Interlayer excitons (IXs) in two-dimensional (2D) heterostructures provide an exciting avenue for exploring optoelectronic and valleytronic phenomena. Presently, valleytronic research is limited to transition metal dichalcogenide (TMD) based 2D heterostructure samples, which require strict lattice (mis) match and interlayer twist angle requirements. Here, we explore a 2D heterostructure system with experimental observation of spin-valley layer coupling to realize helicity-resolved IXs, without the requirement of a specific geometric arrangement, i.e., twist angle or specific thermal annealing treatment of the samples in 2D Ruddlesden-Popper (2DRP) halide perovskite/2D TMD heterostructures. Using first-principle calculations, time-resolved and circularly polarized luminescence measurements, we demonstrate that Rashba spin-splitting in 2D perovskites and strongly coupled spin-valley physics in monolayer TMDs render spin-valley-dependent optical selection rules to the IXs. Consequently, a robust valley polarization of ∼14% with a long exciton lifetime of ∼22 ns is obtained in type-II band aligned 2DRP/TMD heterostructure at ∼1.54 eV measured at 80 K. Our work expands the scope for studying spin-valley physics in heterostructures of disparate classes of 2D semiconductors.
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http://dx.doi.org/10.1021/acsnano.2c12546 | DOI Listing |
Nano Lett
January 2025
Department of Chemistry, York University, Toronto, Ontario M3J1P3, Canada.
The generation of interlayer charge transfer excitons upon photoexcitation is strongly desirable for two-dimensional (2D) materials stacked through van der Waals interactions. In this work, we investigate photoinduced charge transfer in silicanes (SiH) with three typical stackings. A concept of the regional natural hole orbital and its conjugated particle orbital is developed to characterize excited states in solids.
View Article and Find Full Text PDFNature
January 2025
Department of Physics, Brown University, Providence, RI, USA.
Excitons, Coulomb-driven bound states of electrons and holes, are typically composed of integer charges. However, in bilayer systems influenced by charge fractionalization, a more interesting form of interlayer exciton can emerge, in which pairing occurs between constituents that carry fractional charges. Despite numerous theoretical predictions for these fractional excitons, their experimental observation has remained unexplored.
View Article and Find Full Text PDFNano Lett
January 2025
School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China.
In van der Waals (vdW) architectures of transition metal dichalcogenides (TMDCs), the coupling between interlayer exciton and quantum degrees of freedom opens unprecedented opportunities for excitonic physics. Taking the MoSe homobilayer as representative, we identify that the interlayer registry defines the nature and dynamics of the lowest-energy interlayer exciton. The large layer polarization () is proved, which ensures the formation of layer-resolved interlayer excitons.
View Article and Find Full Text PDFNano Lett
January 2025
Department of Materials Science and Engineering, Centre for Functional Photonics, and Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong S.A.R., 999077, China.
The emission efficiency of interlayer excitons (IEs) in twisted 2D heterostructures has long suffered from momentum mismatch, limiting their applications in ultracompact excitonic devices. Here, we report strong room-temperature emission of momentum-forbidden IE in 30°-twisted MoS/WS heterobilayers. Utilizing a plasmonic nanocavity, the Purcell effect boosts the IE emission intensity in the cavity by over 2 orders of magnitude.
View Article and Find Full Text PDFSci Adv
January 2025
Department of Physics, University of Arizona, Tucson, AZ 85721, USA.
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