化学物理
Uncertainty quantification (UQ) to detect samples with large expected errors (outliers) is applied to reactive molecular potential energy surfaces (PESs). Three methods - Ensembles, Deep Evidential Regression (DER), and Gaussian Mixture…
We perform ab initio simulations of the total and partial Auger decay widths of 1s^-1, 2s^-1, and 2p^-1 ionized hydrogen sulfide and 2s^-1 ionized argon with non-Hermitian quantum chemistry. We use coupled cluster theory with single and…
Controlling the internal quantum states of chiral molecules for a selected enantiomer has a wide range of fundamental applications. Using tailored microwave fields, a chosen rotational state can be enriched for a selected enantiomer, even…
Data-driven generation of molecules with desired properties, also known as inverse molecular design (IMD), has attracted significant attention in recent years. Despite the significant progress in the accuracy and diversity of solutions,…
After photo-excitation of DNA, the excited electron (in the LUMO) and the remaining hole (in the HOMO) localized on the same DNA base form a bound pair, called the Frenkel exciton, due to their mutual Coulomb interaction. In this study, we…
The interplay between electronic and intramolecular high-frequency vibrational degrees of freedom is ubiquitous in natural light-harvesting systems. Recent studies have indicated that an intramolecular vibrational donor-acceptor frequency…
Here, we present a study combining Bayesian optimisation structural inference with the machine learning interatomic potential NequIP to accelerate and enable the study of the adsorption of the conformationally flexible lignocellulosic…
Symmetry provides a powerful machinery to classify, interpret, and understand quantum-mechanical theories and results. However, most contemporary quantum chemistry packages lack the ability to handle degeneracy and symmetry breaking…
Among the distinctive structural features of lithium ionic liquids (LILs), a novel class of single-component electrolytes, the variation of the electron-withdrawing group stands out as a key factor in determining their dynamics. To…
Much attention has been devoted to understanding the microscopic pathways of phase transition between two equilibrium condensed phases (such as liquids and solids). However, the microscopic pathways between non-equilibrium, non-diffusive…
Excited electronic states of molecules and solids play a fundamental role in fields such as catalysis and electronics. In electronic structure calculations, excited states typically correspond to saddle points on the surface described by…
The cumulant expansion of the Green's function is a computationally efficient beyond-$GW$ approach renowned for its significant enhancement of satellite features in materials. In contrast to the ubiquitous $GW$ approximation of many-body…
We present the first application to real molecular systems of the recently proposed linear-response theory for the density-based basis-set correction method [J. Chem. Phys. 158, 234107 (2023)]. We apply this approach to accelerate the…
Machine learning interatomic potentials (MLIPs) are an emerging modeling technique that promises to provide electronic structure theory accuracy for a fraction of its cost, however, the transferability of MLIPs is a largely unknown factor.…
Experimental insight into the elementary processes underlying charge transfer across interfaces has blossomed with the wide-spread availability of ultra-high vacuum set-ups that allow the preparation and characterization of solid surfaces…
We propose an array of ultracold polar molecules as a platform to study alignment transport between molecules. We envision a polar molecule being aligned with an intense off-resonant laser field whose alignment migrates to a nearby molecule…
Photoionization as a half-scattering process is not instantaneous. Usually, time delays in photoionization are of the order of few tens of attoseconds (1 as = 10$^{-18}$ s). While going from a single atom to a nano-object, one can expect…
Vibrational strong coupling can modify chemical reaction pathways in unconventional ways. Thus far, Fabry-Perot cavities formed by pairs of facing mirrors have been mostly utilized to achieve vibrational strong coupling. In this study, we…
We present a numerically exact approach for evaluating vibrationally resolved electronic spectra at finite temperatures using the coherence thermofield dynamics. In this method, which avoids implementing an algorithm for solving the von…
Molecular docking is an important tool for structure-based drug design, accelerating the efficiency of drug development. Complex and dynamic binding processes between proteins and small molecules require searching and sampling over a wide…