Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides
arXiv:1810.06570 · doi:10.1038/s41467-019-11497-y
Abstract
We present a many-body formalism for the simulation of time-resolved nonlinear spectroscopy and apply it to study the coherent interaction between excitons and trions in doped transition-metal dichalcogenides. Although the formalism can be straightforwardly applied in a first-principles manner, for simplicity we use a parameterized band structure and a static model dielectric function, both of which can be obtained from a calculation using the approximation. Our simulation results shed light on the interplay between singlet and triplet trions in molybdenum- and tungsten-based compounds. Our two-dimensional electronic spectra are in excellent agreement with recent experiments and we accurately reproduce the beating of a cross-peak signal indicative of quantum coherence between excitons and trions. Although we confirm that the quantum beats in molybdenum-based monolayers unambigously reflect the exciton-trion coherence time, they are shown here to provide a lower-bound to the coherence time of tungsten analogues due to a destructive interference emerging from coexisting singlet and triplet trions.
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- Microscopic theory of exciton and trion polaritons in doped monolayers of transition metal dichalcogenides
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- Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
- Interlayer excitonic spectra of vertically stacked MoSe/WSe heterobilayers
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