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The topologically nontrivial and chemically functional distorted octahedral(T') transition metal dichalcogenides (TMDCs) are a type of layered semimetalthat has attracted significant recent attention. However, the properties ofmonolayer (1L) T'-TMDC, a fundamental unit of the system, is still largelyunknown due to rapid sample degradation in air. Here we report thatwell-protected 1L CVD T'-MoTe2 exhibits sharp and robust intrinsic Raman bands,with intensities about one order of magnitude stronger than those from bulkT'-MoTe2. The high-quality samples enabled us to reveal the set of all nineeven-parity zone-center optical phonons, providing reliable fingerprints forthe previously elusive crystal. By performing light polarization and crystalorientation resolved scattering analysis, we can effectively distinguish theintrinsic modes from Te-metalloid-like modes A (~122 cm-1) and B (~141 cm-1)which are related to the sample degradation. Our studies offer a powerfulnon-destructive method for assessing sample quality and for monitoring sampledegradation in situ, representing a solid advance in understanding thefundamental properties of 1L-T'-TMDCs.

Intrinsic Phonon Bands in High-Quality Monolayer T' Molybdenum Ditelluride