Impact of Hydrogen on Graphene-based Materials: Atomistic Modeling and Simulation of HRSTEM Images

International audienceThe hydrogen energy transition is highly probable, because hydrogen is the most abundant element in the universe and represents an ideal “green” source of energy. Meanwhile, the safe hydrogen production and storage remains a major challenge still in progress. Potential production and storage materials include graphene. In terms of electronic and optoelectronic applications, hydrogen can tune the bandgap of graphene [1]. Hydrogen also plays a major role during the Chemical Vapour Decomposition (CVD) growth of graphene [2]. Hence, hydrogenated graphene-based materials are potentially relevant for various technological applications.To understand and optimize the device efficiency and the interface engineering, it is advantageous to perform advanced nanocharacterizations, linked to numerical modelling and simulations. This task is particularly difficult, because hydrogen is labile and prone to rapid reorganization. This structural evolution may be monitored with transmission electron microscopy (TEM) techniques [3,4,5], but in spite of significant progresses, the direct detection of hydrogen with High Resolution Scanning Transmission Electron Microscopy (HRSTEM) or energy-loss spectroscopy still remains a serious challenge.We investigate here the interaction of hydrogen with graphene using the Brenner module of the SAMSON software platform https://www.samson-connect.net and we propose an original methodology to characterize its structural arrangement at the atomic scale by simulating HRSTEM images to interpret experimental results. In particular, we compare the effect of hydrogen on dark field (DF), bright field (BF), high-angle annular dark filed (HAADF) and annular bright field (ABF) images, to estimate the best technique suited to hydrogen detection.In addition, we present the effect of carbon vacancies and adatoms on the stability of hydrogen coverage, associated to the HRSTEM signatures of the most stable configurations. These results provide the necessary building blocks to analyze the structure and energetics of hydrogenated graphene-based materials at the atomic scale