The Importance of Pure Dephasing in the Optical Response of Excitons in High-quality van der Waals Heterostructures
arXiv:2502.05885 · doi:10.1103/21gh-fxyh
Abstract
Excitons in monolayer transition metal dichalcogenides (TMDs) dominate their optical response due to exceptionally large binding energies arising from their two-dimensional nature. Several theoretical models have been proposed to describe this excitonic behavior, however, it remains unclear which model most accurately captures the underlying physical properties of the response. In this work, we experimentally measure the optical response of high-quality monolayer TMD heterostructures and compare the results with the different theoretical models to address this uncertainty. We find that in high-quality heterostructures, quantum mechanical interactions in the form of pure dephasing plays a dominant role, which has been challenging to isolate experimentally in previous studies. Furthermore, accounting for an additional decay rate to the commonly used radiative and non-radiative rates is found to be important for the accurate description of the excitonic response. These findings establish a robust framework for understanding and predicting the optical properties of TMD-based heterostructures, crucial for both fundamental research and optoelectronic applications.
References in corpus (35)
- Atomically thin MoS2: A new direct-gap semiconductor
- Coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides
- Control of valley polarization in monolayer MoS2 by optical helicity
- Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
- Excitons in atomically thin transition metal dichalcogenides
- Observation of giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
- Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
- Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors
- Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics
- Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides
- Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
- Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
- Robust optical emission polarization in MoS2 monolayers through selective valley excitation
- Cooperative resonances in light scattering from two-dimensional atomic arrays
- Atomically thin mirrors made of monolayer semiconductors
- Exciton Dynamics in Monolayer Transition Metal Dichalcogenides
- Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
- Realization of an atomically thin mirror using monolayer MoSe2
- Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures
- Accessing high optical quality of MoS2 monolayers grown by chemical vapor deposition
- Single-crystalline gold nanodisks on WS mono- and multilayers: Strong coupling at room temperature
- Inhibited nonradiative decay at all exciton densities in monolayer semiconductors
- Plasmon-exciton polaritons in 2D semiconductor/metal interfaces
- Near-unity light absorption in a monolayer WS2 van der Waals heterostructure cavity
- Guide to optical spectroscopy of layered semiconductors
- Well separated trion and neutral excitons on superacid treated MoS2 monolayers
- Highly Confined In-plane Exciton-Polaritons in Monolayer Semiconductors
- Perfect absorption by an atomically thin crystal
- Engineering Effects of Vacuum Fluctuations on Two-dimensional Semiconductors
- Tutorial: Exciton resonances for atomically-thin optics
- Coherent Control of Two-Dimensional Excitons
- In-plane Exciton Polaritons vs Plasmon Polaritons: Nonlocal corrections, confinement and loss
- Interaction-induced photon blockade using an atomically thin mirror embedded in a microcavity
- 2D Semiconductors Superlattices as Hyperbolic Materials
- Electrically Tunable Interband Collective Excitations in Biased Bilayer and Trilayer Graphene
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- The Transmission Line Model for 2D Materials and van der Waals Heterostructures
- Strongly Coupled Exciton--Hyperbolic-phonon-polariton Hybridized States in hBN-encapsulated Biased Bilayer Graphene