Surface vibrational modes of the topological insulator Bi2Se3 observed by Raman spectroscopy

Authors: H.-H. Kung, M. Salehi, I. Boulares, A.F. Kemper, N. Koirala, M. Brahlek, P. Lostak, C. Uher, R. Merlin, X. Wang, S.-W. Cheong, S. Oh, G. Blumberg


We present polarization resolved Raman scattering study of surface vibration modes in the topological insulator Bi2Se3 single crystal and thin films. Besides the 4 Raman active bulk phonons, we observed 4 additional modes with much weaker intensity and slightly lower energy than the bulk counterparts. By symmetry analysis and comparison with theoretical calculation, we assigned these additional modes to out-of-plane surface phonons, where the frequency is slightly modified from the bulk phonon due to out-of-plane lattice distortion near the crystal surface. In particular, two of the surface modes at 60 and 173 cm-1 are associated with Raman active A1g bulk phonon modes, the other two at 136 and 158 cm-1 are associated with infrared active bulk phonons with A2u symmetry. The latter become Raman allowed due to restriction of crystalline symmetry from D3d in the bulk to C3v at the surface of Bi2Se3. The 158 cm-1 surface phonon mode show a Fano line shape, suggesting interaction with an electronic continuum at the crystal surface. In addition, we observed two weak features at 67 and 126 cm-1 likely corresponding to in-plane surface vibrational modes.