Strain-Induced Indirect-to-Direct Bandgap Transition, Photoluminescence Enhancement, and Linewidth Reduction in Bilayer MoTe2.

Abstract

Two-dimensional (2D) layered materials provide an ideal platform for engineering electronic and optical properties through strain control because of their extremely high mechanical elasticity and sensitive dependence of material properties on mechanical strain. In this paper, a combined experimental and theoretical effort is made to investigate the effects of mechanical strain on various spectral features of bilayer MoTe2 photoluminescence (PL). We found that bilayer MoTe2 can be converted from an indirect to a direct bandgap material through strain engineering, resulting in a photoluminescence enhancement by a factor of 2.24. Over 90% of the PL comes from photons emitted by the direct excitons at the maximum strain applied. Importantly, we show that strain effects lead to a reduction of the overall linewidth of PL by as much as 36.6%. We attribute the dramatic decrease of linewidth to a strain-induced complex interplay among various excitonic varieties such as direct bright excitons, trions, and indirect excitons. Our experimental results on direct and indirect exciton emission features are explained by theoretical exciton energies that are based on first-principles electronic band structure calculations. The consistent theory-experimental trend shows that the enhancement of PL and the reduction of linewidth are the consequences of the increasing direct exciton contribution with the increase of strain. Our results demonstrate that strain engineering can lead to a PL quality of the bilayer MoTe2 comparable to that of the monolayer counterpart. The additional benefit of a longer emission wavelength makes the bilayer MoTe2 more suitable for silicon-photonics integration due to the reduced silicon absorption.