The ultrafast carrier dynamics of semiconductor surfaces on a sub-picosecond time scale has become a significant area for study from the viewpoints of basic science and technological innovations 1,2 because of the explosive development of the large-scale integration of semiconductor circuits. Among surface materials, Si is one of the most important for electronic devices, and many studies on its surface ultrafast carrier dynamics have been performed using such methods as the two-photon photoemission method 3,4 and the transient-reflectivity (TR) method. 5,6 The time-resolved two-photon photo-emission method has provided useful information about the carrier thermalization process via carrier-carrier scattering, and the TR method has elucidated the multi-body effect of photo-excited carriers. However, ultrafast carrier dynamics has not yet been clarified. For instance, the time evolutions of a distribution of photoexcited carriers and of the Coulomb interaction should be taken into account under a strong excitation condition on a femtosecond time scale; the validity of the random-phase approximation has already been investigated under such a condition. 7 Experimental difficulties are derived from the fact that most of the ultrafast phenomena are non-radiative processes, and thus band-to-band relaxation cannot be directly observed. For such a case, photothermal spectroscopy, which measures any heat or refractive-index change due to photo-excitation, would be a powerful tool. As a photothermal method, we have developed a transient reflecting grating (TRG) method with a time resolution of 80 ps, and have applied it to semiconductor surfaces. 8,9 The TRG method has many advantages, such as surface selectivity, high sensitivity, background-free detection, and providing directional information. We can expect to observe carrier thermalization and carrier transport dynamics by raising the time resolution to the femtosecond time region of the TRG method.In this study, we developed a femtosecond time-resolved TRG (fs-TRG) method and applied it to measure Si(111) surfaces.We want to use it to clarify the behavior of photo-excited carriers at these surfaces. We present results suggesting the ballistic transport of non-equilibrium carriers, and the Auger recombination and carrier diffusion of equilibrium carriers.
ExperimentalSince the experimental setup for the TRG method was the same as that described in our previous report, 10 only an outline is presented here based on Fig. 1. Two pump pulses of the same wavelength, λpump, were crossed on a sample surface to form an optical interference pattern with a fringe spacing (Λ) of Λ = λpump/2sinθ, where θ is the pump beam incident angle normal to the surface. This interference pattern induced a periodic refractive-index change, which acted as a transient diffraction grating. The probe pulse was incident normal to the grating, and diffracted light was observed. The intensity of the diffracted light was monitored as a function of the delay time of the probe beam. The TRG signal refle...