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Probing phonons, quasi-particle excitations and their coupling has enrichedour understanding of these 2D materials and proved to be crucial for developingtheir potential applications. Here, we report comprehensive temperature, 4-330K, and polarization-dependent Raman measurements on mono and bilayer MoSe2.Phonon's modes up to fourth-order are observed including forbidden Raman and IRmodes, understood considering Frohlich mechanism of exciton-phonon coupling.Most notably, anomalous variations in the phonon linewidths with temperaturepointed at the significant role of electron-phonon coupling in these systems,especially for the out-of-plane (A1g) and shear mode (E22g), which is found tobe more prominent in the narrow-gaped bilayer than the large gapped monolayer.Via polarization-dependent measurements, we deciphered the ambiguity insymmetry assignments, especially to the peaks around ~ 170 cm-1 and ~ 350 cm-1.Temperature-dependent thermal expansion coefficient, an important parameter forthe device performance, is carefully extracted for both mono and bilayer bymonitoring the temperature-dependence of the real-part of the phononself-energy parameter. Our temperature-dependent in-depth Raman studies providea pave for uncovering the deeper role of phonons in these 2D layered materialsfrom a fundamental as well as application point of view.

Electron-Phonon Coupling, Thermal Expansion Coefficient, Resonance Effect and Phonon Dynamics in High Quality CVD Grown Mono and Bilayer MoSe2