Intervalley scattering by acoustic phonons in two-dimensional MoS2 revealed by double-resonance Raman spectroscopy

Bruno R. Carvalho (), Yuanxi Wang, Sandro Mignuzzi, Debdulal Roy, Mauricio Terrones, Cristiano Fantini, Vincent H. Crespi, Leandro M. Malard () and Marcos A. Pimenta ()
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Bruno R. Carvalho: Universidade Federal de Minas Gerais
Yuanxi Wang: The Pennsylvania State University
Sandro Mignuzzi: National Physical Laboratory
Debdulal Roy: National Physical Laboratory
Mauricio Terrones: The Pennsylvania State University
Cristiano Fantini: Universidade Federal de Minas Gerais
Vincent H. Crespi: The Pennsylvania State University
Leandro M. Malard: Universidade Federal de Minas Gerais
Marcos A. Pimenta: Universidade Federal de Minas Gerais

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract Double-resonance Raman scattering is a sensitive probe to study the electron-phonon scattering pathways in crystals. For semiconducting two-dimensional transition-metal dichalcogenides, the double-resonance Raman process involves different valleys and phonons in the Brillouin zone, and it has not yet been fully understood. Here we present a multiple energy excitation Raman study in conjunction with density functional theory calculations that unveil the double-resonance Raman scattering process in monolayer and bulk MoS2. Results show that the frequency of some Raman features shifts when changing the excitation energy, and first-principle simulations confirm that such bands arise from distinct acoustic phonons, connecting different valley states. The double-resonance Raman process is affected by the indirect-to-direct bandgap transition, and a comparison of results in monolayer and bulk allows the assignment of each Raman feature near the M or K points of the Brillouin zone. Our work highlights the underlying physics of intervalley scattering of electrons by acoustic phonons, which is essential for valley depolarization in MoS2.

Date: 2017
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DOI: 10.1038/ncomms14670

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