Abstract
Fundamental processes on the molecular level, such as vibrations and rotations in single molecules, liquids or crystal lattices and the breaking and formation of chemical bonds, occur on timescales of femtoseconds to picoseconds. The electronic changes associated with such processes can be monitored in a time-resolved manner by ultrafast optical spectroscopic techniques1, but the accompanying structural rearrangements have proved more difficult to observe. Time-resolved X-ray diffraction has the potential to probe fast, atomic-scale motions2,3,4,5. This is made possible by the generation of ultrashort X-ray pulses6,7,8,9,10, and several X-ray studies of fast dynamics have been reported6,7,8,11,12,13,14,15. Here we report the direct observation of coherent acoustic phonon propagation in crystalline gallium arsenide using a non-thermal, ultrafast-laser-driven plasma — a high-brightness, laboratory-scale source of subpicosecond X-ray pulses16,17,18,19. We are able to follow a 100-ps coherent acoustic pulse, generated through optical excitation of the crystal surface, as it propagates through the X-ray penetration depth. The time-resolved diffraction data are in excellent agreement with theoretical predictions for coherent phonon excitation20 in solids, demonstrating that it is possible to obtain quantitative information on atomic motions in bulk media during picosecond-scale lattice dynamics.
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
Elsaesser, T., Fujimoto, J. G., Wiersma, D. A. & Zinth, W. (eds) Ultrafast Phenomena XI(Springer, Berlin, (1998).
Rentzepis, P. M. & Helliwell, J. R. (eds) Time-Resolved Diffraction(Oxford Univ. Press, (1997).
Bergsma, J. P. et al. Transient x-ray scattering calculated from molecular dynamics. J. Chem. Phys. 84, 6151–6160 (1986).
Wark, J. Time-resolved x-ray diffraction. Contemp. Phys. 37, 205–218 (1996).
Ben-Nun, M., Cao, J. S. & Wilson, K. R. Ultrafast x-ray and electron diffraction: Theoretical considerations. J. Phys. Chem. A 101, 8743–8761 (1997).
Larson, B. C., Tischler, J. Z. & Mills, D. M. Nanosecond resolution time-resolved x-ray study of silicon during pulsed-laser irradiation. J. Mater. Res. 1, 144–154 (1986).
Srajer, V. et al. Photolysis of the carbon monoxide complex of myoglobin: nanosecond time-resolved crystallography. Science 274, 1726–1729 (1996).
Chen, P., Tomov, I. V. & Rentzepis, P. M. Time resolved heat propagation in gold crystals by means of picosecond x-ray diffraction. J. Chem. Phys. 104, 10001–10007 (1996).
Schoenlein, R. W. et al. Femtosecond x-ray pulses at 0.4 Å generated by 90 degree Thomson scattering: a tool for probing the structural dynamics of materials. Science 274, 236–238 (1996).
Murnane, M. M., Kapteyn, H. C., Rosen, M. D. & Falcone, R. W. Ultrafast x-ray pulses from laser-produced pulses. Science 251, 531–536 (1991).
Rischel, C. et al. Femtosecond time-resolved X-ray diffraction from laser-heated organic films. Nature 390, 490–492 (1997).
Chin, A. H. et al. in Ultrafast Phenomena XI(eds Elsaesser, T., Fujimoto, J. G., Wiersma, D. A. & Zinth, W.) 401–403 (Springer, Berlin, (1998).
Buschert, J. R., Tischler, J. Z., Mills, D. M., Zhao, Q. & Corella, R. Time-resolved x-ray diffraction study of laser annealing in silicon at grazing-incidence. J. Appl. Phys. 66, 3523–3525 (1989).
Wark, J. S., Riley, D., Woolsey, N. C., Keihn, G. & Whitlock, R. R. Direct measurement of compressive and tensile strain during shock breakout by use of subnanosecond x-ray diffraction. J. Appl. Phys. 68, 4531–4534 (1990).
Larsson, J. et al. Ultrafast structural changes measured by time-resolved x-ray diffraction. Appl. Phys. A 66, 587–591 (1998).
Kieffer, J. -C. et al. Ultrafast x-ray sources. Phys. Fluids B 5, 2676–2681 (1993).
Rousse, A. et al. Efficient K alpha x-ray source from femtosecond laser-produced plasmas. Phys. Rev. E 50, 2200–2207 (1994).
Kmetec, J. D. et al. MeV x-ray generation with a femtosecond laser. Phys. Rev. Lett. 68, 1527–1530 (1992).
Gallant, P. et al. Subpicosecond time-resolved x-ray spectroscopy of plasmas produced by high intensity ultrashort laser pulses. Proc. SPIE 3157, 44–51 (1997).
Thomsen, C., Grahn, H. T., Maris, H. J. & Tauc, J. Surface generation and detection of phonons by picosecond light pulses. Phys. Rev. B 34, 4129–4138 (1986).
Blakemore, J. S. Semiconducting and other major properties of gallium arsenide. J. Appl. Phys. 53, R123–R181 (1981).
Shah, J. Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures(Springer, Berlin, (1996).
Shank, C. V., Yen, R. & Hirlimann, C. Femtosecond-time-resolved surface structural dynamics of optically excited silicon. Phys. Rev. Lett. 51, 900–902 (1983).
Saeta, P., Wang, J. -K., Siegal, Y., Bloembergen, N. & Mazur, E. Ultrafast electronic disordering during the femtosecond laser melting of GaAs. Phys. Rev. Lett. 67, 1023–1026 (1991).
Downer, M. C. & Shank, C. V. Ultrafast heating of silicon on sapphire by femtosecond optical pulses. Phys. Rev. Lett. 56, 761–764 (1986).
Strauss, U. & Ruhle, W. W. Auger recombination in intrinsic GaAs. Appl. Phys. Lett. 62, 55–57 (1993).
Takagi, S. Adynamical theory of diffraction for a distorted crystal. J. Phys. Soc. Jpn 26, 1239–1253 (1969).
Taupin, D. Théorie dynamique de la diffraction des rayon X par les cristaux déformés. Bull. Soc. Fr. Minér. Crist. 87, 469–511 (1964).
Larson, B. C., White, C. W., Noggle, T. S., Barhost, J. F. & Mills, D. M. Time-resolved x-ray diffraction measurement of the temperature and temperature gradients in silicon during pulsed laser annealing. Appl. Phys. Lett. 42, 282–284 (1983).
Barty, C. P. J. et al. Generation of 18-fs, multiterawatt pulses using regenerative pulse shaping and chirped pulse amplification. Opt. Lett. 21, 668–670 (1996).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Rose-Petruck, C., Jimenez, R., Guo, T. et al. Picosecond–milliångström lattice dynamics measured by ultrafast X-ray diffraction. Nature 398, 310–312 (1999). https://doi.org/10.1038/18631
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/18631
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.