Robust Interlayer Exciton Interplay in Twisted van der Waals Heterotrilayer on a Broadband Bragg Reflector up to Room Temperature

Abstract

We report robust room temperature interlayer excitons in transition metal dichalcogenide heterostructures engineered via precise stacking orientation and twist-angle control. We integrate 2H-stacked MoSe${}_2$/${}^1$WSe${}_2$/${}^2$WSe${}_2$ heterotrilayer onto a chirped distributed Bragg reflector that acts as a backside mirror. This way, we fabricate a platform that hosts distinct heterotrilayer, heterobilayer, and homobilayer regions with enhanced excitonic features at elevated temperatures. Although the heterobilayer supports temperature-tunable singlet and triplet interlayer excitons, it exhibits low emission yield at 4 K. In comparison, the heterotrilayer shows remarkable excitonic properties, including pronounced band modulation, intervalley interlayer exciton transitions, and a tenfold photoluminescence enhancement along with a sevenfold increase in exciton decay time at cryogenic temperatures compared to the heterobilayer system. Temperature-dependent studies reveal intriguing interlayer exciton dynamics in the heterotrilayer, including the emergence of valley-polarized interlayer excitons, and the ability to maintain optical stability up to room temperature. Our results establish a clear strategy for engineering excitonic states across multilayer van der Waals heterostructures from 4 K to room temperature, providing a versatile platform for excitonic optoelectronics, quantum photonics, and tunable long-lived interlayer exciton states in scalable TMD heterostructures.

References in corpus (37)

• Electric Field Effect in Atomically Thin Carbon Films
• Atomically thin MoS2: A new direct-gap semiconductor
• Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures
• Moiré Excitons in Van der Waals Heterostructures
• Signatures of moiré-trapped valley excitons in MoSe${}_2$/WSe${}_2$ heterobilayers
• Three-band tight-binding model for monolayers of group-VIB transition metal dichalcogenides
• Resonantly hybridised excitons in moiré superlattices in van der Waals heterostructures
• Observation of Intense Second Harmonic Generation from MoS${}_2$ Atomic Crystals
• The hot pick-up technique for batch assembly of van der Waals heterostructures
• Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides
• Electrical control of interlayer exciton dynamics in atomically thin heterostructures
• Long-lived direct and indirect interlayer excitons in van der Waals heterostructures
• Fast pick up technique for high quality heterostructures of bilayer graphene and hexagonal boron nitride
• Electronic and Thermoelectric Properties of Few-Layer Transition Metal Dichalcogenides
• Interlayer Exciton Optoelectronics in a 2D Heterostructure p-n Junction
• Double Indirect Interlayer Exciton in a MoSe2/WSe2 van der Waals Heterostructure
• Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure
• Twist Angle Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures
• Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers
• Giant Zeeman splitting inducing near-unity valley polarization in van der Waals heterostructures
• Tunable Phases of Moiré Excitons in van der Waals Heterostructures
• The role of momentum-dark excitons in the elementary optical response of bilayer WSe${}_2$
• Giant Valley-Zeeman Splitting from Spin-Singlet and Spin-Triplet Interlayer Excitons in WSe2/MoSe2 Heterostructure
• Highly Valley-Polarized Singlet and Triplet Interlayer Excitons in van der Waals Heterostructure
• Moiré excitons in MoSe${}_2$-WSe${}_2$ heterobilayers and heterotrilayers
• Cavity-control of bright and dark interlayer excitons in van der Waals heterostructures
• Exciton g-factors in monolayer and bilayer WSe${}_2$ from experiment and theory
• Exciton dynamics in WSe2 bilayers
• Quadrupolar Excitons and Hybridized Interlayer Mott Insulator in a Trilayer Moiré Superlattice
• Quantum phase transitions of tri-layer excitons in atomically thin heterostructures
• Localization and interaction of interlayer excitons in MoSe${}_2$/WSe${}_2$ heterobilayers
• Evidence for Exciton Crystals in a 2D Semiconductor Heterotrilayer
• Stacking-dependent exciton multiplicity in WSe${}_2$ bilayers
• Spatially indirect intervalley excitons in bilayer WSe2
• A room-temperature moiré interlayer exciton laser
• Interlayer Exciton Valleytronics in Bilayer Heterostructures Interfaced with a Metasurface
• Temperature-dependent Optical and Polaritonic Properties of hBN-encapsulated Monolayer TMDs