Chemical Physics
Accurate modeling of aqueous monovalent ions is essential for understanding the function of biomolecules, such as nucleic acid stability and binding of charged drugs to protein targets. The 1D and 3D reference interaction site models (1D-…
Machine learned interaction potentials (MLIPs) have become a critical component of large-scale, high-quality simulations for a range of chemical and biochemical systems. Yet, despite their in-distribution accuracy, molecular dynamics…
Nonlinear Four-wave mixing processes are a powerful technique to unravel ultrafast dynamics in solid-state systems. Here, we employ attosecond four-wave mixing spectroscopy with one extreme ultraviolet (XUV) pump and two independently…
Understanding ligand properties is essential for computational high-throughput screening of transition metal complexes. However, ligand properties such as net charge and other information such as their application area are often absent or…
Deep-lying core electrons carry highly localized, site-specific information that forms the basis of X-ray photoelectron spectroscopy. Accurately predicting their associated core ionization potentials (IPs) is a demanding theoretical task,…
Dissociative ionization processes of simple heterocyclic molecules like pyridine are relevant for an understanding of radiation damage processes in biological material that occur naturally in complex condensed environments. Pyridine can…
Calculations of the lowest valence {\pi}* as well as the 3s and higher energy 3p{\sigma} Rydberg excited states of the CO2 molecule are carried out using density functionals with variational optimization of the orbitals, an approach…
Empirical force fields remain the primary tool for large-scale molecular simulation, yet their limited flexibility and transferability often hinder predictive modeling in chemically complex condensed-phase systems. Here we present ORION, a…
The $\Delta$-Self-Consistent-Field ($\Delta$SCF) method permits calculations of core electron binding energies in materials and molecules at a modest computational cost. However, it has been reported that whilst this method works well for…
In this work, we access the performance of RI-CC2 for ultrafast internal conversion using pyrazine as a benchmark system. We implement analytical gradients and nonadiabatic coupling vectors for RI-CC2 in the Q-Chem package and employ them…
Nonlinear spectroscopy is widely used to study the transient dynamics of molecules under strong light-matter coupling, though it remains unclear to what extent uncoupled intracavity molecules obscure signals from the strongly-coupled…
Enhanced sampling methods typically require predefined collective variables (CVs) that presuppose knowledge of reaction coordinates, restricting the discovery of unanticipated transition mechanisms or intermediates. Here, we show that a…
Spin-orbit, charge-transfer intersystem crossing (SOCT-ISC) allows for the efficient production of triplet excited states in donor-acceptor (DA) dyads without the involvement of heavy atoms, for use in a myriad of technologies. This process…
Density functional theory (DFT) and linear-response time-dependent density functional theory (LR-TDDFT) rely on an exchange-correlation (xc) approximation that provides not only energy but also its functional derivatives that enter the…
Accurate determination of transition states is central to an understanding of reaction kinetics. Double-endpoint methods where both initial and final states are specified, such as the climbing image nudged elastic band (CI-NEB), identify…
Diffusion quantum Monte Carlo (DMC) and coupled cluster theory [CCSD(T)] are widely-employed benchmark methods for noncovalent interactions (NCIs). However, recent studies have reported notable discrepancies across several hydrogen-bonded…
Density functional approximations (DFAs) suffer from delocalization error, which limits their accuracy in predicting electron affinities (EAs), ionization potentials (IPs), and quasiparticle energies. In this work, we present a theoretical…
Tensor hypercontraction provides an attractive four-center two-electron repulsion integral format that can lower the scaling of many electronic structure methods while only requiring O(N^2) memory. However, in its grid-based least-squares…
The discovery of new energetic materials remains a pressing challenge hindered by limited availability of high-quality data. To address this, we have developed generative molecular language models that have been pretrained on extensive…
In this work, we investigated the influence of base pairing and {\pi}-{\pi} stacking interactions on electron attachment induced shape resonances in the adenine-thymine (AT) base pair. Resonance positions and widths are computed using a…