化学物理
We present a channel-resolved interpretation of laser-driven Coulomb explosion of the HCl dimer from an ensemble of trajectories. Three dominant outcomes are identified: a minor three-body channel and two four-body channels (sequential and…
We develop an axiomatic reconstruction of thermodynamics based entirely on two primitive components: a description of what aspects of a system are observed and a reference measure that encodes the underlying descriptive convention. These…
A simplification of the VV10 van der Waals density functional [J. Chem. Phys. 133, 244103 (2010)] is made by an approximation of the integrand of the six-dimentional integral in terms of a few products of three-dimensional density-like…
The development of reliable luminescent nanothermometers for cryogenic applications is essential for advancing quantum technologies, superconducting systems, and other fields that require precise, high-spatial-resolution temperature…
Nonadiabatic molecular dynamics simulations aim to describe the coupled electron-nuclear dynamics of molecules in excited electronic states. These simulations have been applied to understand a plethora of photochemical and photophysical…
There will be a paradigm shift in chemical and biological research, to be enabled by autonomous, closed-loop, real-time self-directed decision-making experimentation. Spectrum-to-structure correlation, which is to elucidate molecular…
Incorporating self-interaction corrections (SIC) significantly improves chemical reaction barrier height predictions made using density functional theory methods. We present a detailed, orbital-by-orbital analysis of these corrections for…
Progress towards quantum utility in chemistry requires not only algorithmic advances, but also the identification of chemically meaningful problems whose electronic structure fundamentally challenges classical methods. Here, we introduce a…
In the study of non-adiabatic chemical processes such as photocatalysis and photosynthesis, non-adiabatic molecular dynamics (NAMD) is an indispensable theoretical tool, which requires precise potential energy surfaces (PESs) of ground and…
Computational high-throughput virtual screening is essential for identifying redox-active molecules for sustainable applications such as electrochemical carbon capture. A primary challenge in this approach is the high computational cost…
We demonstrate for the specific case of $C_{3v}$ how the direct-product decomposition scheme for the treatment of symmetry in coupled-cluster (CC) calculations can be extended to non-Abelian point groups. We show that for the two-electron…
The molecular electrostatic potential (MEP) is a key quantity for describing and predicting intermolecular and ion-molecule interactions. Here, we assess the ability of machine-learning (ML) models to infer the MEP, based on the equivariant…
Flavins are the chromophores in several blue-light-sensitive photoreceptor proteins and act as redox cofactors in many enzymes relevant for biological processes. Despite their biological relevance and numerous, detailed optical…
Accurately capturing electron correlation in large-scale molecular systems remains one of the foremost challenges in quantum chemistry and a primary driver for the development of quantum algorithms. Classical configuration-interaction…
Effective water management is essential for the optimal performance of PEM fuel cells. We have developed an impedance model for liquid water transport through the membrane and coupled it with the two-phase model for cathode side impedance.…
A capacitor consisting of the [bmim][NTf$_2$] ionic liquid (IL) confined in between planar graphite electrodes has been investigated by molecular dynamics based on an all-atom, unpolarizable force field. Despite a few peculiarities due to…
In transitions between different environmental settings, a molecular system inevitably undergoes a range of detectable changes, and the ability to accurately simulate such responses, e.g., in the form of shifts to molecular energies,…
Strong light--matter interactions forming hybrid quasiparticles termed polaritons can specifically tailor molecular photophysics. In this spirit, enhancing energy transport has recently been of special interest. Exciton--exciton…
The spectroscopic fingerprints of vibrationally excited states of astronomical molecules are interesting for multiple reasons. They are excellent temperature probes of the corresponding astronomical regions and are thought to be the origin…
Nickel/zinc (Ni/Zn) technology is a promising post-lithium battery type for stationary applications with respect to aspects such as safety, environmental compatibility and resource availability. Although this battery type has been known for…