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Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses

Abstract

Soon after it was discovered that intense laser pulses of nanosecond duration from a ruby laser could anneal the lattice of silicon, it was established that this so-called pulsed laser annealing is a thermal process. Although the radiation energy is transferred to the electrons, the electrons transfer their energy to the lattice on the timescale of the excitation. The electrons and the lattice remain in equilibrium and the laser simply 'heats' the solid to the melting temperature within the duration of the laser pulse. For ultrashort laser pulses in the femtosecond regime, however, thermal processes (which take several picoseconds) and equilibrium thermodynamics cannot account for the experimental data. On excitation with femtosecond laser pulses, the electrons and the lattice are driven far out of equilibrium and disordering of the lattice can occur because the interatomic forces are modified due to the excitation of a large (10% or more) fraction of the valence electrons to the conduction band. This review focuses on the nature of the non-thermal transitions in semiconductors under femtosecond laser excitation.

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Figure 1: Timescales of various electron and lattice processes in laser-excited solids (after ref. 10).
Figure 2: Electron and lattice excitation and relaxation processes in a laser-excited direct gap semiconductor. CB is the conduction band and VB the valence band.
Figure 3: Summary of the electronic and structural dynamics in GaAs on excitation with short laser pulses (after ref. 10).
Figure 4: Laser-induced lattice heating of crystalline GaAs at three different excitations below the threshold for irreversible changes Fth.
Figure 5: Thickness of the molten layer as function of the absorbed laser fluence.
Figure 6: Duration of the melting process as a function of the absorbed laser fluence.
Figure 7: Illustration of structural changes in the diamond structure of GaAs induced by longitudinal and transverse distortions.
Figure 8: Evolution of a diamond lattice during the first 100 fs after the excitation of a dense electron–hole plasma.

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Acknowledgements

Collaboration between the authors was made possible with support from the Department of Energy under the Environmental Management Science Program. We thank C. A. D. Roeser for a careful review of the manuscript and many helpful comments. S.K.S. acknowledges the support from the Pacific Northwest National Laboratory (PNNL) while writing this review. Battelle Memorial Institute operates PNNL for the United States Department of Energy under Contract DE-AC06-76RLO 1830.

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Sundaram, S., Mazur, E. Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses. Nature Mater 1, 217–224 (2002). https://doi.org/10.1038/nmat767

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