Coherent LO phonons are excited at the surface of bulk GaAs with femtosecond laser pulses. They are observed for the first time through electro-optic modulations of the transient reflectivity. The corresponding signal oscillations are superimposed upon an additional longitudinal polarization feature which decays exponentially and whose rise time is sufficiently short to act as a driving force for the coherent phonons. The components of the coherent phonon states dephase relative to each other in the order of picoseconds depending on the density of optically excited electron-hole pairs.

Above-band-gap pulsed optical excitation of electron-hole pairs within the surface-space-charge region of semiconductors alters the surface-space-charge field via free-carrier transport. We report on the direct observation of this ultrafast transient screening and the associated charge-carrier transport by applying reflective electro-optic sampling (REOS) with subpicosecond time resolution to (100)-oriented GaAs surfaces. The REOS measurements performed under different initial surface field conditions and various optical excitation densities are compared to numerical simulations of hotcarrier transport, including the calculation of the optical response. The simulations, which are based on a simple drift-diffusion model for optically excited electron-hole pairs, are in quantitative agreement with the experiment. The strength and sign of the static built-in field can be determined and the carrier drift velocities can be derived on a subpicosecond time scale.

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