Donnan equilibrium in charged slit-pores from a hybrid nonequilibrium Molecular Dynamics / Monte Carlo method with ions and solvent exchangeIon partitioning between different compartments (e.g. a porous material and a bulk solution reservoir), known as Donnan equilibrium, plays a fundamental role in various contexts such as…Jeongmin Kim, Benjamin Rotenberg·May 29, 2024SaveLearn
Screening and antiscreening effects in endohedral nanotubesRecently we investigated from first principles screening properties in systems where small molecules, characterized by a finite electronic dipole moment, are encapsulated into different nanocages.…Pier Luigi Silvestrelli, Matteo Tessarolo, Abdolvahab Seif et al.·May 29, 2024SaveLearn
Design and Implementation of a New Apparatus for Astrochemistry: Kinetic Measurements of the CH + OCS Reaction and Frequency Comb Spectroscopy in a Cold Uniform Supersonic FlowWe present the development of a new astrochemical research tool HILTRAC, the Highly Instrumented Low Temperature ReAction Chamber. The instrument is based on a pulsed form of the CRESU (Cin\'etique…Daniel I. Lucas, Théo Guillaume, Dwayne E. Heard et al.·May 29, 2024SaveLearn
Effective phase diffusion for spin phase evolution under random nonlinear magnetic fieldThe general theoretical description of spin self-diffusion under nonlinear gradient is proposed, which extends the effective phase diffusion method for linear gradient field. Based on the phase…Guoxing Lin·May 28, 2024SaveLearn
A physics-inspired evolutionary machine learning method: from the Schr\"odinger equation to an orbital-free-DFT kinetic energy functionalWe introduce a machine learning (ML) supervised model function that is inspired by the variational principle of physics. This ML hypothesis evolutionary method, termed ML-Omega, allows us to go from…Juan I. Rodriguez, Ulises A. Vergara-Beltran·May 28, 2024SaveLearn
Ensemble Generalization of the Perdew-Zunger Self-Interaction Correction: a Way Out of Multiple Minima and Symmetry BreakingThe Perdew-Zunger (PZ) self-interaction correction (SIC) is an established tool to correct unphysical behavior in density functional approximations. Yet, PZ-SIC is well-known to sometimes break…Sebastian Schwalbe, Wanja Timm Schulze, Kai Trepte et al.·May 28, 2024SaveLearn
Fine Tuning of the Rotational Rate of Light-Driven, Second Generation Molecular Motors by Fluorine SubstitutionsThe relaxation time of several second generation molecular motors is analysed by calculating the minimum energy path between the metastable and stable states and evaluating the transition rate within…Ivan Tambovtsev, Yorick L. A. Schmerwitz, Gianluca Levi et al.·May 28, 2024SaveLearn
A Theoretical Framework for an Efficient Normalizing Flow-Based Solution to the Electronic Schrodinger EquationA central problem in quantum mechanics involves solving the Electronic Schrodinger Equation for a molecule or material. The Variational Monte Carlo approach to this problem approximates a particular…Daniel Freedman, Eyal Rozenberg, Alex Bronstein·May 28, 2024SaveLearn
The influence of solvent on surface adsorption and desorptionThe adsorption and desorption of reactants and products from a solid surface is essential for achieving sustained surface chemical reactions. At a liquid-solid interface, these processes can involve…Ardavan Farahvash, Mayank Agrawal, Adam P. Willard et al.·May 28, 2024SaveLearn
Computing solvation free energies of small molecules with experimental accuracyFree energies play a central role in characterising the behaviour of chemical systems and are among the most important quantities that can be calculated by molecular dynamics simulations. Solvation…J. Harry Moore, Daniel J. Cole, Gabor Csanyi·May 28, 2024SaveLearn
Water at negative pressure: Nuclear quantum effectsVarious condensed phases of water, spanning from the liquid state to multiple ice phases, have been systematically investigated under extreme conditions of pressure and temperature to delineate their…Carlos P. Herrero, Rafael Ramirez·May 28, 2024SaveLearn
Molecular Structure and Rotational Dynamics in the Acetonitrile:Acetylene (1:2) Plastic Co-Crystal at Titan ConditionsThe surface of Saturn's moon Titan is coated with small molecule organic solids termed cryominerals. Cryominerals play an analogous role to minerals on Earth in Titan's surface geology and…Atul C. Thakur, Richard C. Remsing·May 28, 2024SaveLearn
