Enabling Photoemission Electron Microscopy in Liquids via Graphene-Capped Microchannel Arrays

Photoelectron emission microscopy (PEEM) is a powerful tool to spectroscopically image dynamic surface processes at the nanoscale, but it is traditionally limited to ultrahigh or moderate vacuum conditions. Here, we develop a novel graphene-capped multichannel array sample platform that extends the capabilities of photoelectron spectromicroscopy to routine liquid and atmospheric pressure studies with standard PEEM setups. Using this platform, we show that graphene has only a minor influence on the electronic structure of water in the first few layers and thus will allow for the examination of minimally perturbed aqueous-phase interfacial dynamics. Analogous to microarray screening technology in biomedical research, our platform is highly suitable for applications in tandem with large-scale data mining, pattern recognition, and combinatorial methods for spectro-temporal and spatiotemporal analyses at solid-liquid interfaces. Applying Bayesian linear unmixing algorithm to X-ray induced water radiolysis process, we were able to discriminate between different radiolysis scenarios and observe a metastable "wetting" intermediate water layer during the late stages of bubble formation.