Neutral and Charged Inter-Valley Biexcitons in Monolayer MoSe${}_2$

Abstract

In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods alone. Here, we implement polarization-resolved two-dimensional coherent spectroscopy to unravel the complex optical response of monolayer MoSe${}_2$ and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ~20 meV and ~5 meV binding energies--similar to recent calculations using variational and Monte Carlo methods. A theoretical model taking into account the valley-dependent optical selection rules reveals the specific quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprised of neutral and charged excitons from different valleys, offer new opportunities for creating exotic exciton-polariton condensates and for developing ultrathin biexciton lasers and polarization-entangled photon sources.

References in corpus (9)

• Strong light-matter coupling in two-dimensional atomic crystals
• Exciton Binding Energy of Monolayer WS2
• Splitting between Bright and Dark excitons in Transition Metal Dichalcogenide Monolayers
• Trion induced negative photoconductivity in monolayer MoS2
• Many-Body Theory of Trion Absorption Features in Two-Dimensional Semiconductors
• Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2
• Trion and Biexciton in Monolayer Transition Metal Dichalcogenides
• Theory of intervalley Coulomb interactions in monolayer transition-metal dichalcogenides
• Radiatively limited dephasing and exciton dynamics in MoSe${}_2$ monolayers

Cited by in corpus (77)

• Magneto-Optics of Exciton Rydberg States in a Monolayer Semiconductor
• Charge-tuneable biexciton complexes in monolayer WSe${}_2$
• Enhanced Light-Matter Interaction in Two-Dimensional Transition Metal Dichalcogenides
• Nanophotonics with 2D Transition Metal Dichalcogenides
• Coulomb-bound four- and five-particle valleytronic states in an atomically-thin semiconductor
• Electroluminescence from multi-particle exciton complexes in transition metal dichalcogenide semiconductors
• Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder
• Biexciton fine structure in monolayer transition metal dichalcogenides
• Raman spectrum of Janus transition metal dichalcogenide monolayers WSSe and MoSSe
• Filtering the photoluminescence spectra of atomically thin semiconductors with graphene
• Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon
• Diffusion quantum Monte Carlo study of excitonic complexes in two-dimensional transition-metal dichalcogenides
• Nanomaterials for Quantum Information Science and Engineering
• Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS2
• Direct Observation of Gate Tunable Dark Trions in Monolayer WSe2
• Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors
• Exciton optics, dynamics and transport in atomically thin semiconductors
• Luminescent emission of excited Rydberg excitons from monolayer WSe2
• Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides
• Exciton-phonon coupling strength in single-layer MoSe2 at room temperature
• Exciton-polaron interactions in monolayer WS${}_2$
• Excitons, trions, and biexcitons in transition metal dichalcogenides: magnetic field dependence
• Cross-over from trion-hole to exciton-polaron in n-doped semiconductor quantum wells
• Trion Valley Coherence in Monolayer Semiconductors
• Exciton-exciton interaction beyond the hydrogenic picture in a MoSe${}_2$ monolayer in the strong light-matter coupling regime
• Antiferromagnet-semiconductor van der Waals heterostructures: interlayer interplay of exciton with magnetic ordering
• Magnetooptics of layered two-dimensional semiconductors and heterostructures: progress and prospects
• Trion and Biexciton in Monolayer Transition Metal Dichalcogenides
• Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots
• Encapsulation Narrows Excitonic Homogeneous Linewidth of Exfoliated MoSe${}_2$ Monolayer
• Polariton interactions in microcavities with atomically thin semiconductor layers
• Localized Excitons in NbSe${}_2$-MoSe${}_2$ Heterostructures
• Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe${}_2$ bilayers
• Few-body systems in condensed matter physics
• Broadband pump-probe study of biexcitons in chemically exfoliated layered WS${}_2$
• Tutorial: Exciton resonances for atomically-thin optics
• Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides
• Strongly-bound excitons and trions in anisotropic 2D semiconductors
• Three-particle states and brightening of intervalley excitons in a doped MoS${}_2$ monolayer
• Tuning the Optical Properties of an MoSe${}_2$ Monolayer Using Nanoscale Plasmonic Antennas
• Direct Measurement of Biexcitons in Monolayer WS2
• Controlling valley splitting and Polarization of dark- and bi-excitons in monolayer WS${}_2$ by a tilted magnetic field
• Local field effects in ultrafast light-matter interaction measured by pump-probe spectroscopy of monolayer MoSe${}_2$
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Interaction induced AC-Stark shift of exciton-polaron resonances
• Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopy
• Combined tensor network/cluster expansion method using logic gates: Illustrated for (bi-)excitons by a single layer MoS${}_2$ model system
• Tuning exciton complexes in twisted bilayer WSe2 at intermediate misorientation
• Effects of dynamical dielectric screening on the excitonic spectrum of monolayer semiconductors
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• Enhanced exciton-exciton collisions in an ultra-flat monolayer MoSe2 prepared through deterministic flattening
• Tensor network strategies for calculating biexcitons and trions in monolayer 2D materials beyond the ground state
• Multidimensional Spectroscopy of Time-Dependent Impurities in Ultracold Fermions
• Pump-triple sum-frequency-probe spectroscopy of transition metal dichalcogenides
• Charge-carrier complexes in monolayer semiconductors
• Polaronic polariton quasiparticles in a dark excitonic medium
• Effects of Floquet Engineering on the Coherent Exciton Dynamics in Monolayer WS${}_2$
• Effect of intravalley and intervalley electron-hole exchange on the nonlinear optical response of monolayer MoSe${}_2$
• Shaping Exciton Polarization Dynamics in 2D Semiconductors by Tailored Ultrafast Pulses
• Destructive photon echo formation in six-wave mixing signals of a MoSe${}_2$ monolayer
• Interplay between polarization and quantum correlations of confined polaritons
• Efficient calculation of trion energies in monolayer transition metal dichalcogenides
• Influence of local fields on the dynamics of four-wave mixing signals from 2D semiconductor systems
• Fundamentals of heterodyne wave mixing spectroscopy: a tutorial
• Pairing of electro-magnetic bosons under spin-orbit coupling
• Signatures of defect-localized charged excitons in the photoluminescence of monolayer molybdenum disulfide
• Electrostatic control of the trion fine structure in transition metal dichalcogenide monolayers
• Theory of interlayer exciton dynamics in 2D TMDCs Heterolayers under the influence of strain reconstruction and disorder
• Sustained biexciton emission in colloidal quantum wells assisted by dopant-host interaction
• AC-Stark Spectroscopy of Interactions between Moiré Excitons and Polarons
• Direct observation of ultrafast defect-bound and free exciton dynamics in defect-engineered WS${}_2$ monolayers
• Microscopic many-body theory of two-dimensional coherent spectroscopy of excitons and trions in atomically thin transition metal dichalcogenides
• Controllable fusion of electromagnetic bosons in two-dimensional semiconductors
• Room Temperature Continuous-wave Excited Biexciton Emission in CsPbBr3 Nanocrystals
• Steady-state nonlinear optical response of excitons in monolayer MoSe${}_2$
• Momentum-resolved two-dimensional spectroscopy as a probe of nonlinear quantum field dynamics
• Valley-Selective Response of Nanoantennas Coupled to 2D Transition Metal Dichalcogenides