化学物理
We recently introduced a new theoretical description of Landau--Zener--St\"{u}ckelberg--Majorana (LZSM) transitions that accounts for both adiabatic and spin-dephasing losses during sweeps through resonance. Here, we use this new…
Perchloric acid (HClO$_4$) is widely used to prepare perchlorate salts with applications in propellants, industry, environmental chemistry, and biology. In this work, we used the intermolecular parameters from the extended Madrid-2019 force…
Literature values of disjoining pressure in liquid nanofilms from different molecular simulation methods show significant discrepancies. We demonstrate that these arise from neglecting long-range dispersion interactions and inconsistent…
Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…
We present the formulation and implementation of triples correction scheme to the relativistic equation-of-motion coupled-cluster method for ionization potential. Both full and partial triples correction schemes are implemented using the…
Cyclic swing adsorption processes, such as pressure/vacuum swing adsorption (PVSA), are a promising technology for upgrading biogas by separating carbon dioxide (CO2) from methane (CH4). The rational design of adsorbent materials with…
Accurate, global Potential Energy Surfaces (PES) expressed in sum-of-products (SOP) form are a prerequisite for efficient high-dimensional quantum dynamics simulations using the MCTDH method. This work introduces a methodology for…
In this work, we describe various improved implementations of the mapping approach to surface hopping (MASH) for simulating nonadiabatic dynamics. These include time-reversible and piecewise-continuous integrators, which is only formally…
We report on the control and characterization of the isomer population of ions inside superfluid helium nanodroplets, using two-color operation of a dual-oscillator infrared free-electron laser. The timing of both lasers is highly…
Predicting how protein mutations affect drug binding remains a major challenge, particularly when the mutations are distal from the binding site. In this study, we introduce a coupled simulation workflow that combines long-time-scale…
Liquid structure at solid-liquid interfaces is critical for many natural and engineered processes ranging from biological signal transduction to electrochemical energy conversion. Advanced experimental and computational methods have…
Machine learning models of chemical bioactivity are increasingly used for prioritizing a small number of compounds in virtual screening libraries for experimental follow-up. In these applications, assessing model accuracy by early hit…
The $\Delta$SCF DFT approach defines the system energy as a function of orbital occupancy. Inspired by Landau Fermi liquid theory, we develop an occupancy extrapolation (OE) method that captures excited-state energies via a Taylor expansion…
The third and fourth density and acoustic virial coefficients of neon were determined at temperatures between 10 and 5000 K from first principles employing the path-integral Monte Carlo (PIMC) approach. For these calculations, we used the…
Machine-learned interatomic potentials (MLIPs) are increasingly used to replace computationally demanding electronic-structure calculations to model matter at the atomic scale. The most commonly used model architectures are constrained to…
A time-domain representation of chromatographic peak shapes is presented as an analytic expression designed for high computational efficiency, which can be used for direct time-domain peak fitting with parameters that represent physical…
A faithful description of chemical processes requires exploring extended regions of the molecular potential energy surface (PES), which remains challenging for strongly correlated systems. Transferable deep-learning variational Monte Carlo…
Aqueous solutions of HF and HCl behave very differently at intermediate concentrations: HCl dissociates completely, whereas HF remains only partially dissociated and forms bifluoride (HF$_2^-$). This should lead to different excess-proton…
In complex molecular systems, the reaction coordinate (RC) that characterizes transition pathways is essential to understand underlying molecular mechanisms. This review surveys a framework for identifying the RC by applying deep learning…
Microalgae are an abundant bioorganic material source and play a significant role in life on Earth by conducting photosynthesis for carbon dioxide (CO2) capture and its conversion to oxygen (O2). In this study, a combination of microalgae…