Theoretical and experimental study of second harmonic generation from the surface of the topological insulator Bi2Se3

We develop a theoretical model that describes the second harmonic generation of light from the surface of the topological insulator Bi2Se3 and experimentally demonstrate that the technique is sensitive to the surface electrons. By performing a crystal symmetry analysis of Bi2Se3(111) we determine the nonlinear electric susceptibility tensor elements that give rise to second harmonic generation. Using these results, we present a phenomenological model that shows that the relative magnitudes of these tensor elements can be determined by measuring the polarization and intensity of the radiated second harmonic light as a function of the in-plane crystal orientation and incident laser polarization. We describe optical techniques capable of isolating second harmonic light and, using these techniques, we measure the first-order linear optical and second-order nonlinear optical responses as a function of crystal orientation and laser polarization on bulk single crystals of Bi2Se3(111). The experimental results are consistent with our theoretical description. By comparing the data to our theoretical model we determine that a portion of the measured second harmonic light originates from the accumulation region of Bi2Se3(111), which we confirm by performing surface doping-dependent studies. Our results show that second harmonic generation is a promising tool for spectroscopic studies of topological surfaces and buried interfaces.