The significance of fuzzy boundaries of the barrier regions in single-molecule measurements of failed barrier crossing attemptsA recent experimental study reports on measuring the temporal duration and the spatial extent of failed attempts to cross an activation barrier (i.e., "loops") for a folding transition in a single…Alexander M. Berezhkovskii, Dmitrii E. Makarov·May 27, 2024SaveLearn
Simulating Attochemistry: Which Dynamics Method to Use?Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be…Thierry Tran, Anthony Ferté, Morgane Vacher·May 27, 2024SaveLearn
Which Electronic Structure Method to Choose in Trajectory Surface Hopping Dynamics Simulations? Azomethane as a Case StudyNon-adiabatic dynamics simulations have become a standard approach to explore photochemical reactions. Such simulations require underlying potential energy surfaces and couplings between them,…Thomas V. Papineau, Denis Jacquemin, Morgane Vacher·May 27, 2024SaveLearn
Dissociation and isomerization following ionization of ethylene: insights from non-adiabatic dynamics simulationsPhotoionized and electronically excited ethylene C2H4+ can undergo H-loss, H2-loss, and ethylene-ethylidene isomerization, where the latter entails a hydrogen migration. Recent…Lina Fransén, Thierry Tran, Saikat Nandi et al.·May 27, 2024SaveLearn
Do Molecular Geometries Change Under Vibrational Strong Coupling?As pioneering experiments have shown, strong vibrational coupling between molecular vibrations and light modes in an optical cavity can significantly alter molecular properties and even affect…Thomas Schnappinger, Markus Kowalewski·May 27, 2024SaveLearn
An improved penalty-based excited-state variational Monte Carlo approach with deep-learning ansatzesWe introduce several improvements to the penalty-based variational quantum Monte Carlo (VMC) algorithm for computing electronic excited states of Entwistle et al. [M. T. Entwistle…P. Bernát Szabó, Zeno Schätzle, Mike T. Entwistle et al.·May 27, 2024SaveLearn
Stochastically accelerated perturbative triples correction in coupled cluster calculationsWe introduce a novel algorithm that leverages stochastic sampling techniques to compute the perturbative triples correction in the coupled-cluster (CC) framework. By combining elements of randomness…Yann Damour, Alejandro Gallo, Anthony Scemama·May 27, 2024SaveLearn
Renormalized Internally-Contracted Multireference Coupled Cluster with Perturbative TriplesIn this work, we combine the many-body formulation of the internally contracted multireference coupled cluster (ic-MRCC) method with Evangelista's multireference formulation of the driven similarity…Robin Feldmann, Markus Reiher·May 25, 2024SaveLearn
The Singlet-Triplet Gap of Cyclobutadiene: The CIPSI-Driven CC(P;Q) StudyAn accurate determination of singlet-triplet gaps in biradicals, including cyclobutadiene in the automerization barrier region where one has to balance the substantial nondynamical many-electron…Swati S. Priyadarsini, Karthik Gururangan, Jun Shen et al.·May 24, 2024SaveLearn
Sensitivity of Kβ mainline X-ray emission to structural dynamics in iron photosensitizerPhotochemistry and photophysics processes involve structures far from equilibrium. In these reactions, there is often strong coupling between nuclear and electronic degrees of freedom. For first-row…Johanna Rogvall, Roshan Singh, Morgane Vacher et al.·May 24, 2024SaveLearn
Discovering deposition process regimes: leveraging unsupervised learning for process insights, surrogate modeling, and sensitivity analysisThis work introduces a comprehensive approach utilizing data-driven methods to elucidate the deposition process regimes in Chemical Vapor Deposition (CVD) reactors and the interplay of physical…Geremy Loachamín Suntaxi, Paris Papavasileiou, Eleni D. Koronaki et al.·May 24, 2024SaveLearn
Syngas conversion to higher alcohols via wood-framed Cu/Co-carbon catalystSyngas conversion into higher alcohols represents a promising avenue for transforming coal or biomass into liquid fuels. However, the commercialization of this process has been hindered by the high…Guihua Yan, Paulina Pršlja, Gaofeng Chen et al.·May 24, 2024SaveLearn
Plasmon-driven substitution of 4 mercaptophenylboronic acid to 4-nitrothiophenol monitored by surface-enhanced Raman spectroscopyPlasmon-driven reactions on plasmonic nanoparticles (NPs) occur under significantly different conditions from those of classical organic synthesis and provide a promising pathway for enhancing the…Jan Kozisek, Jana Hrncirova, Miroslav Slouf et al.·May 24, 2024SaveLearn