Three-dimensional topological insulators are materials that behave as an insulator in the interior, but as a metal on the surface with Dirac surface states protected by the topological properties of the bulk wavefunctions. The newly discovered second surface state, located about 1.5 eV above the conduction band in Bi2Se3 allows direct photoexcitation of the surface electrons in n-doped samples with a Ti:sapphire femtosecond laser. We have observed efficient THz generation from the Bi2Se3basal plane upon femtosecond optical excitation. By performing polarization-resolved studies on the emitted THz spectrum, two emission mechanisms have been identified, namely, emission generated from the transient photocurrent under the influence of the surface depletion field and from nonlinear optical rectification. The two types of emission are governed by distinct selection rules. And while the former is characterized by a narrow-band spectrum, the latter, involving almost instantaneous optical transitions, has a broad bandwidth and is enhanced by the presence of resonant transitions. These two emission mechanisms are further separated by their distinct doping dependence upon exposure to ambient air. With surface selectivity, THz emission spectroscopy thus provides a valuable spectroscopic tool for studies of the optical conductivity and dynamics of the surface state in centrosymmetric Bi2Se3.
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