Behavior ofχ(2)during a laser-induced phase transition in GaAs

We explicitly determine the second-order optical susceptibility of GaAs following intense femtosecond laser-pulse excitation from second-harmonic-generation measurements. To separate the dependence of the 4.4-eV second-harmonic signal on the second-order susceptibility from its dependence on the linear dielectric constant, we use experimentally determined values for the dielectric constant of GaAs at 2.2 and 4.4 eV. The results show that the excitation of electrons and the resulting changes in the lattice affect the behavior of the second-order susceptibility. At pump fluences of 0.6 kJ/${\mathrm{m}}^2$ and higher, the material loses long-range order on a time scale ranging from 100 femtoseconds to tens of picoseconds, depending on the pump fluence. A recovery of the second-order susceptibility to its initial value at pump fluences between 0.6 and 1.0 kJ/${\mathrm{m}}^2$ shows that the loss of long-range order is reversible in this fluence regime.