Chemical Physics
This work reports an efficient density-fitting implementation of the density-based basis-set correction (DBBSC) method in the MOLPRO software. This method consists in correcting the energy calculated by a wave-function method with a given…
Hierarchy configuration interaction (hCI) has been recently introduced as an alternative configuration interaction (CI) route combining excitation degree and seniority number, which showed to efficiently recover both dynamic and static…
Most mathematical models of the transport of charged species in battery electrodes require a constitutive relation describing intercalation of Lithium, which is a reversible process taking place on the interface between the electrolyte and…
The relative energies of different phases or polymorphs of molecular solids can be small, less than a kiloJoule/mol. Reliable description of such energy differences requires high quality treatment of electron correlations, typically beyond…
An approach to modeling the oligomer composition distribution function in the irreversible step growth homopolymerization process based on a mixture of oligomers of arbitrary composition is developed. The approach is based on consideration…
In this work, we present ab initio cavity QED methods which include interactions with a static magnetic field and nuclear spin degrees of freedom using different treatments of the quantum electromagnetic field. We derive explicit…
We developed a mid-infrared optical frequency comb-based Fourier-transform spectrometer and performed a line-shape study of the fundamental vibrational band of CO perturbed by N${_2}$, which is crucial for atmospheric science and…
Short nanopores find extensive applications capitalizing on their high throughput and detection resolution. Ionic behaviors through long nanopores are mainly determined by charged inner-pore walls. When pore lengths decrease to sub-200 nm,…
We present the result of our calculations of ultrafast electron diffraction (UED) for cyclobutanone excited into $S_2$ electronic state, which are based on the non-adiabatic dynamics simulations with \textit{Ab Initio} Multiple Cloning…
Recent years have seen vast progress in the development of machine learned force fields (MLFFs) based on ab-initio reference calculations. Despite achieving low test errors, the reliability of MLFFs in molecular dynamics (MD) simulations is…
Silicon is a promising anode material for next-generation lithium-ion batteries. However, the volume change and the voltage hysteresis during lithiation and delithiation are two substantial drawbacks to their lifetime and performance. We…
The tiny-core generalized (Gatchina) relativistic pseudopotential (GRPP) model provides an accurate approximation for many-electron Hamiltonians of molecules containing heavy atoms, ensuring a proper description of the effects of…
The reaction dynamics of H$_2$COO to form linear HCOOH and dioxirane as first steps for OH-elimination is quantitatively investigated. Using a machine learned potential energy surface at the CASPT2/aug-cc-pVTZ level of theory vibrational…
Quantum dynamics simulations are becoming a standard tool for simulating photo-excited molecular systems involving a manifold of coupled states, known as non-adiabatic dynamics. While these simulations have had many successes in explaining…
This research examines the nonadiabatic dynamics of cyclobutanone after excitation into the n-3s Rydberg S2 state. It stems from our contribution to the Special Topic of the Journal of Chemical Physics to test the predictive capability of…
The multistate Bennett acceptance ratio (MBAR) method is a prevalent approach for computing free energies of thermodynamic states. In this work, we introduce BayesMBAR, a Bayesian generalization of the MBAR method. By integrating…
Owing to ring-strain, cyclic ketones exhibit complex excited-state dynamics with multiple competing photochemical channels active on the ultrafast timescale. While the excited-state dynamics of cyclobutanone after $\pi^{\ast}\leftarrow n$…
The comprehension of nonadiabatic dynamics in polyatomic systems relies heavily on the simultaneous advancements in theoretical and experimental domains. The gas-phase electron diffraction (GUED) technique has attracted widespread attention…
Molecular orbital theory is powerful both as a conceptual tool for understanding chemical bonding, and as a theoretical framework for ab initio quantum chemistry. Despite its undoubted success, MO theory has well documented shortcomings,…
Frozen natural orbitals (FNOs) are used to augment IP/EA-EOM-CCSD calculations targeting the band gap of trans-polyacetylene and polyacene. We show the resulting electron affinities (EAs), ionization potentials (IPs), and extrapolated band…