The growth of three-dimensional ultra-fine spherical nano-particles of silver on few layers of graphene derived from highly oriented pyrolytic graphite in ultra-high vacuum were characterized using in situ scanning tunneling microscopy (STM) in conjunction with X-ray photoelectron spectroscopy. The energetics of the Ag clusters was determined by DFT simulations. The Ag clusters appeared spherical with size distribution averaging approximately 2 nm in diameter. STM revealed the preferred site for the position of the Ag atom in the C-benzene ring of graphene. Of the three sites, the C-C bridge, the C-hexagon hollow, and the direct top of the C atom, Ag prefers to stay on top of the C atom, contrary to expectation of the hexagon-close packing. Ab initio calculations confirm the lowest potential energy between Ag and the graphene structure to be at the exact site determined from STM imaging.
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http://dx.doi.org/10.1186/1556-276X-7-173 | DOI Listing |
Nat Commun
January 2025
Institute for Materials Science, University of Stuttgart, D-70569, Stuttgart, Germany.
The knowledge of diffusion mechanisms in materials is crucial for predicting their high-temperature performance and stability, yet accurately capturing the underlying physics like thermal effects remains challenging. In particular, the origin of the experimentally observed non-Arrhenius diffusion behavior has remained elusive, largely due to the lack of effective computational tools. Here we propose an efficient ab initio framework to compute the Gibbs energy of the transition state in vacancy-mediated diffusion including the relevant thermal excitations at the density-functional-theory level.
View Article and Find Full Text PDFSci Data
January 2025
IBM Research, Hursley, SO21 2JN, UK.
A significant challenge in computational chemistry is developing approximations that accelerate ab initio methods while preserving accuracy. Machine learning interatomic potentials (MLIPs) have emerged as a promising solution for constructing atomistic potentials that can be transferred across different molecular and crystalline systems. Most MLIPs are trained only on energies and forces in vacuum, while an improved description of the potential energy surface could be achieved by including the curvature of the potential energy surface.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
Cornell University, Ithaca, New York 14853, USA.
J Phys Chem A
January 2025
Institute of Modern Physics, Shaanxi Key Laboratory for Theoretical Physics Frontiers, Northwest University, Xi'an, Shaanxi 710127, China.
The full-dimensional potential energy surface (PES) for the photodissociation of HNCS in the S(″) electronic state has been built up by the neural network method based on more than 48,000 points, which were calculated at the multireference configuration interaction level with Davidson correction using the augmented correlation consistent polarized valence triple-ζ basis set. It was found that two minima, namely, and isomers of HNCS, and seven stationary points exist on the S PES for the three dissociation pathways: HNCS(S) → H + NCS/HNC + S(D)/HN(Δ) + CS(Σ). The dissociation energies of two lowest product channels H + NCS and HNC + S(D) calculated on the PES are in good agreement with experimental results, validating the high accuracy of the PES.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
Biophysics Graduate Program, The Ohio State University, Columbus, Ohio 43210, United States.
Fragment-based quantum chemistry methods offer a means to sidestep the steep nonlinear scaling of electronic structure calculations so that large molecular systems can be investigated using high-level methods. Here, we use fragmentation to compute protein-ligand interaction energies in systems with several thousand atoms, using a new software platform for managing fragment-based calculations that implements a screened many-body expansion. Convergence tests using a minimal-basis semiempirical method (HF-3c) indicate that two-body calculations, with single-residue fragments and simple hydrogen caps, are sufficient to reproduce interaction energies obtained using conventional supramolecular electronic structure calculations, to within 1 kcal/mol at about 1% of the computational cost.
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