Journal of Physical Chemistry B, Vol.108, No.12, 3789-3793, 2004
Ultrafast time-evolution of the nonlinear susceptibility of hot carriers at the Ge(111)-GeO2 interface as probed by SHG
Time-resolved second harmonic generation (SHG) was used to study hot carrier dynamics at the Ge(111)-GeO2 interface on the ferntosecond time scale. A linear dependence of the change in SHG on the pump power was observed for the carrier density range of 3 x 10(18) to 2.2 x 10(19) cm(-1). The ratio of the hot carrier to valence band nonlinear susceptibilities was determined to be 924 40 in the Ge(I I I)-GeO2 system, an order of magnitude greater than for Si(111)-SiO2. The dynamic SHG response is attributed to a change in the nonlinear susceptibility of the excited carriers and the diffusion of excited carriers away from the interface. The time to reach SHG steady-state response (410 +/- 70 fs) appears independent of carrier density in the range explored. The time evolution of the hot carrier nonlinear susceptibilities for Ge(I I I)-GeO2 at the 211 azimuth was extracted and shown to follow a double exponential evolution with time constants of 170 50 fs and 3500 1450 fs, similar to the literature values for bulk scattering times of electrons out of the Gamma valley (similar to100 fs) and into the L valley (similar to3.7 ps).