化学物理
Ultrafast reaction processes take place when resonant features of nonlinear model systems are taken into account. In the targeted energy or electron transfer dimer model this is accomplished through the implementation of nonlinear…
In all applications of Density Functional Theory there is always a degree of one-electron self-interaction error (SIE). Here, we propose a simple self-interaction correction by applying an effective core potential (ECP) that replaces no…
Solid electrolytes with fast ion transport are one of the key challenges for solid state lithium metal batteries. To improve ion conductivity, chemical doping has been the most effective strategy, and atomistic simulation with…
We assessed three schemes for propagating a variable-width (thawed) Gaussian wave packet moving under the influence of Morse or double-well potentials with parameters that are chemically representative. The most rigorous scheme is based on…
Quantum computing, with its superior computational capabilities compared to classical approaches, holds the potential to revolutionize numerous scientific domains, including pharmaceuticals. However, the application of quantum computing for…
Attosecond science offers unprecedented precision in probing the initial moments of chemical reactions, revealing the dynamics of molecular electrons that shape reaction pathways. A fundamental question emerges: what role, if any, do…
Modern graphics processing units (GPUs) provide an unprecedented level of computing power. In this study, we present a high-performance, multi-GPU implementation of the analytical nuclear gradient for Kohn-Sham time-dependent density…
The physicochemical characterization of trivalent ions is limited due to a lack of accurate force fields. By leveraging the latest machine learning force field to model aqueous $\text{AlCl}_{3}$, we discover that upon dissolution of…
Akin to the traditional quasi-classical trajectory method for investigating the dynamics on a single adiabatic potential energy surface for an elementary chemical reaction, we carry out the dynamics on a 2-state ab initio potential energy…
With the establishment of machine learning (ML) techniques in the scientific community, the construction of ML potential energy surfaces (ML-PES) has become a standard process in physics and chemistry. So far, improvements in the…
Non-adiabatic coupling matrix elements (NACMEs) are important in quantum chemistry, particularly for molecular dynamics methods such as surface hopping. However, NACMEs are gauge dependent. This presents a difficulty for their calculation…
The reactivity and mechanistic intricacies of azatrienes in Diels-Alder reactions have been relatively unexplored despite their intriguing potential applications. In this study, we employ Molecular Electron Density Theory to theoretically…
Recent theoretical studies have explored how ultra-strong light--matter coupling can be used as a handle to control chemical transformations. {\em Ab initio} cavity quantum electrodynamics (QED) calculations demonstrate that large changes…
Fermi's golden rule (FGR) offers an empirical framework for understanding the dynamics of spin-lattice relaxation in magnetic molecules, encompassing mechanisms like direct (one-phonon) and Raman (two-phonon) processes. These principles…
We simulate the photodynamics of gas-phase cyclobutanone excited to the S$_2$ state using fewest switches surface hopping (FSSH) dynamics powered by time-dependent density functional theory (TDDFT). We predict a total C3+C2 photoproduct…
We introduce FENNIX (Force-Field-Enhanced Neural Network InteraXions), a hybrid approach between machine-learning and force-fields. We leverage state-of-the-art equivariant neural networks to predict local energy contributions and multiple…
We investigate the possibility of using a transcorrelated Hamiltonian to describe electron correlation. Amethod to obtain transcorrelatedwavefunctionswas developed based on the mathematical framework of the bi-variational principle. This…
We show that the complete photoemission dynamics in situations of electron-ion entanglement can be retrieved from photoelectron spectral measurements without information on the ion. To this end, we develop an energy-time analysis of the…
Ambient condition linear amines, from propylamine up to nonylamine, are studied by x-ray scattering and Molecular Dynamics simulations of various force field models. The major finding is that the pre-peak in alkylamines is of about one…
In molecular dynamics simulations, rare events, such as protein folding, are typically studied using enhanced sampling techniques, most of which are based on the definition of a collective variable (CV) along which acceleration occurs.…