Two-photon IR pumped UV-Vis transient absorption spectroscopy of Dirac fermions in the topological insulator Bi₂Se₃

It is often taken for granted that in pump-probe experiments on the topological insulator (TI) Bi₂Se₃using IR pumping with a commercial Ti:sapphire laser [∼800 nm (1.55 eV photon energy)], the electrons are excited in the one-photon absorption regime, even when pumped with absorbed fluences in the mJ cm^-2range. Here, using UV-Vis transient absorption (TA) spectroscopy, we show that even at low-power Infrared (IR) pumping with absorbed fluences in theμJ cm^-2range, the TA spectra of the TI Bi₂Se₃extend across a part of the UV and the entire visible region. This observation suggests unambiguously that the two-photon pumping regime accompanies the usual one-photon pumping regime even at low laser powers applied. We attribute the high efficiency of two-photon pumping to the giant nonlinearity of Dirac fermions in the Dirac surface states (SS). On the contrary, one-photon pumping is associated with the excitation of bound valence electrons in the bulk into the conduction band. Two mechanisms of absorption bleaching were also revealed since they manifest themselves in different spectral regions of probing and cause the appearance of three different relaxation dynamics. These two mechanisms were attributed to the filling of the phase-space in the Dirac SS and bulk states, followed by the corresponding Pauli blocking.