Picosecond–milliångström lattice dynamics measured by ultrafast X-ray diffraction

Christoph Rose-Petruck, Ralph Jimenez, Ting Guo, Andrea Cavalleri, Craig W. Siders, Ferenc Rksi, Jeff A. Squier, Barry C. Walker, Kent R. Wilson () and Christopher P. J. Barty
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Christoph Rose-Petruck: The University of California
Ralph Jimenez: The University of California
Ting Guo: The University of California
Andrea Cavalleri: The University of California
Craig W. Siders: The University of California
Ferenc Rksi: The University of California
Jeff A. Squier: The University of California
Barry C. Walker: The University of California
Kent R. Wilson: The University of California
Christopher P. J. Barty: The Institute for Nonlinear Science, The University of California

Nature, 1999, vol. 398, issue 6725, 310-312

Abstract: 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.

Date: 1999
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DOI: 10.1038/18631

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