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Stokes and anti-Stokes Raman scattering are performed on atomic layers of hexagonal molybdenum ditelluride (MoTe2), a prototypical transition metal dichalcogenide (TMDC) semiconductor. The data reveal all six types of zone center optical phonons, along with their corresponding Davydov splittings, which have been challenging to see in other TMDCs. We discover that the anti-Stokes Raman intensity of the low energy layer-breathing mode becomes more intense than the Stokes peak under certain experimental conditions, and find the effect to be tunable by excitation frequency and number of atomic layers. These observations are interpreted as a result of resonance effects arising from the C excitons in the vicinity of the Brillouin zone center in the photon-electron-phonon interaction process.
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UMass SOAR Fund, the University of Massachusetts Amherst, the National Science Foundation Center for Hierarchical Manufacturing (CMMI-1025020) and in part by the Armstrong Fund for Science. D.X. acknowledges support from Office of Emerging Frontiers in Research and Innovation (EFRI-1433496).
Goldstein, Thomas; Chen, Shao-Yu; Tong, Jiayue; Xiao, Di; Ramasubramaniam, Ashwin; and Yan, Jun, "Raman Scattering and Anomalous Stokes-anti-Stokes Ratio in MoTe2 Atomic Layers" (2016). Scientific Reports. 1245.