Atypical exciton-phonon interactions in WS2 and WSe2 monolayers revealed by resonance Raman spectroscopy
Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS and WSe using more than 25 laser lines. The Raman excitation profiles of both materials sh...
| Autores: | , , , , , , , , , , , , , |
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| Tipo de recurso: | artículo |
| Fecha de publicación: | 2016 |
| País: | España |
| Institución: | Universitat Autònoma de Barcelona |
| Repositorio: | Dipòsit Digital de Documents de la UAB |
| Idioma: | inglés |
| OAI Identifier: | oai:ddd.uab.cat:306919 |
| Acceso en línea: | https://ddd.uab.cat/record/306919 https://dx.doi.org/urn:doi:10.1021/acs.nanolett.5b05096 |
| Access Level: | acceso abierto |
| Palabra clave: | Two-dimensional materials Transition metal dichalcogenides Resonant Raman spectroscopy First-principles calculations Exciton-phonon interaction |
| Sumario: | Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS and WSe using more than 25 laser lines. The Raman excitation profiles of both materials show unexpected differences. All Raman features of WS monolayers are enhanced by the first-optical excitations (with an asymmetric response for the spin-orbit related X and X excitons), whereas Raman bands of WSe are not enhanced at X energies. Such an intriguing phenomenon is addressed by DFT calculations and by solving the Bethe-Salpeter equation. These two materials are very similar. They prefer the same crystal arrangement, and their electronic structure is akin, with comparable spin-orbit coupling. However, we reveal that WS and WSe exhibit quite different exciton-phonon interactions. In this sense, we demonstrate that the interaction between X and X excitons with phonons explains the different Raman responses of WS and WSe, and the absence of Raman enhancement for the WSe modes at X energies. These results reveal unusual exciton-phonon interactions and open new avenues for understanding the two-dimensional materials physics, where weak interactions play a key role coupling different degrees of freedom (spin, optic, and electronic). |
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