化学物理

To follow up on the unexpectedly-good performance of several coupled-cluster models with approximate inclusion of 3-body clusters [J. Chem. Phys. 151, 064102 (2019)] we performed a more complete assessment of the 3CC method [J. Chem. Phys.…

The effect of substituting a hydrogen atom by a chlorine atom or a methyl group by a trichloromethyl (CCl3) group at the stereogenic center of light-driven second generation molecular motors is calculated in order to assess the effect on…

The role of graphene nanowindows in the nanohydroxyapatite bone scaffold preparation is important for the preparation of mechanically robust scaffolds and implementation in bone recovery. Here, we report a graphene-nanohydroxyapatite…

Understanding molecular structure, dynamics, and reactivity requires bridging processes that occur across widely separated time scales. Conventional molecular dynamics simulations provide atomistic resolution, but their femtosecond time…

Conventional theoretical and computational approaches to fully coupled quantum molecular dynamics, i.e. when both the electrons and nuclei are treated as quantum-mechanical particles, are impractical for all but the smallest chemical…

The Exact Factorization (XF) of molecular wavefunctions can be viewed as an 'electronic wavepacket' framework for quantum dynamics. It is an appealing alternative to the conventional non-adiabatic dynamics, unfolding in the space of coupled…

We develop a numerical approach based on the sinc basis set for first-principles electronic structure calculations in one-dimensional systems. The method exploits the inherent accuracy and non-local character of the sinc functions to handle…

An optical centrifuge is a laser pulse which enables controlled rotational excitation of molecules. Centrifuged molecules rotating with well-defined angular frequencies are ideal candidates to probe many-body quantum systems at the…

The response of water to electric fields is critical to the performance and stability of electrochemical devices, and the selectivity of enzymatic, atmospheric, and organic reactions. A key process in this context is the water…

The relaxation time of several second generation molecular motors is analysed by calculating the minimum energy path between the metastable and stable states and evaluating the transition rate within harmonic transition state theory based…

We investigate trends in the data-error scaling laws of machine learning (ML) models trained on discrete combinatorial spaces that are prone-to-mutation, such as proteins or organic small molecules. We trained and evaluated kernel ridge…

We demonstrate accurate data-starved models of molecular properties for interpolation in chemical compound spaces with low-dimensional descriptors. Our starting point is based on three-dimensional, universal, physical descriptors derived…

Implementation of Effective Core Potentials (ECPs) into the molecular scattering suite UKRmol+ is presented together with a set of calculations for a range of targets relevant for plasma modeling. Continuum description in scattering and…

We extend the use of coupled cluster (CC) trial states in the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method beyond single and double excitations to include both triple and quadruple excitations. With this AFQMC/CC hierarchy,…

A general semiclassical theory for the calculation of reaction rate constants is developed. The theory can be understood as a formal framework that encompasses existing semiclassical methods: instanton theory and semiclassical transition…

We present a numerical method for grand canonical density functional theory (DFT) tailored to solid-state systems, employing Gaussian-type orbitals as the primary basis. Our approach directly minimizes the grand canonical free energy using…

Physicochemical characterization of materials is central to the field of science and engineering and is essential to design new/engineered materials with specific properties. Assays available for small-molecules, e.g., XRD, NMR, LC-MS,…

We present a perturbative triples correction to the relativistic quadratic unitary coupled cluster singles and doubles (qUCCSD) method, denoted as qUCCSD[T]. The method builds upon the Hermitian structure of the unitary ansatz and employs a…

We present a relativistic third-order algebraic diagrammatic construction (ADC(3)) approach for calculating double ionization potentials (DIPs). By employing the exact two-component atomic mean-field (X2CAMF) Hamiltonian in combination with…

Time delays in photoemission are on the order of attoseconds and have been experimentally determined in atoms, molecules and solids. Their magnitude and energy dependence are expected to yield fundamental insights into the properties of the…