化学物理
Investigating processes in complex molecular systems, which are characterized by many variables, is a crucial problem in computational physics. These systems can be reduced to a few meaningful degrees of freedom known as collective…
Graphene oxide (GO) materials are widely studied, and yet their atomic-scale structures remain to be fully understood. Here we show that the chemical and configurational space of GO can be rapidly explored by advanced machine-learning…
Hydrogen has been identified as a clean, zero carbon, sustainable, and promising energy source for the future, and electrochemical water splitting for hydrogen production is an emission-free, efficient energy conversion technology. A major…
In an effort to increase the speed and efficiency of ballistic energy transport via oligomeric chains, we performed measurements of the transport in compounds featuring long alkyl chains of up to 37 methylene units. Compounds of the…
To understand the recently observed mysterious non-adiabatic energy transfer for hyperthermal H atom scattering from a semiconductor surface, Ge(111)c(2*8), we present a mixed quantum-classical non-adiabatic molecular dynamics model based…
We embark on a quest to identify small molecules in the chemical space that can potentially violate Hund's rule. Utilizing twelve TDDFT approximations and the ADC(2) many-body method, we report the energies of S$_1$ and T$_1$ excited states…
We present a combined experimental and theoretical investigation of the radiationless decay spectrum of an O 1s double core hole in liquid water. Our experiments were carried out using liquid-jet electron spectroscopy from cylindrical…
Ab initio molecular dynamics (AIMD) simulations have been performed on aqueous solutions of four simple sugars, {\alpha}-D-glucose, \b{eta}-D-glucose, {\alpha}-D-mannose and {\alpha}-D-galactose. Hydrogen bonding (HB) properties, such as…
Quantum chemical calculations of one-photon absorption, electronic circular dichroism and anisotropy factor spectra for the A-band transition of fenchone, camphor and 3-methylcyclopentanone (3MCP) are reported. While the only weakly allowed…
We show empirically that a phase-space non-Born-Oppenheimer electronic Hamiltonian approach to quantum chemistry (where the electronic Hamiltonian is parameterized by both nuclear position and momentum, (H(R,P)) is both a practical and…
The performance of time-independent, orbital optimized calculations of excited states is assessed with respect to charge transfer excitations in organic molecules in comparison to the linear-response time-dependent density functional theory…
The properties of supercritical fluids are dictated by intermolecular interactions that involve two or more molecules. Such intermolecular interactions were described via intermolecular potentials in historical supercritical combustion…
Transition metal ions play crucial roles in the structure and function of numerous proteins, contributing to essential biological processes such as catalysis, electron transfer, and oxygen binding. However, accurately modeling the…
We investigate the impact of electronic correlations and quantum delocalization onto the static structure factor and static density response function of the strongly coupled electron liquid. In contrast to a classical system, the density…
We report on a theoretical study of a Cs$_2$ molecule illuminated by two lasers and show how it can result in novel quantum dynamics. We reveal that these interactions facilitate the bypass of the non-crossing rule, forming Light-Induced…
Nuclear spin hyperpolarization provides a promising route to overcome the challenges imposed by the limited sensitivity of nuclear magnetic resonance. Here we demonstrate that dissolution of spin-polarized pentacene-doped naphthalene…
Reduced order models based on the transport of a lower dimensional manifold representation of the thermochemical state, such as Principal Component (PC) transport and Machine Learning (ML) techniques, have been developed to reduce the…
[Abridged] The extension of conceptual DFT to include external fields in chemical systems is utilised to investigate the effects of strong magnetic fields on the electronic charge distribution and its consequences on the reactivity of…
Literate programming - the bringing together of program code and natural language narratives - has become a ubiquitous approach in the realm of data science. This methodology is appealing as well for the domain of Density Functional Theory…
Forte is an open-source library specialized in multireference electronic structure theories for molecular systems and the rapid prototyping of new methods. This paper gives an overview of the capabilities of Forte, its software…