Revealing the Water Structure at Neutral and Charged Graphene/Water Interfaces through Quantum Simulations of Sum Frequency Generation Spectra.

The structure and dynamics of water at charged graphene interfaces fundamentally influence molecular responses to electric fields with implications for applications in energy storage, catalysis, and surface chemistry. Leveraging the realism of the MB-pol data-driven many-body potential and advanced path-integral quantum dynamics, we analyze the vibrational sum frequency generation (vSFG) spectrum of graphene/water interfaces under varying surface charges. Our quantum simulations reveal a distinctive dangling OH peak in the vSFG spectrum at neutral graphene, consistent with recent experimental findings yet markedly different from those of earlier studies.

Electroreduction-Driven Formation and Connectivity of Polyoxometalate Coordination Networks.

We present the synthesis of metal oxide coordination networks based on Preyssler-type polyoxoanions ([NaPWO] and [NaPMoWO]) bridged with metal-aquo complexes ([M(HO)], M = Co, Ni, Zn, Y), induced by electrochemical reduction. Networks bridged with first-row transition metals are isostructural with a previously reported Co-bridged structure, while the Y-bridged structure is new. All networks feature an uncommon binding motif of the metal cation to the oxygen atoms at cap positions, which we hypothesize is due to increased electron density at the cap upon reduction.

Dissecting the Molecular Structure of the Air/Ice Interface from Quantum Simulations of the Sum-Frequency Generation Spectrum.

Ice interfaces are pivotal in mediating key chemical and physical processes such as heterogeneous chemical reactions in the environment, ice nucleation, and cloud microphysics. At the ice surface, water molecules form a quasi-liquid layer (QLL) with properties distinct from those of the bulk. Despite numerous experimental and theoretical studies, a molecular-level understanding of the QLL has remained elusive.

Current Status of the MB-pol Data-Driven Many-Body Potential for Predictive Simulations of Water Across Different Phases.

Developing a molecular-level understanding of the properties of water is central to numerous scientific and technological applications. However, accurately modeling water through computer simulations has been a significant challenge due to the complex nature of the hydrogen-bonding network that water molecules form under different thermodynamic conditions. This complexity has led to over five decades of research and many modeling attempts.

Concentration-Dependent Layer-Stacking and the Influence on Phase-Conversion in Colloidally Synthesized WSe Nanocrystals.

We report a synthesis of WSe nanocrystals in which the number of layers is controlled by varying the precursor concentration. By altering the ratios and concentrations of W(CO) and PhSe in trioctylphosphine oxide, we show that high [Se] and large Se/W ratios lead to an increased number of layers per nanocrystal. As the number of layers per nanocrystal is increased, the nanocrystal ensembles show less phase-conversion from the metastable 2M phase to the thermodynamically favored 2H phase.