Many-body simulation of two-dimensional electronic spectroscopy of excitons and trions in monolayer transition metal dichalcogenides

Abstract

Indications of coherently interacting excitons and trions in doped transition metal dichalcogenides have been measured as quantum beats in two-dimensional electronic spectroscopy, but the microscopic principles underlying the optical signals of exciton-trion coherence remain to be clarified. Here we present calculations of two-dimensional spectra of such monolayers based on a microscopic many-body formalism. We use a parameterized band structure and a static model dielectric function, although a full ab initio implementation of our formalism is possible in principle. Our simulated spectra are in excellent agreement with experiments, including the quantum beats, while revealing the interplay between excitons and trions in molybdenum- and tungsten-based transition metal dichalcogenides. Quantum beats are confirmed to unambiguously reflect the exciton-trion coherence time in molybdenum compounds, but are shown to provide a lower bound to the coherence time for tungsten analogues due to a destructive interference from coexisting singlet and triplet trions.