化学物理

Stochastic electronic structure theories, e.g., Quantum Monte Carlo methods, enable highly accurate total energy calculations which in principle can be used to construct highly accurate potential energy surfaces. However, their stochastic…

State-specific complete active space self-consistent field (SS-CASSCF) theory has emerged as a promising route to accurately predict electronically excited energy surfaces away from molecular equilibria. However, its accuracy and…

We propose an approach to represent the second-quantized electronic Hamiltonian in a compact sum-of-products (SOP) form. The approach is based on the canonical polyadic decomposition (CPD) of the original Hamiltonian projected onto the…

The process of dissociation for two hydrofluorocarbon molecules in low triplet states excited by electron impact in plasma is investigated by ab initio Molecular Dynamics (AIMD). The interest in dissociation of hydrofluorocarbons in plasma…

Recently, we introduced a class of molecular representations for kernel-based regression methods -- the spectrum of approximated Hamiltonian matrices (SPA$^\mathrm{H}$M) -- that takes advantage of lightweight one-electron Hamiltonians…

Structure and function in nanoscale atomistic assemblies are tightly coupled, and every atom with its specific position and even every electron will have a decisive effect on the electronic structure, and hence, on the molecular properties.…

Uncertainty control and scalability to large datasets are the two main issues for the deployment of Gaussian process (GP) models within the autonomous machine learning-based prediction pipelines in material science and chemistry. One way to…

Physics-inspired molecular representations are the cornerstone of similarity-based learning applied to solve chemical problems. Despite their conceptual and mathematical diversity, this class of descriptors shares a common underlying…

This research introduces a Machine Learning-centric approach to replicate olfactory experiences, validated through experimental quantification of perfume perception. Key contributions encompass a hybrid model connecting perfume molecular…

We propose a new formulation of time-dependent coupled cluster with adaptive basis functions and division of the one-particle space into active and secondary subspaces. The formalism is fully bivariational in the sense of a real-valued…

Here we assess two machine-learned potentials, one using the symmetric gradient domain machine learning (sGDML) method and one based on permutationally invariant polynomials (PIPs). These are successors to a PIP potential energy surface…

For years, theoretical calculations and scalable computer simulations have complemented ultrafast experiments as they offer the advantage to overcome experimental restrictions and have access to the whole dynamics. This synergy between…

The charge/mass distribution f(q/m) of nanodrops and ions electrosprayed in vacuum from mixtures of formamide (FM) and methylammonium formate (MAF) is studied by time of flight mass spectrometry at MAF/FM volumetric concentrations of 5%,…

The many-body Green's function provides access to electronic properties beyond density functional theory level in ab inito calculations. In this manuscript, we propose a deep learning framework for predicting the finite-temperature Green's…

Molecules that violate Hund's rule and exhibit an inverted gap between the lowest singlet $S_1$ and triplet $T_1$ excited states have attracted considerable attention due to their potential applications in optoelectronics. Amongst these…

To enrich and enhance the diversity of the \textsc{quest} database of highly-accurate excitation energies [\href{https://doi.org/10.1002/wcms.1517}{V\'eril \textit{et al.}, \textit{WIREs Comput.~Mol.~Sci.}~\textbf{11}, e1517 (2021)}], we…

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…