Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors

Abstract

Enhanced Coulomb interactions in monolayer transition metal dichalcogenides cause tightly bound electron-hole pairs (excitons) which dominate their linear and nonlinear optical response. The latter includes bleaching, energy renormalizations, and higher-order Coulomb correlation effects like biexcitons and excitation-induced dephasing (EID). While the first three are extensively studied, no theoretical footing for EID in exciton dominated semiconductors is available so far. In this study, we present microscopic calculations based on excitonic Heisenberg equations of motion and identify the coupling of optically pumped excitons to exciton-exciton scattering continua as the leading mechanism responsible for an optical power dependent linewidth broadening (EID) and sideband formation. Performing time-, momentum-, and energy-resolved simulations, we quantitatively evaluate the EID for the most common monolayer transition metal dichalcogenides and find an excellent agreement with recent experiments.

References in corpus (65)

• Atomically thin MoS2: A new direct-gap semiconductor
• Two Dimensional Atomic Crystals
• Black phosphorus field-effect transistors
• Phosphorene: A New 2D Material with High Carrier Mobility
• Coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides
• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Tunable Band Gap and Anisotropic Optical Response in Few-layer Black Phosphorus
• Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
• k.p theory for two-dimensional transition metal dichalcogenide semiconductors
• Theory of Neutral and Charged Excitons in Monolayer Transition Metal Dichalcogenides
• Quasiparticle band structure and tight-binding model for single- and bilayer black phosphorus
• Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics
• Valley-selective optical Stark effect in monolayer WS2
• 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
• Intrinsic Transport Properties of Electrons and Holes in Monolayer Transition Metal Dichalcogenides
• Screening and Many-Body Effects in Two-Dimensional Crystals: Monolayer MoS${}_2$
• Bright excitons in monolayer transition metal dichalcogenides: from Dirac cones to Dirac saddle points
• Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment
• Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides
• Titanium trisulfide monolayer: A new direct-gap semiconductor with high and anisotropic carrier mobility
• Nonanalyticity, Valley Quantum Phases, and Light-like Exciton Dispersion in Monolayer TMDs: Theory and First-Principles Calculations
• 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${}_2$: Experiments and Theory
• The dielectric genome of van der Waals heterostructures
• Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe${}_2$
• Excitons versus electron-hole plasma in monolayer transition metal dichalcogenide semiconductors
• Intervalley biexcitons and many-body effects in monolayer MoS2
• Phonon Sidebands in Transition Metal Dichalcogenides
• Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
• Exciton-phonon coupling in MoSe2 monolayers
• Biexciton fine structure in monolayer transition metal dichalcogenides
• Large, valley-exclusive Bloch-Siegert shift in monolayer WS2
• Temperature Dependent Valley Relaxation Dynamics in Single Layer WS2 Measured Using Ultrafast Spectroscopy
• Spectroscopic observation of resonant electric dipole-dipole interactions between cold Rydberg atoms
• Diffusion quantum Monte Carlo study of excitonic complexes in two-dimensional transition-metal dichalcogenides
• Binding energies of trions and biexcitons in two-dimensional semiconductors from diffusion quantum Monte Carlo calculations
• Binding energies and spatial structures of small carrier complexes in monolayer transition metal dichalcogenides via diffusion Monte Carlo
• Broadband Femtosecond Transient Absorption Spectroscopy for CVD MoS2 monolayer
• Impact of strain on the excitonic linewidth in transition metal dichalcogenides
• Ultrafast dynamics in monolayer TMDCs: the interplay of dark excitons, phonons and intervalley Coulomb exchange
• Theory of exciton dynamics in time-resolved ARPES: intra- and intervalley scattering in two-dimensional semiconductors
• Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers
• Observation of intervalley biexcitonic optical Stark effect in monolayer WS2
• Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects
• Influence of exciton-exciton correlations on the polarization characteristics of the polariton amplification in semiconductor microcavities
• Observation of exciton-exciton interaction mediated valley depolarization in monolayer MoSe${}_2$
• Excitonic structure of the optical conductivity in MoS${}_2$ monolayers
• Dependence of the hBN Layer Thickness on the Band Structure and Exciton Properties of Encapsulated WSe2 Monolayers
• Excitons, trions, and biexcitons in transition metal dichalcogenides: magnetic field dependence
• Exciton dynamics and non-linearities in 2D-hybrid organic perovskites
• Trion and Biexciton in Monolayer Transition Metal Dichalcogenides
• Excitation-induced transition to indirect band gaps in atomically thin transition metal dichalcogenide semiconductors
• Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites
• Theory of absorption lineshape in monolayers of transition metal dichalcogenides
• Quenching of Intervalley Exchange Coupling in the Presence of Momentum-Dark States in TMDCs
• Coherent dynamics and mapping of excitons in single-layer MoSe${}_2$ and WSe${}_2$ at the homogeneous limit
• Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides
• Frequency-dependent substrate screening of excitons in atomically thin transition metal dichalcogenide semiconductors
• Excitonic complexes in anisotropic atomically thin two-dimensional materials: black phosphorus and TiS${}_3$
• Dynamical screening effects of substrate phonons on two-dimensional excitons
• Coherent Propagation of Polaritons in Semiconductor Heterostructures: Nonlinear Pulse Transmission in Theory and Experiment
• Combined tensor network/cluster expansion method using logic gates: Illustrated for (bi-)excitons by a single layer MoS${}_2$ model system
• Tensor network strategies for calculating biexcitons and trions in monolayer 2D materials beyond the ground state

