化学物理
Spontaneous emission and internal conversion rates are calculated within harmonic approximations and compared to results obtained within the semi-classical extended thawed Gaussian approximation. This is the first application of the ETGA in…
The self-assembled monolayers of alkane thiolates on Ag (111) surfaces and nanoparticles are studied using molecular dynamics. Reactive force fields allow simulations of very large systems such as nanoparticles of 10 nm. Stable (sqrt(7) X…
A light-matter hybrid quasiparticle, called a polariton, is formed when molecules are strongly coupled to an optical cavity. Recent experiments have shown that polariton chemistry can manipulate chemical reactions. Polariton chemistry is a…
XYG3-type doubly hybrid approximations (xDH) have gained a widespread recognition for their accuracy in describing a diverse range of chemical and physical interactions. However, a recent study (J. Phys. Chem. 2021, 12, 800-807) has…
This work combines for the first time ab initio molecular dynamics (AIMD) within the Born-Oppenheimer approximation, with a global natural orbital functional (GNOF), an approximate functional of the one-particle reduced density matrix. The…
The correct interpretation of magnetic properties in the weak-exchange regime has remained a challenging task for several decades. In this regime, the effective exchange interaction between local spins is quite weak, of the same order of…
In this article we present a machine learning model to obtain fast and accurate estimates of the molecular Hessian matrix. In this model, based on a random forest, the second derivatives of the energy with respect to redundant internal…
Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…
We describe a multiple electronic state adaptation of the mapping approach to surface hopping introduced recently by Mannouch and Richardson (J. Chem. Phys. 158, 104111 (2023)). This adaptation treats populations and coherences on an equal…
We propose to relax geometries throughout chemical compound space (CCS) using alchemical perturbation density functional theory (APDFT). APDFT refers to perturbation theory involving changes in nuclear charges within approximate solutions…
Experiments have demonstrated that vibrational strong coupling between molecular vibrations and light modes can significantly change molecular properties, such as ground-state reactivity. Theoretical studies towards the origin of this…
Traditional theories of the NMR autocorrelation function for intramolecular dipole pairs assume single-exponential decay, yet the calculated autocorrelation of realistic systems display a rich, multi-exponential behavior resulting in…
In recent years, deep learning has made remarkable strides, surpassing human capabilities in tasks like strategy games, and it has found applications in complex domains, including protein folding. In the realm of quantum chemistry, machine…
Even though nucleation is ubiquitous in different science and engineering problems, investigating nucleation is extremely difficult due to the complicated ranges of time and length scales involved. In this work, we simulate NaCl nucleation…
The calculation of molecular excited states is critically important to decipher a plethora of molecular properties. In this manuscript, we develop an equation of motion formalism on top of a bi-exponentially parametrized ground state…
The conventional approaches to the inverse density functional theory problem typically assume non-degeneracy of the Kohn-Sham (KS) eigenvalues, greatly hindering their use in open-shell systems. We present a generalization of the inverse…
We propose an efficient deterministic method to calculate the full configuration interaction (FCI) ground state energy. This method leverages the sparseness of the Lanczos basis vectors that span the Krylov subspace associated with the…
Recent developments in machine learning interatomic potentials (MLIPs) have empowered even non-experts in machine learning to train MLIPs for accelerating materials simulations. However, the current literature lacks clear standards for…
An exchange-correction to the Fixed Diagonal Matrices (FDM) method is introduced to improve accuracy when employing a single reference wavefunction. Also, the performance of the Becke-Roussel exchange-hole for approximating the pair density…
We formulate a one-center non-orthogonal configuration interaction singles (1C-NOCIS) theory for the computation of core excited states of an initial singlet state with two unpaired electrons. This model, which we refer to as 1C-NOCIS…