Microscopic Theory of Exciton-Exciton Annihilation in Two-Dimensional Semiconductors

Abstract

Auger-like exciton-exciton annihilation (EEA) is considered the key fundamental limitation to quantum yield in devices based on excitons in two-dimensional (2d) materials. Since it is challenging to experimentally disentangle EEA from competing processes, guidance of a quantitative theory is highly desirable. The very nature of EEA requires a material-realistic description that is not available to date. We present a many-body theory of EEA based on first-principle band structures and Coulomb interaction matrix elements that goes beyond an effective bosonic picture. Applying our theory to monolayer MoS${}_2$ encapsulated in hexagonal BN, we obtain an EEA coefficient in the order of $10^{-3}$ cm${}^2$s${}^{-1}$ at room temperature, suggesting that carrier losses are often dominated by other processes, such as defect-assisted scattering. Our studies open a perspective to quantify the efficiency of intrinsic EEA processes in various 2d materials in the focus of modern materials research.

References in corpus (31)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures
• Moiré Excitons in Van der Waals Heterostructures
• Three-band tight-binding model for monolayers of group-VIB transition metal dichalcogenides
• Quasiparticle band structures and optical properties of strained monolayer MoS2 and WS2
• Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics
• Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
• Exciton-exciton annihilation in MoSe2 monolayers
• Binding energies of exciton complexes in transition metal dichalcogenides and effect of dielectric environment
• Nonlinear Photoluminescence in Atomically Thin Layered WSe2 Arising from Diffusion-Assisted Exciton-Exciton Annihilation
• Vibrational and optical properties of MoS${}_2$: from monolayer to bulk
• Excitons versus electron-hole plasma in monolayer transition metal dichalcogenide semiconductors
• Fundamental Limits of Exciton-Exciton Annihilation for Light Emission in Transition Metal Dichalcogenide Monolayers
• The dielectric impact of layer distances on exciton and trion binding energies in van der Waals heterostructures
• Testing several recent van der Waals density functionals for layered structures
• Exciton diffusion in monolayer semiconductors with suppressed disorder
• RESPACK: An ab initio tool for derivation of effective low-energy model of material
• Exciton propagation and halo formation in two-dimensional materials
• Fast Exciton Annihilation by Capture of Electrons or Holes by Defects via Auger Scattering in Monolayer Metal Dichalcogenides
• Suppressing Diffusion-Mediated Exciton Annihilation in 2D Semiconductors Using the Dielectric Environment
• Wannier Function Approach to Realistic Coulomb Interactions in Layered Materials and Heterostructures
• Electron-hole correlations govern Auger recombination in nanostructures
• Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy
• The Effective Bosonic Hamiltonian for Excitons Reconsidered
• Bright excitons with negative-mass electrons
• Hot exciton transport in WSe2 monolayers
• Auger recombination of dark excitons in $\mathrm{W}{\mathrm{S}}_2$ and $\mathrm{WS}{\mathrm{e}}_2$ monolayers
• Coulomb-Engineered Heterojunctions and Dynamical Screening in Transition Metal Dichalcogenide Monolayers
• Interplay of screening and superconductivity in low-dimensional materials
• Low-Temperature Annihilation Rate for Quasi-Localized Excitons in Monolayer MoS2