Tunable Phases of Moir\'e Excitons in van der Waals Heterostructures

TL;DR

This study combines first-principles calculations and excitonic models to explore how twist angles in MoSe2/WSe2 heterostructures influence moiré exciton phases and their optical properties, revealing phase transitions at specific angles.

Contribution

It provides a microscopic understanding of twist-angle dependent moiré exciton phases and their impact on optical spectra in van der Waals heterostructures.

Findings

Flat, moiré trapped exciton states at angles < 2°

Transition to delocalized excitons at 3°

Predictable linear and quadratic angle dependence of excitonic resonances

Abstract

Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moir\'e superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. While recent experimental studies have confirmed twist-angle dependent optical spectra, the microscopic origin of moir\'e exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions between different moir\'e exciton phases and their impact on optical properties of the twisted MoSe$_2$/WSe$_2$ heterostructure. At angles smaller than 2$^{\circ}$ we find flat, moir\'e trapped states for inter- and intralayer excitons. This moir\'e exciton phase drastically changes into completely delocalized states already at 3$^{\circ}$. We predict a linear and quadratic twist-angle dependence of excitonic resonances for the moir\'e-trapped and delocalized exciton phase, respectively. Our work provides microscopic insights opening the possibility to tailor moir\'e exciton phases in van der Waals superlattices.