Femtosecond time-resolved five-wave mixing at silicon surfaces

The ultrafast dynamics of photoexcitations at silicon surfaces is investigated using a surface-sensitive purely optical technique. In the experiments, the diffracted second harmonic generated by sequences of ultrashort laser pulses is detected as a function of the time delay between the pulses. It is demonstrated that this five-wave-mixing technique can be used to measure the temporal evolution of the optical polarization and the photoexcited populations at the surface. The experimental results can be reproduced by numerical solutions of optical Bloch equations. The theoretical analysis allows one to investigate which dephasing times and relaxation processes are compatible with experiment. Furthermore, it is outlined how one can describe optical nonlinearities at surfaces using a microscopic theory within the framework of semiconductor Bloch equations.