Chemical Physics
A classical coulombic correlation functional in one-loop (1L) and local-density-approximation (LDA) is derived for electrolyte solutions, starting from a first-principles many-body partition function. The 1L-LDA functional captures…
Some rate of oxidation and reduction side-reactions will inevitably coexist in most rechargeable batteries, contributing to reversible and irreversible self-discharge. While parasitic reduction traps electrons, parasitic oxidation donates…
In this article, we present a method for computing accurate and scalable nuclear forces within the phaseless auxiliary-field quantum Monte Carlo (AFQMC) framework. Our approach leverages automatic differentiation of the energy functional to…
Transitions between distinct dynamical regimes are ubiquitous in nonequilibrium systems. As a prototypical example, deposition growth is often accompanied by irreversible morphological instabilities. Forecasting such transitions from…
Neural quantum states (NQS) provide a flexible and highly expressive parameterization of wave functions for strongly correlated problems in quantum chemistry. Despite rapid advances in network architectures, the evaluation of electronic…
Quantum-chemical calculations often make use of point-group theory to exploit molecular symmetry, resulting in a reduction of the computational cost and in insights into the electronic structure. This exploitation is often limited to…
We incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment…
Two-pulse correlation experiments performed using pulses of different intensities on Pd(111) with different CO coverages showed that the CO photodesorption probability depends on whether the strong or the weak pulse arrives first to the…
Higher lying excited states beyond S1 and T1 are widely recognized in many photophysical systems, including thermally activated delayed fluorescence (TADF). However, their explicit and quantitative impact on photophysical observables such…
Standard harmonic-to-anharmonic thermodynamic integration (TI) is known to develop a near singularity in the integrand for solids exhibiting diffusive degrees of freedom, such as rotating functional groups or migrating defects. This…
High-throughput quantum-chemical calculations underpin modern molecular modelling, materials discovery, and machine-learning workflows, yet even semi-empirical methods become restrictive when many molecules must be evaluated. Here we report…
Quantum-state-controlled reactivity is a long-standing goal in the field of physical chemistry. In this work, we explore the vibrational-state-dependent behavior of the ion-molecule reaction between O2+ in distinct vibrational states and…
We study the strong-field interaction of a helical bi-chromatic pump with an anisotropic and inhomogeneous molecular system in the form of planar distribution of radially aligned molecular ensemble. This setting gives rise to macroscopic…
We investigate a diabatization procedure that localizes charges (in real space) and localizes spins (in spin space) for open-shell systems that exhibit charge transfer in the presence of spin-orbit coupling. The procedure is applied to a…
We present a generalized extension of the recently developed electron/hole-transfer Dynamically-weighted State-Averaged Constrained CASSCF (eDSC/hDSC) method to model charge transfer in the presence of spin-orbit coupling (SOC) for systems…
A data-driven computational method is introduced to extract chemical reaction mechanisms from time series chemical concentration data. It is realized through the use of dynamic symbolic regression in which a sparse analytical form for a…
Binding energies (BEs) of adsorbates on interstellar dust grains critically control adsorption, desorption, diffusion, and surface reactivity, and therefore strongly influence astrochemical models of star- and planet-forming regions. While…
Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…
Coupled-cluster (CC) theory and Green's function many-body perturbation theory (MBPT) have long evolved as distinct yet complementary frameworks for describing electronic correlation. While CC methods employ exponential wavefunction…
We investigate ion pairing dynamics in electrolytes driven far from equilibrium using molecular simulations and nonequilibrium rate theory. Focusing on 0.5 M $\mathrm{LiPF_6}$ in water and acetonitrile under uniform electric fields, we…