Thickness-dependent electronic transport induced by in situ transformation of point defects in MBE-grown Bi2Te3 thin films

Abstract

Interactions among various film growth parameters, such as the substrate temperature (Tsub), film thickness (d), and composition, play a crucial role in controlling the type and density of the intrinsic point defects. In turn, the point defects modulate and control electronic transport properties of Bi2Te3 films. We have grown n-type Bi2Te3 films with different d by molecular beam epitaxy at different Tsub. The formation of point defects was analyzed by a combined use of angle-resolved photoelectron spectroscopy (ARPES) and electronic transport measurements. Two important findings were made: (i) the negatively charged vacancies, VTe··, initially the dominant intrinsic defects, transform gradually during the growth process into positively charged anti-site defects, BiTe′, driven by thermal annealing from a continuously heated substrate; and (ii) from the film's surface into the inner strata of the film, the density of VTe·· decreases while the density of BiTe′ increases, leading to a gradient of vacancies and anti-site defects along the film growth direction. As a result, the electron density in Bi2Te3 films decreases monotonically with increasing d. Moreover, elevating Tsub leads to a more significant in situ annealing effect and an eventual onset of intrinsic excitations that deteriorates electronic transport properties. The thinnest Bi2Te3 film (16 nm) grown at Tsub = 245 °C has the highest electron concentration of 2.03 × 1020 cm−3 and also the maximum room temperature power factor of 1.6 mW m−1 K−2 of all grown epitaxial films. The new insights regarding the defect formation and transformation pave the way for further optimization of electronic transport properties of n-type Bi2Te3-based films.