Browsing by Author "Scully, Marlan O."

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    Quantum plasmonic control of trions in a picocavity with monolayer WS2
    (AAAS, 2019) He, Zhe; Han, Zehua; Yuan, Jiangtan; Sinyukov, Alexander M.; Eleuch, Hichem; Niu, Chao; Zhang, Zhenrong; Lou, Jun; Hu, Jonathan; Voronine, Dmitri V.; Scully, Marlan O.
    Monitoring and controlling the neutral and charged excitons (trions) in two-dimensional (2D) materials are essential for the development of high-performance devices. However, nanoscale control is challenging because of diffraction-limited spatial resolution of conventional far-field techniques. Here, we extend the classical tip-enhanced photoluminescence based on tip-substrate nanocavity to quantum regime and demonstrate controlled nano-optical imaging, namely, tip-enhanced quantum plasmonics. In addition to improving the spatial resolution, we use the scanning probe to control the optoelectronic response of monolayer WS2 by varying the neutral/charged exciton ratio via charge tunneling in Au-Ag picocavity. We observe trion “hot spots” generated by varying the picometer-scale probe-sample distance and show the effects of weak and strong coupling, which depend on the spatial location. Our experimental results are in agreement with simulations and open an unprecedented view of a new range of quantum plasmonic phenomena with 2D materials that will help to design new quantum optoelectronic devices.
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    Spatially-Resolved Photoluminescence of Monolayer MoS2 under Controlled Environment for Ambient Optoelectronic Applications
    (American Chemical Society, 2018) Birmingham, Blake; Yuan, Jiangtan; Filez, Matthias; Fu, Donglong; Hu, Jonathan; Lou, Jun; Scully, Marlan O.; Weckhuysen, Bert M.; Zhang, Zhenrong
    Monolayer (ML) MoS2 has become a very promising two-dimensional material for photorelated applications, potentially serving as the basis for an ultrathin photodetector, switching device, or transistors because of its strong interaction with light in ambient conditions. Establishing the impact of individual ambient gas components on the optical properties of MoS2 is a necessary step toward application development. By using in situ Raman microspectroscopy with an environment-controlled reaction cell, the photoluminescence (PL) intensity of chemical vapor deposition (CVD)-grown MoS2 MLs is monitored at different intralayer locations under ambient and controlled gas environments, such as N2, O2, and H2O. This new approach enables us to monitor the optical properties of MoS2 at different locations on the flakes and separate the role of photoreaction of various gases during laser irradiation. Upon mild photoirradiation in ambient conditions, the PL intensity in the interior of the ML MoS2 flakes remains unchanged, while the PL intensity at the edge region increases drastically. Photoirradiation in controlled gas environments reveals that O2 is necessary to increase the PL intensity at the MoS2 flake edges, attributed to the charge transfer of chemisorbed O2. N2 or H2O and N2 environments induce decreasing PL intensity upon repetitive laser irradiation. However, the H2O and O2 gas mixture, a combination designed to mimic ambient conditions, is necessary to maintain the PL intensity at the interior of the ML MoS2 flakes. Our study demonstrates that photoreactions with the gaseous environment on the MoS2 ML flakes should be taken into consideration even upon mild photoirradiation because they strongly impact the flakes’ optical properties.