Time-resolved studies of laser-induced phase transitions in GaAs


This thesis describes a series of time-resolved experiments of the linear and nonlinear optical properties of GaAs during laser-induced phase transitions. The first set of experiments consists of a direct determination of the behavior of the linear dielectric constant at photon energies of 2.2 eV and 4.4 eV following excitation of the sample with 1.9-eV, 70-fs laser pulses spanning a fluence range from 0 to 2.5 kJ/m2. The results from this set of experiments were used to extract the behavior of the second-order optical susceptibility from second-harmonic generation measurements made under identical excitation conditions. These experiments are unique because they provide explicit information on the behavior of intrinsic material properties - the linear and nonlinear optical susceptibilities - during laser- induced phase transitions in semiconductors without the ambiguities in interpretation that are generally inherent in reflectivity and second-harmonic generation measurements. The dielectric constant data indicate a drop in the average bonding- antibonding splitting of GaAs following the laser pulse excitation. This behavior leads to a collapse of the band-gap on a picosecond time scale for excitation at fluences near the damage threshold of 1.0 kJ/m 2 and even faster at higher excitation fluences. The changes in the electronic band structure result from a combination of electronic screening by the excited free carriers and structural deformation of the lattice caused by the destabilization of the covalent bonds. The behavior of the second- order susceptibility shows that the material loses long-range order before the average bonding-antibonding splitting, which is more sensitive to short- range structure, changes significantly. Loss of long-range order and a drop of more than 2 eV in the average bonding-antibonding splitting are seen even at fluences below the damage threshold, a regime in which the laser- induced changes are reversible.
Last updated on 07/24/2019