Layer-dependent Charge Transfer and inter-layer coupling in WSe2/Graphene Heterostructures

Abstract: Understanding interfacial interactions in two-dimensional (2D) heterostructures is essential for advancing optoelectronic and quantum technologies. We investigate metal-organic chemical vapor deposition (MOCVD)-grown WSe$_2$ films (one to five layers) on graphene/SiC, directly compared to exfoliated WSe$_2$ on SiO$_2$, using Raman and photoluminescence (PL) spectroscopy complemented by atomic force microscopy (AFM). Raman measurements reveal compressive strain and interfacial charge transfer in WSe$_2$/graphene heterostructures, evidenced by blue-shifted phonon modes and the emergence of higher-order interlayer breathing modes absent on SiO$_2$. Concomitant shifts and attenuation of graphene's G and 2D modes with increasing WSe$_2$ thickness indicate progressive p-type doping of graphene, while WSe$_2$ phonon shifts point to n-type doping of the semiconductor, consistent with interfacial electron transfer. PL shows strong quenching for monolayer WSe$_2$ on graphene due to ultrafast charge transfer and F"orster resonance energy transfer (FRET), with partial emission recovery in multilayers relative to SiO$_2$-supported flakes. Exciton behavior differs strongly between substrates: on SiO$_2$, A- and B-exciton energies vary markedly with thickness, whereas on graphene they remain nearly pinned. This stability reflects the combined effects of graphene's strong dielectric screening and charge-transfer-induced free-carrier screening, with strain playing a secondary role. These results establish graphene, unlike SiO$_2$, as an active interfacial partner that stabilizes excitonic states and enables engineering of the optical response of 2D heterostructures.