化学物理

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A $b$-type electrostatic…

The electronic properties and optical response of ice and water are intricately shaped by their molecular structure, including the quantum mechanical nature of hydrogen atoms. In spite of numerous studies appeared over decades, a…

We have investigated how Langevin dynamics is affected by the friction coefficient using the novel algorithm ISOKANN, which combines the transfer operator approach with modern machine learning techniques. ISOKANN describes the dynamics in…

We present a novel way to predict molecular conformers through a simple formulation that sidesteps many of the heuristics of prior works and achieves state of the art results by using the advantages of scale. By training a diffusion…

We present an optimization strategy for atom-specific spin-polarization constants within the spin-polarized GFN2-xTB framework, aiming to enhance the accuracy of molecular simulations. We compare a sequential and global optimization of spin…

In recent years, the Na-ion SuperIonic CONductor (NASICON) based polyanionics are considered the pertinent cathode materials in sodium-ion batteries due to their 3D open framework, which can accommodate a wide range of Na content and can…

Symmetry-adapted perturbation theory (SAPT) is a popular and versatile tool to compute and decompose noncovalent interaction energies between molecules. The intramolecular SAPT (ISAPT) variant provides a similar energy decomposition between…

We present a computational scheme for predicting the ligands that bind to a pocket of known structure. It is based on the generation of a general abstract representation of the molecules, which is invariant to rotations, translations and…

Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction…

Spin-orbit coupling induces a current density in the ground state, which consequently requires a generalization for meta-generalized gradient approximations. That is, the exchange-correlation energy has to be constructed as an explicit…

Hydrogen bonds are typically treated as sufficiently localized directional intermolecular bonds, in which dispersion and electrostatic contributions can be distinguished. However, being formed chiefly due to the overlapping of p orbitals of…

A new computational framework for spinor-based relativistic exact two-component (X2C) calculations is developed using contracted basis sets with a spin-orbit contraction scheme. Generally contracted j-adapted basis sets using primitive…

Although Gillespie's algorithm is justified under a set of axioms based on the assumption of homogeneity of the system, many chemical systems deviate from this assumption, as is the case for reactions taking place in low-mobility media.…

Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…

In this article, we explore the dynamical decoherence of the chromophores within a green fluorescent protein when coupled to a finite-temperature dielectric environment. Such systems are of significant interest due to their anomalously long…

The stationary nonempirical simulations of Na+(H2O)n clusters with n in a range of 28 to 51 carried out at the density functional level with a hybrid B3LYP functional and the Born-Oppenheimer molecular dynamics modeling of the size selected…

Analysis of the electron density distribution in clusters composed of hydrogen fluoride, water, and ammonia molecules, especially within the hydrogen-bond domains, reveals the existence of both \sigma- and \pi-binding between molecules. The…

We inspect the origin of the inverted singlet-triplet gap (INVEST) and slow change in the reverse intersystem crossing (rISC) rate with temperature, as recently observed. A Wigner phase space study reveals, that though INVEST is found at…

The objective of this study is to explore conditions that facilitate a significant reduction in substrate temperature during diamond growth. The typical temperature for this process is around 1200K; we aim to reduce it to a much lower…

Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…