Isotope Effect in Bilayer WSe2

Isotopes of an element have the same electron number but differ in neutron number and atomic mass. However, due to the thickness-dependent properties in MX2 (M = Mo, W; X = S, Se, Te) transition metal dichalcogenides (TMDs), the isotopic effect in atomically thin TMDs still remains unclear especially for phonon-assisted indirect excitonic transitions. Here, we report the first observation of the isotope effect on the electronic and vibrational properties of a TMD material, using naturally abundant NAWNASe2 and isotopically pure 186W80Se2 bilayer single crystals over a temperature range of 4.4–300 K. We demonstrate a higher optical band gap energy in 186W80Se2 than in NAWNASe2 (3.9 ± 0.7 meV from 4.41 to 300 K), which is surprising as isotopes are neutral impurities. Phonon energies decrease in the isotopically pure crystal due to the atomic mass dependence of harmonic oscillations, with correspondingly longer E2g and A21g phonon lifetimes than in the naturally abundant sample. The change in electronic ban...