Bound electron-hole pairs called excitons govern the electronic and optical response of many organic and inorganic semiconductors. Excitons with spatially displaced wave functions of electrons and holes (interlayer excitons) are important for Bose-Einstein condensation, superfluidity, dissipationless current flow, and the light-induced exciton spin Hall effect. Here we report on the discovery of interlayer excitons in a bulk van der Waals semiconductor. They form due to strong localization and spin-valley coupling of charge carriers. By combining high-field magneto-reflectance experiments and ab initio calculations for 2H-MoTe, we explain their salient features: the positive sign of the g-factor and the large diamagnetic shift. Our investigations solve the long-standing puzzle of positive g-factors in transition metal dichalcogenides, and pave the way for studying collective phenomena in these materials at elevated temperatures.Excitons, quasi-particles of bound electron-hole pairs, are at the core of the optoelectronic properties of layered transition metal dichalcogenides. Here, the authors unveil the presence of interlayer excitons in bulk van der Waals semiconductors, arising from strong localization and spin-valley coupling of charge carriers.
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http://dx.doi.org/10.1038/s41467-017-00691-5 | DOI Listing |
Nature
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.
Angew Chem Int Ed Engl
January 2025
Huaqiao University College of Materials Science and Engineering, No.668 Jimei Avenue, Xiamen, Fujian, 361021, Xiamen, CHINA.
The advancement of tin-based perovskite solar cells (TPSCs) has been severely hindered by the poor controllability of perovskite crystal growth and the energy level mismatch between the perovskite and fullerene-based electron transport layer (ETL). Here, we synthesized three cis-configured pyridyl-substituted fulleropyrrolidines (PPF), specifically 2-pyridyl (PPF2), 3-pyridyl (PPF3), and 4-pyridyl (PPF4), and utilized them as precursor additives to regulate the crystallization kinetics during film formation. The spatial distance between the two pyridine groups in PPF2, PPF3, and PPF4 increases sequentially, enabling PPF4 to interact with more perovskite colloidal particles.
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