Biexciton fine structure in monolayer transition metal dichalcogenides

Abstract

The optical properties of atomically thin transition metal dichalcogenide (TMDC) semiconductors are shaped by the emergence of correlated many-body complexes due to strong Coulomb interaction. Exceptional electron-hole exchange predestines TMDCs to study fundamental and applied properties of Coulomb complexes such as valley depolarization of excitons and fine-structure splitting of trions. Biexcitons in these materials are less understood and it has been established only recently that they are spectrally located between exciton and trion. Here we show that biexcitons in monolayer TMDCs exhibit a distinct fine structure on the order of meV due to electron-hole exchange. Ultrafast pump-probe experiments on monolayer WSe${}_2$ reveal decisive biexciton signatures and a fine structure in excellent agreement with a microscopic theory. We provide a pathway to access biexciton spectra with unprecedented accuracy, which is valuable beyond the class of TMDCs, and to understand even higher Coulomb complexes under the influence of electron-hole exchange.

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Cited by in corpus (42)

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• Coulomb-bound four- and five-particle valleytronic states in an atomically-thin semiconductor
• Emerging Photoluminescence from the Dark-Exciton Phonon Replica in Monolayer WSe2
• The ultrafast onset of exciton formation in 2D semiconductors
• Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon
• Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors
• Exciton g-factors in monolayer and bilayer WSe${}_2$ from experiment and theory
• The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe${}_2$
• Exciton optics, dynamics and transport in atomically thin semiconductors
• Opportunities in Electrically Tunable 2D Materials Beyond Graphene: Recent Progress and Future Outlook
• Heralded spectroscopy reveals exciton-exciton correlations in single colloidal quantum dots
• Dark exciton-exciton annihilation in monolayer WSe${}_2$
• Few-body systems in condensed matter physics
• Stacking-dependent exciton multiplicity in WSe${}_2$ bilayers
• Strongly-bound excitons and trions in anisotropic 2D semiconductors
• Band nesting and exciton spectrum in monolayer MoS${}_2$
• Three-particle states and brightening of intervalley excitons in a doped MoS${}_2$ monolayer
• Direct Measurement of Biexcitons in Monolayer WS2
• Trions in MoS${}_2$ are quantum superpositions of intra- and intervalley spin states
• Two Biexciton Types Coexisting in Coupled Quantum Dot Molecules
• Probing biexciton in monolayer WS${}_2$ through controlled many-body interaction
• Light-matter coupling and non-equilibrium dynamics of exchange-split trions in monolayer WS2
• Combined tensor network/cluster expansion method using logic gates: Illustrated for (bi-)excitons by a single layer MoS${}_2$ model system
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Computational methods for 2D materials modelling
• Tuning exciton complexes in twisted bilayer WSe2 at intermediate misorientation
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• Biexcitons in Highly Excited CdSe Nanoplatelets
• Biexciton-like quartet condensates in an electron-hole liquid
• Tensor network strategies for calculating biexcitons and trions in monolayer 2D materials beyond the ground state
• Effect of intravalley and intervalley electron-hole exchange on the nonlinear optical response of monolayer MoSe${}_2$
• Efficient calculation of trion energies in monolayer transition metal dichalcogenides
• Magneto-Optical Measurements of the Negatively Charged 2$s$ Exciton in WSe${}_2$
• Energy shifts and broadening of excitonic resonances in electrostatically-doped semiconductors
• Sustained biexciton emission in colloidal quantum wells assisted by dopant-host interaction
• Impact of an electron Wigner crystal on exciton propagation
• Variational and field-theoretical approach to exciton-exciton interactions and biexcitons in semiconductors
• Steady-state nonlinear optical response of excitons in monolayer MoSe${}_2$
• Valley-controlled many-body exciton interactions in monolayer WSe${}_2$ phototransistors
• Increased formation of trions and charged biexcitons by above-gap excitation in single-layer $WS{e}_2$