化学物理
Accurate and fast thermophysical models are needed to embed vapor-liquid equilibrium (VLE) calculations in design, optimization, and control loops for cryogenic mixtures. This study asks whether a structure-aware graph neural network (GNN;…
Machine learning potentials have become a standard tool for atomistic materials modelling. While models continue to become more generalisable, an open challenge relates to efficient uncertainty predictions for active learning and robust…
In this study, we investigate the effect of incorporating explicit dispersion interactions in the functional form of machine learning interatomic potentials (MLIPs), particularly in the Moment Tensor Potential and Equivariant Tensor Network…
We develop an algorithm for bosonic path integral molecular dynamics (PIMD) simulations with periodic boundary conditions (PBC) that scales quadratically with the number of particles. Path integral methods are a powerful tool to simulate…
To determine the effect of nonradiative excitation energy transfer on the fluorescence of a rigid multicomponent solution, a new analytical method was developed by treating this transfer as a time-resolved Markov chain (TRMC). In the TRMC…
Ring Polymer Surface-Hopping (RPSH) has been recently introduced as a well-tailored method for incorporating nuclear quantum effects (NQEs), such as zero-point energy and tunneling, into non-adiabatic molecular dynamics simulations. The…
Controlling chemical and material properties through strong light-matter coupling in optical cavities has gained considerable attention over the past decade. However, the underlying mechanisms remain insufficiently understood, and a…
Strain-level identification of viruses is critical for effective public health responses to potential outbreaks, yet current diagnostic methods often lack the necessary speed or sensitivity. Surface-enhanced Raman spectroscopy (SERS) offers…
Electrochemical energy and substance conversion devices involve complex electrode processes, characterized by multiple charge transfer steps, competing pathways, and various intermediates. Such complexity makes it challenging to enhance…
Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question…
Poor scaling of dynamics simulations with number of dimensions is currently a major limiting factor in the simulation of photochemical processes. In this work, we investigate ways to reduce the dimensionality of many-atom systems with a…
Symmetry governs nature's law, yet many of the natural phenomena occur due to the breakdown of symmetry. Here, we show how isotope-induced inversion symmetry breaking influences ultrafast photoisomerization processes in ethylene. Using…
This study investigates the H2O and CO2 sorption behavior of two ion exchange sorbents: a primary amine and a permanently charged strong base quaternary ammonium (QA) with (bi)carbonate counter-anions.
While the variational principle for excited-state energies leads to a route to obtaining excited-state densities from time-dependent density functional theory, relatively little attention has been paid to the quality of the resulting…
Advanced X-ray spectroscopic techniques are widely recognized as state-of-the-art tools for probing the electronic structure, bonding, and chemical environments of the heaviest elements in the periodic table. In this study, we employ X-ray…
The multiphoton ionization of the simplest aromatic amine, aniline, was examined utilizing a kinetic energy-correlated time-of-flight mass spectrometer at a wavelength of 266 nm. The primary and secondary fragment channels have been…
We investigate configuration-interaction (CI) calculations on a basis of molecular orbitals generated by preliminary density-functional theory (DFT) calculations. We use this CI/DFT framework to improve the modeling of core-excited states…
Molten salts are high-temperature ionic liquids whose unique combination of strong Coulombic interactions, large polarizabilities, and high ionic conductivities makes them central to energy storage, metallurgy, and nuclear technology.…
Methods for reconstructing the spectral density of a vibrational environment from experimental data can yield key insights into the impact of the environment on molecular function. Although such experimental methods exist, they generally…
The experimental realization of strong light-matter coupling with molecules initiated the rapidly evolving field of molecular polaritonics. Most studies focus on how exciton polaritons, which combine electronic excitations with confined…