Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2
arXiv:2405.07058 · doi:10.1063/5.0218973
Abstract
We present a mixed quantum-classical framework for the microscopic and non-Markovian modeling of exciton-phonon scattering in solid-state materials, and apply it to calculate the optical linewidths of monolayer MoS2. Within this framework, we combine reciprocal-space mixed quantum-classical dynamics with models for the quasiparticle band structure as well as the electron-hole and carrier-phonon interactions, parametrized against ab initio calculations, although noting that a direct interfacing with ab initio calculations is straightforward in principle. We introduce various parameters for truncating the Brillouin zone to select regions of interest. Variations of these parameters allow us to determine linewidths in the limit of asymptotic material sizes. Obtained asymptotic linewidths are found to agree favorably with experimental measurements across a range of temperatures. As such, our framework establishes itself as a promising route towards unraveling the non-Markovian and microscopic principles governing the nonadiabatic dynamics of solids.
9 pages, 3 figures
References in corpus (37)
- 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
- Valley polarization in MoS2 monolayers by optical pumping
- Observation of tightly bound trions in monolayer MoS2
- MoS_2 as an ideal material for valleytronics: valley-selective circular dichroism and valley Hall effect
- Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
- First-principles study of the phonon-limited mobility in n-type single-layer MoS2
- Probing Excitonic Dark States in Single-layer Tungsten Disulfide
- Three-band tight-binding model for monolayers of group-VIB transition metal dichalcogenides
- Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
- Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors
- Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides
- Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
- Intrinsic Electrical Transport Properties of Monolayer Silicene and MoS2 from First Principles
- Robust optical emission polarization in MoS2 monolayers through selective valley excitation
- Screening and Many-Body Effects in Two-Dimensional Crystals: Monolayer MoS
- Valley depolarization due to inter- and intra-valley electron-hole exchange interactions in monolayer MoS
- Exciton band structure of monolayer MoS2
- How dielectric screening in two-dimensional crystals affects the convergence of excited-state calculations: Monolayer MoS
- Excitons in van der Waals heterostructures: The important role of dielectric screening
- Absorption of Light by Excitons and Trions in Monolayers of Metal Dichalcogenide MoS: Experiments and Theory
- Phonon Sidebands in Transition Metal Dichalcogenides
- Spin-Orbit mediated spin relaxation in monolayer MoS2
- Exciton-phonon coupling in MoSe2 monolayers
- Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2
- Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition-metal dichalcogenides
- Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides
- Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2
- Exciton-phonon coupling strength in single-layer MoSe2 at room temperature
- Exciton lifetime and optical linewidth profile via exciton-phonon interactions: Theory and first-principles calculations for monolayer MoS
- Theory of absorption lineshape in monolayers of transition metal dichalcogenides
- Coherent charge carrier dynamics in the presence of thermal lattice vibrations
- Revealing Ultrafast Phonon Mediated Inter-Valley Scattering through Transient Absorption and High Harmonic Spectroscopies
- Microscopic theory of cavity-confined monolayer semiconductors: polariton-induced valley relaxation and the prospect of enhancing and controlling the valley pseudospin by chiral strong coupling
- A Reciprocal-Space Formulation of Mixed Quantum-Classical Dynamics
- Overcoming positivity violations for density matrices in surface hopping