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On the Catalytic Activity of Sn Monomers and Dimers at Graphene Edges and the Synchronized Edge Dependence of Diffusing Atoms in Sn Dimers
In this study, in situ transmission electron microscopy is performed to study the interaction between single (monomer) and paired (dimer) Sn atoms at graphene edges. The results reveal that a single Sn atom can catalyze both the growth and etching of graphene by the addition and removal of C atoms respectively. Additionally, the frequencies of the energetically favorable configurations of an Sn atom at a graphene edge, calculated using density functional theory calculations, are compared with experimental observations and are found to be in good agreement. The remarkable dynamic processes of binary atoms (dimers) are also investigated and is the first such study to the best of the knowledge. Dimer diffusion along the graphene edges depends on the graphene edge termination. Atom pairs (dimers) involving an armchair configuration tend to diffuse with a synchronized shuffling (step-wise shift) action, while dimer diffusion at zigzag edge terminations show a strong propensity to collapse the dimer with each atom diffusing in opposite directions (monomer formation). Moreover, the data reveals the role of C feedstock availability on the choice a single Sn atom makes in terms of graphene growth or etching. This study advances the understanding single atom catalytic activity at graphene edges. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
Modeling Photodetection at the Graphene/Ag2S Interface
Mixed-dimensional systems host interesting phenomena that involve electron and ion transport along or across the interface, with promising applications in optoelectronic and electrochemical devices. Herein, a heterosystem consisting of a graphene monolayer with a colloidal Ag2S nanocrystal film atop, in which both ions and electrons are involved in photoelectrical effects, is studied. An investigation of the transport at the interface in different configurations by using a phototransistor configuration with graphene as a charge-transport layer and semiconductor nanocrystals as a light-sensitive layer is performed. The key feature of charge transfer is investigated as a function of gate voltage, frequency, and incident light power. A simple analytical model of the photoresponse is developed, to gain information on the device operation, revealing that the nanocrystals transfer electrons to graphene in the dark, but the opposite process occurs upon illumination. A frequency-dependence analysis suggests a fractal interface between the two materials. This interface can be modified using solid-state electrochemical reactions, leading to the formation of metallic Ag particles, which affect the graphene properties by additional doping, while keeping the photoresponse. Overall, these results provide analytical tools and guidelines for the evaluation of coupled electron/ion transport in hybrid systems.