  Topological insulators possess completely different spin-orbit coupled bulk
and surface electronic spectra that are each predicted to exhibit exotic
responses to light. Here we report time-resolved fundamental and second
harmonic optical pump-probe measurements on the topological insulator Bi2Se3 to
independently measure its photo-induced charge and spin dynamics with bulk and
surface selectivity. Our results show that a transient net spin density can be
optically induced in both the bulk and surface, which may drive spin transport
in topological insulators. By utilizing a novel rotational anisotropy analysis
we are able to separately resolve the spin de-polarization, intraband cooling
and interband recombination processes following photo-excitation, which reveal
that spin and charge degrees of freedom relax on very different time scales
owing to strong spin-orbit coupling.
