Abstract: Ensemble Density Functional Theory (EDFT) is a generalization of ground-state Density Functional Theory (GS DFT), which is based on an exact formal theory of finite collections of a system's ground and excited states. EDFT in various forms has been shown to improve the accuracy of calculated energy level differences in isolated model syst...
Water structure near electrode interfaces may play an important role in controlling CO2 electroreduction. Using plasmon-enhanced vibrational sum frequency generation spectroscopy, we demonstrate the emergence of an interfacial water subpopulation with large electric fields along their OH bonds, when Na2CO3 ions are present near the electrode under ...
Ever since they have been studied, gas discharges have been classified by their visual appearance as well as by their current and voltage levels. Glow and arc discharges are the most prominent and well-known modes of discharges involving electrodes. In a first approximation, they are distinguished by their current and voltage levels, and current–vo...
Modeling the behavior of a prototype cantilevered X-ray adaptive mirror (held from one end) demonstrates its potential for use on high-performance X-ray beamlines. Similar adaptive mirrors are used on X-ray beamlines to compensate optical aberrations, control wavefronts and tune mirror focal distances at will. Controlled by 1D arrays of piezocerami...
Nanowires have emerged as an important family of one-dimensional (1D) nanomaterials owing to their exceptional optical, electrical, and chemical properties. In particular, Cu nanowires (NWs) show promising applications in catalyzing the challenging electrochemical CO2 reduction reaction (CO2RR) to valuable chemical fuels. Despite early reports show...
The advent of machine learning potentials (MLPs) provides a unique opportunity to access simulation time scales and to directly compute physicochemical properties that are typically intractable using density functional theory (DFT). In this study, we use an active learning curriculum to train a generalizable MLP using the DeepMD-kit architecture. B...
Aggregation of protein-based therapeutics can occur during development, production, or storage and can lead to loss of efficacy and potential toxicity. Native mass spectrometry of a covalently linked pentameric monoclonal antibody complex with a mass of ∼800 kDa reveals several distinct conformations, smaller complexes, and abundant higher-order ag...
Geological CO2 sequestration (GCS) can help mitigate global warming and enhance methane recovery from coal beds. However, few studies have linked the effects of CO2 to surface chemistry changes controlling wetting behavior in deep coal beds. Contact angles (CAs) of CO2/N2-high volatile bituminous coal-water systems were measured under different tem...
This study presents the polarizable quantum mechanics/molecular mechanics (QM/MM) embedding of the state-averaged complete active space self-consistent field (SA-CASSCF) in the atomic multipole optimized energetics for biomolecular applications (AMOEBA) force field for the purpose of studying photoreactions in protein environments. We describe two ...
