Ultrafast probes of photovoltage and two-dimensional electron gas in the topological insulator Bi2Te3 by angle-resolved photoemission and terahertz spectroscopy

Photoexcited carriers in three-dimensional topological insulators (3D TIs) decay rapidly through the electron-electron and electron-phonon scattering. While most studies focus on such fast dynamics, recent experiments find the slow photovoltage (PV) dynamics arising from the band-bending potentials, in which the optical transitions in two-dimensional electron gas (2DEG) are effective. Although early investigations speculated the existence of multiple band-bending structures from the TI surface to the TI bulk, how PV and 2DEG are correlated in the presence of such multiple band bendings has been less explored. Here, we employ the combination of time- and angle-resolved photoemission spectroscopy (tr-ARPES) and ultrafast time-resolved terahertz (tr-THz) spectroscopy to investigate the PV and 2DEG dynamics in the prototypical topological insulator Bi2Te3. Our tr-ARPES analysis identifies two spatially separated PV dynamics associated with two types of band bending: one is the well-known surface PV, and another PV is formed deep within the bulk, which we call "internal bulk PV."For the surface PV, our tr-THz spectra substantiate that the μs-long transient signal arises from the surface-PV-induced increase of the TSS and 2DEG carrier density, which appears as a transient blueshift of a Fermi cutoff and an increased ARPES intensity in the tr-ARPES measurements. In contrast, the effect of the internal bulk PV shows only marginal changes in the 2DEG and TSS carrier densities but shifts the entire binding energy of the near-surface bands.