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We demonstrate the possibility in quantifying the Raman intensities for bothspecimen and substrate layers in a common stacked experimental configurationand, consequently, propose a general and rapid thickness identificationtechnique for atomic-scale layers on dielectric substrates. Unprecedentedlywide-range Raman data for atomically flat MoS2 flakes are collected to comparewith theoretical models. We reveal that all intensity features can beaccurately captured when including optical interference effect. Surprisingly,we find that even freely suspended chalcogenide few-layer flakes have astronger Raman response than that from the bulk phase. Importantly, despite theoscillating intensity of specimen spectrum versus thickness, the substrateweighted spectral intensity becomes monotonic. Combined with its sensitivity tospecimen thickness, we suggest this quantity can be used to rapidly determinethe accurate thickness for atomic layers.

Quantitative Raman Spectrum and Reliable Thickness Identification for Atomic Layers on Insulating Substrates