Multi-scale calculation of light-induced structural changes in low-angle twisted bilayer WSe$_2$

Abstract

Exciton-phonon interactions in transition metal dichalcogenides (TMD) are strong and lead to phenomena such as coherent phonon generation. When stacked and twisted, their properties can be tuned by the twisting angle. In experiments with 1.1$^\circ$ twisted 2L WSe$_2$, a change of 0.1 Å in the interlayer distance was observed when light was shone on this material, and here we explain the microscopic mechanism behind this. Theoretical works to study such systems are limited because the Moiré unit cell is too large. To overcome this, we combined classical force field relaxations with our implementation of ab initio GW/Bethe-Salpeter excited state forces (ESF). From the relaxations we found that the low-angle twisting induced an in-plane strain field, the AB regions are large enough to be simulated as periodic AB stacked 2L WSe2, and the interlayer force constant becomes softer in relation to the perfect AB stacking. From the ab initio ESF we obtained that the in-plane strain increases the out of plane ESFs. Those two effects combined, the weakening of the interlayer force constant and strain dependence of the ESF, make light-induced changes in the interlayer distance of twisted 2L WSe2 stronger than in the perfectly stacked case, in agreement with experimental observations. Therefore, our results show that the exciton-phonon interactions can be tuned in twisted 2L TMDs and can be observed experimentally, which makes those materials excellent platforms to study light-induced changes in materials.