Ultrafast Optical Properties of Dense Electron Gas in Silicon Nanostructures

We investigate the ultrafast dynamics of carriers in a silicon nanostructure by performing spectrally resolved femtosecond spectroscopy measurements with a supercontinuum probe. The nanostructure consists of a 158-nm-thick crystalline Si layer on top of which a SiO₂ passivation layer leads to a very high quality of the Si surface. In addition, a dielectric function approach, including contributions from a Drude part and interband transitions, combined with the Transition Matrix Approximation is used to model the photogenerated carrier dynamics. The spectrotemporal reflectivity reveals two mechanisms. First, an electron-hole plasma is created by the pump pulse and lasts for a few picoseconds. Importantly, its spectral signature is either a positive or a negative change of reflectivity, depending on the probe wavelength. This is complementary to the already reported results obtained with degenerate frequency measurements. The second mechanism is a thermal diffusion of carriers which occurs during several hundreds of picoseconds. The overall dynamics at short and long delays in the whole visible spectrum is well explained with our model which shows that the main contribution to the reflectivity dynamics is due to the Drude dielectric function. The observation of this predominance of free carriers requires both a long lived high density of carriers as well as a little influence of surface scattering as provided by our thin crystalline Si layer with passivated Si/SiO₂ interface.