höfer, U. Phase transformations of an InSb surface induced by strong femtosecond laser pulses. Phys. Rev. B 53, 15878–15884 (1996).
Stampfli, P. & Bennemann, K. H. Theory for the laser-induced femtosecond phase transition of silicon and GaAs. Appl. Phys. A 60, 191–196 (1995).
Silvestrelly, P. L., Alavi, A., Parrinello, M. & Frenkel, D. Ab initio molecular dynamics simulation of laser melting of silicon. Phys. Rev. Lett. 77, 3149–3152 (1996).
Graves, J. S. & Allen, R. E. Response of GaAs to fast intense laser pulse. Phys Rev. B 58, 13627–13633 (1999).
Laude, L. D. Cohesive Properties of Semiconductors Under Laser Irradiation. (NATO ASI Series Martinus Nijhoff Vol. 69, The Hague, 1983).
Rischel, C. et al. Femtosecond time-resolved X-ray diffraction from laser-heated organic films. Nature 390, 490–492 (1997).
Rose-Petruck, C. et al. Picosecond-milliangström lattice dynamics measured by ultrafast X-ray diffraction. Nature 398, 310–312 (1999).
Larsson, J. et al. Ultrafast structural changes measured by time-resolved X-ray diffraction. Appl. Phys. A 66, 587–591 (1998).
Chin, A. H. et al. Ultrafast structural dynamics in InSb probed by time-resolved X-ray diffraction. Phys. Rev. Lett. 83, 336–339 (1999).
Siders, C. W. et al. Detection of non-thermal melting by ultrafast x-ray diffraction. Science 286, 1340–1342 (1999).
Lindenberg, A. M. et al. Time-resolved X-ray diffraction from coherent phonons during a laser-induced phase transition. Phys. Rev. Lett. 84, 111–114 (2000).
Phillpot, S. R., Yip, S. & Wolf, D. How do crystals melt ? Comput. Phys. 3, 20–31 (1989).
Hellwege, K. H. (ed.) in Landolt-Börnstein Semiconductors Vol. 17-a Group IV elements and III-V Compounds (Springer, Berlin, 1991).
Yoffa, E. J. Dynamics of dense laser-induced plasmas. Phys. Rev. B 21, 2415–2425 (1980).
Vetelino, J. F., Gaur, S. P. & Mitra, S. S. Debye–Waller factor for zinc-blende-type crystals. Phys. Rev. B 5, 2360–2366 (1971).
Sokolowski-Tinten, K. et al. Transient states of matter during short laser pulse ablation. Phys. Rev. Lett. 81, 224–227 (1998).
Aspnes, D. E. & Studna, A. A. Dielectric functions and optical parameters of Si, Ge, GaP, GaAs, GaSb, InP, InAs, and InSb from 1.5 to 6 eV. Phys. Rev. B 27, 985–1008 (1983).
Thomsen, C., Grahn, H. T., Maris, H. J. & Tauc, J. Surface generation and detection of phonons by picosecond light pulses. Phys. Rev. B 34, 4129–4137 (1986).
Liebl, U. et al. Coherent reaction dynamics in a bacterial cytochrome c oxidase. Nature 401, 181–184 (1999).
Pronko, P. P., Dutta, S. K., Du, D. & Singh, R. K. Thermophysical effects in laser processing of materials with picosecond and femtosecond pulses. J. Appl. Phys. 78, 6233–6240 (1995).
Acknowledgements
We thank G. Hamoniaux, P. Rousseau, K. Ta Phuoc and A. Alexandrou from the Laboratoire d’Optique Appliquée, and T. Moreno from Caminotec Inc, for support; and Veeco Instruments Inc. and A. Semerok from CEA-Saclay for the use of the atomic force microscope (AFM) and the profilers. This work was supported by the European Community.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Rousse, A., Rischel, C., Fourmaux, S. et al. Non-thermal melting in semiconductors measured at femtosecond resolution. Nature 410, 65–68 (2001). https://doi.org/10.1038/35065045
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/35065045
This article is cited by
-
Nanoscale reshaping of resonant dielectric microstructures by light-driven explosions
Nature Communications (2023)
-
Structural measurement of electron-phonon coupling and electronic thermal transport across a metal-semiconductor interface
Scientific Reports (2022)
-
Superionic states formation in group III oxides irradiated with ultrafast lasers
Scientific Reports (2022)
-
The critical role of hot carrier cooling in optically excited structural transitions
npj Computational Materials (2021)
-
Direct treatment of interaction between laser-field and electrons for simulating laser processing of metals
Scientific Reports (2021)
Comments
By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.