Strong suppression of emission quenching in core quantum dots coupled to monolayer MoS2.

Non-radiative processes like energy and charge transfer in 0D-2D semiconductor quantum dot (QD)-transition metal dichalcogenides (TMDs) and other two-dimensional layered materials, like graphene and analogs, leading to strong quenching of the photoluminescence (PL) of the usually highly emissive QDs, have been widely studied. Here we report control of the emission efficiency of core QDs placed in close proximity to the monolayers of MoS2. The QDs are transferred in the form of a high-density compact monolayer with the dot-dot separation, δ as well as the MoS2-QD separation, d, being controlled through chemical methods. While at larger separations we observe some quenching due to non-radiative processes, at smaller separations we observe enhanced emission from QDs on MoS2 as compared to the reference despite the presence of significant non-radiative charge transfer. Interestingly, at small separations δ, we see evidence of strong dot-dot interactions and a significant red shift of QD PL which enhances spectral overlap with the B exciton of MoS2. However, we observe significant reduction of PL quenching of QDs relative to longer δ and d cases, despite increased probability of non-radiative resonant energy transfer to MoS2, due to the enhanced spectral overlap, as well as charge transfer. Significantly we observe that simultaneously the intensity of the B exciton of MoS2 increases significantly suggesting the possibility of coherent and resonant radiative energy exchange between the 0D excitons in QDs and the 2D B exciton in MoS2. Our study reveals interesting nanoscale light-matter interaction effects which can suppress quenching of QDs leading to potential applications of these nanoscale materials in light emitting and photonic devices.

Evolution of inter-layer coupling in artificially stacked bilayer MoS2.

In this paper, we show experimentally that for van der Waals heterostructures (vdWh) of atomically-thin materials, the hybridization of bands of adjacent layers is possible only for ultra-clean interfaces. This we achieve through a detailed experimental study of the effect of interfacial separation and adsorbate content on the photoluminescence emission and Raman spectra of ultra-thin vdWh. For vdWh with atomically-clean interfaces, we find the emergence of novel vibrational Raman-active modes whose optical signatures differ significantly from that of the constituent layers. Additionally, we find for such systems a significant modification of the photoluminescence emission spectra with the appearance of peaks whose strength and intensity directly correlate with the inter-layer coupling strength. Our ability to control the intensity of the photoluminescence emission led to the observation of detailed optical features like indirect-band peaks. Our study establishes that it is possible to engineer atomically-thin van der Waals heterostructures with desired optical properties by controlling the inter-layer spacing, and consequently the inter-layer coupling between the constituent layers.