Photogating in the Graphene-Dye-Graphene Sandwich Heterostructure

In this work, we developed an atomically thin (∼2.5 nm) heterostructure consisting of a monolayer rhodamine 6G (R6G) film as a photoactive layer that was sandwiched between graphene films functioning as channels (graphene-R6G-graphene, G-R-G). Through a comparison of results of both photocurrent measurements and chemically enhanced Raman scattering (CERS) experiments, we found that our G-R-G heterostructure exhibited ∼7 and ∼30 times better performance than R6G-attached single-graphene (R6G-graphene, R-G) and MoS₂ devices, respectively; here, the CERS enhancement factor was highly correlated with the relative photoinduced Dirac voltage change. Furthermore, the photocurrent of the G-R-G device was found to be ∼40 times better than that of the R-G photodetector. The top graphene was highly operative in the monolayer, of which the performance is significantly deteriorated by fluorescence and tailored charge transfer efficiency with the increment of R6G film thickness. Overall, the responsivity of the G-R-G photodetector was ∼40 times higher than that of the R-G photodetector because of the more efficient carrier transfer between the organic dye and graphene induced by weaker π-π interactions between the top and bottom graphene channels in the former device. This atomically thin (∼2.5 nm) and highly photosensitive photodetector can be employed for post-Si-photodiode (PD) image sensors, single-photon detection devices, and optical communications.