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• Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
• Exciton optics, dynamics and transport in atomically thin semiconductors
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• Dipolar and magnetic properties of strongly absorbing hybrid interlayer excitons in pristine bilayer MoS${}_2$
• Time-domain observation of interlayer exciton formation and thermalization in a MoSe${}_2$/WSe${}_2$ heterostructure
• Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe${}_2$ bilayers
• Dark exciton-exciton annihilation in monolayer WSe${}_2$
• Temporal evolution of low-temperature phonon sidebands in WSe${}_2$ monolayers
• Microscopic origin of anomalous interlayer exciton transport in van der Waals heterostructures
• Extended spatial coherence of interlayer excitons in MoSe${}_2$/WSe${}_2$ heterobilayers
• Exciton-phonon interaction calls for a revision of the "exciton" concept
• Quantum theory of two-dimensional materials coupled to electromagnetic resonators
• Exciton-phonon-scattering: A competition between bosonic and fermionic nature of bound electron-hole pairs
• Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes
• Strong coupling regime and hybrid quasinormal modes of a single plasmonic resonator coupled to a TMDC monolayer
• Impact of dark excitons on Förster type resonant energy transfer between dye molecules and atomically thin semiconductors
• Local field effects in ultrafast light-matter interaction measured by pump-probe spectroscopy of monolayer MoSe${}_2$
• Pure Dephasing of Light-Matter Systems in the Ultrastrong and Deep-Strong Coupling Regimes
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
• Semiconductor Bloch equation analysis of optical Stark and Bloch-Siegert shifts in monolayers WSe${}_2$ and MoS${}_2$
• Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape
• Shaping Exciton Polarization Dynamics in 2D Semiconductors by Tailored Ultrafast Pulses
• Effect of intravalley and intervalley electron-hole exchange on the nonlinear optical response of monolayer MoSe${}_2$
• Influence of local fields on the dynamics of four-wave mixing signals from 2D semiconductor systems
• Doping-induced non-Markovian interference causes excitonic linewidth broadening in monolayer WSe${}_2$
• Stochastic exciton-scattering theory of optical lineshapes: Renormalized many-body contributions
• Exciton-exciton Interactions -- A Quantitative Comparison Between Complimentary Phenomenological Models
• Fermionic vs. bosonic thermalization in the phonon-driven exciton dynamics: An analytic dimensionality study
• Dissecting intervalley coupling mechanisms in monolayer transition metal dichalcogenides
• Signatures of valley drift in the diversified band dispersions of bright, gray, and dark excitons in MoS2 monolayers under uni-axial strains
• Valley-controlled many-body exciton interactions in monolayer WSe${}_2$ phototransistors
• Efficient quadrature-squeezing from biexcitonic parametric gain in atomically thin semiconductors