Chemical Physics
Mapping methods are often used for the numerical simulation of nonadiabatic systems by propagating classical mapping variable trajectories. A recently popularised mapping method is spin-mapping, whose mapping variables arise from quantum…
Static and frequency-dependent polarizabilities were computed for 41 molecules using RPA, RPA(D), HRPA, HRPA(D), SOPPA, SOPPA(CC2), and SOPPA(CCSD) with the aug-cc-pVTZ basis set and benchmarked against CCSD reference values and available…
Whether topology directly shapes chemical dynamics remains an open question in theoretical chemistry. The issue arises because degeneracies of adiabatic electronic states can generate nontrivial topological structure, and such degeneracies…
Quantum mechanical (QM) cluster models provide an effective framework for mechanistic studies of enzymatic reactions but remain computationally demanding. Neural network potentials (NNPs) offer a promising route to reduce this cost, but…
High-order coupled-cluster theories with iterative triples (CCSDT), perturbative quadruples [CCSDT(Q)], and iterative quadruples (CCSDTQ) provide benchmark-quality correlation energies, but their steep computational scalings, $O(N^8),…
Electric double-layer capacitors (EDLCs) rely on the dynamical response of confined electrolytes to store and release charge, yet the interplay between ion transport, electrostatic interactions, and electrode metallicity remains poorly…
Attosecond technologies provide unique opportunities to study electron dynamics and electron correlation on their intrinsic timescales. From a theoretical perspective, this places strong constraints as an accurate treatment of electron…
Recent discoveries of electron-induced coherence in both resonant and non-resonant interactions have introduced new perspectives in the field. In non-resonant processes, coherence has been observed in dipolar dissociation, where…
Molecular simulations of complex chemical systems, such as catalysis, electrochemistry, and energy storage, often need to capture the interplay of effects such as electronic structure, finite-temperature fluctuations, and electric-field…
Finding exact solutions to the quantum many-body problem is computationally intractable (QMA-hard). Traditional approximations for electrons in an atom or molecule -- density functional theory and wavefunction methods -- have been…
Intramolecular electron transport in biological systems is typically described as a diffusive hopping process, according to the semi-classical rate theories of Marcus and Hopfield combined with classical Pauli-type master equations.…
Multireference behavior in molecules often arises when a small gap between frontier orbitals results in mixing of closed and open-shell configurations. Standard multireference diagnostics of this regime usually rely on correlated…
The Obara-Saika (OS) method is one of the most widely used techniques in quantum chemistry for evaluating electron repulsion integrals (ERIs) via a set of recurrence relations that build higher angular momentum integrals from lower-order…
Experiments have shown that, by tuning a microcavity to resonance with a vibrational mode of the molecules contained within it, one can modify chemical properties, such as reaction rates. This gives rise to the exciting prospect of steering…
Molecular spintronics seeks to control spin states in single molecules for ultrafast switching and efficient information processing. Transition metal complexes are promising candidates for such applications due to their modular ligand…
The highly variable physico-chemical properties of thin molecular films play an essential role in numerous research fields ranging from biophysics to the fabrication of functional devices such as molecular sensors. The properties of…
Machine learning interatomic potentials are trained to predict energies and forces but built to be sampled: their purpose is to drive molecular simulations whose observables average over the equilibrium distribution the potential defines.…
We introduce an additive reference correction for the transcorrelated (TC) method and its three-body mean-field approximation (xTC), to improve energy differences computed in small orbital basis sets. The correction is motivated by the…
Atmospheric entry processes are characterized by high-enthalpy gas flows in strong thermo-chemical non-equilibrium. Accurate simulations of such conditions remain challenging due to the extreme conditions and the complex influence of…
Non-collinear density functional theories were developed to extend the use of established collinear exchange-correlation functionals to systems with unpaired electrons in the presence of significant spin-orbit coupling. A comparison of…