Accelerated Bayesian Inference for Molecular Simulations using Local Gaussian Process Surrogate ModelsWhile Bayesian inference is the gold standard for uncertainty quantification and propagation, its use within physical chemistry encounters formidable computational barriers. These bottlenecks are…B. L. Shanks, H. W. Sullivan, A. R. Shazed et al.·Oct 29, 2023SaveLearn
Systematic Improvement of Empirical Energy Functions in the Era of Machine LearningThe impact of targeted replacement of individual terms in empirical force fields is quantitatively assessed for pure water, dichloromethane (DCM), and solvated K+ and Cl- ions. For the…Mike Devereux, Eric D. Boittier, Markus Meuwly·Oct 28, 2023SaveLearn
The Role of Reference Points in Machine-Learned Atomistic Simulation ModelsThis paper introduces the Chemical Environment Modeling Theory (CEMT), a novel, generalized framework designed to overcome the limitations inherent in traditional atom-centered Machine Learning Force…Xiangyun Lei, Weike Ye, Joseph Montoya et al.·Oct 28, 2023SaveLearn
First-principles molecular quantum electrodynamics theory at all coupling strengthsThe ever-growing intersection of quantum electrodynamics (QED) and molecular processes has shown remarkable and unanticipated advancements in altering molecular properties and reactivity by…Xinyang Li, Yu Zhang·Oct 27, 2023SaveLearn
Reaching high accuracy for energetic properties at second-order perturbation cost by merging self-consistency and spin-opposite scalingQuantum chemical methods dealing with challenging systems while retaining low computational costs have attracted attention. In particular, many efforts have been devoted to developing new methods…Nhan Tri Tran, Hoang Thanh Nguyen, Lan Nguyen Tran·Oct 27, 2023SaveLearn
Orbital-optimized Density Functional Calculations of Molecular Rydberg Excited States with Real Space Grid Representation and Self-Interaction CorrectionDensity functional calculations of Rydberg excited states up to high energy are carried out for several molecules using an approach where the orbitals are variationally optimized by converging on…Alec E. Sigurðarson, Yorick L. A. Schmerwitz, Dagrún K. V. Tveiten et al.·Oct 26, 2023SaveLearn
Universal method to extract the average electron spin relaxation in organic semiconductors from muonium ALC resonancesMuon spin spectroscopy and in particular the avoid level crossing (ALC) technique is a sensitive probe of electron spin relaxation (eSR) in organic semiconductors. In complex ALC spectra, eSR can be…Licheng Zhang, J. S. Lord, A. J. Drew·Oct 25, 2023SaveLearn
Unsupervised Learning of Molecular Embeddings for Enhanced Clustering and Emergent Properties for Chemical CompoundsThe detailed analysis of molecular structures and properties holds great potential for drug development discovery through machine learning. Developing an emergent property in the model to understand…Jaiveer Gill, Ratul Chakraborty, Reetham Gubba et al.·Oct 25, 2023SaveLearn
Singlet fission spin dynamics from molecular structure: a modular computational pipelineSinglet fission, which has applications in areas ranging form solar energy to quantum information, relies critically on transitions within a multi-spin manifold. These transitions are driven by…Dominic Jones, Thomas MacDonald, Timothy W. Schmidt et al.·Oct 24, 2023SaveLearn
Unveiling low THz Dynamics of Liquid Crystals: Identification of Intermolecular Interaction among Intramolecular ModesLiquid crystal based technologies have found considerably diversified uses and areas of application over the last few decades, proving to be excellent materials for tunable optical elements from…Patrick Friebel, Daria Ruth Galimberti, Matteo Savoini et al.·Oct 24, 2023SaveLearn
Label-free Imaging of Catalytic H2O2 Decomposition on Single Colloidal Pt Nanoparticles using Nanofluidic Scattering MicroscopySingle particle catalysis aims at determining factors that dictate nanoparticle activity and selectivity. Existing methods often use fluorescent model reactions at low reactant concentrations,…Björn Altenburger, Carl Andersson, Sune Levin et al.·Oct 24, 2023SaveLearn
Natural liquid organic hydrogen carrier with low dehydrogenation energy: A first principles studyLiquid organic hydrogen carriers (LOHCs) represent a promising approach for hydrogen storage due to their favorable properties including stability and compatibility with the existing infrastructure.…Chunguang Tang, Shunxin Fei, G. David Lin et al.·Oct 24, 2023SaveLearn
A Theoretical Perspective on the Photochemistry of Boron-Nitrogen Lewis AdductsBoron-Nitrogen (B-N) Lewis adducts form a versatile family of compounds with numerous applications in functional molecules. Despite the growing interest in this family of compounds for optoelectronic…Emanuele Marsili, Basile F. E. Curchod·Oct 23, 2023SaveLearn
Electric Fields in Liquid Water Irradiated with Protons at Ultrahigh Dose RatesWe study the effects of irradiating water with 3 MeV protons at high doses by observing the motion of charged polystyrene beads outside the proton beam. By single-particle tracking, we measure a…F. Gobet, P. Barberet, M. -H. Delville et al.·Oct 23, 2023SaveLearn
Nuclear mass and size corrections to the magnetic shieldingWe derive finite nuclear mass and finite nuclear size corrections to the magnetic shielding in light ions. These corrections are important for the accurate determination of nuclear magnetic moments.…Krzysztof Pachucki·Oct 23, 2023SaveLearn
Stochastic resolution of identity to CC2 for large systems: excited state propertiesWe apply a stochastic resolution of identity approximation (sRI) to the CC2 method for excitation energy calculations. A set of stochastic orbitals are employed to decouple the crucial 4-index…Chongxiao Zhao, Qi Ou, Joonho Lee et al.·Oct 23, 2023SaveLearn
Molecular integral equations theory in the near critical region of CO2Environmental concerns are driving the search for greener yet efficient solvents. Supercritical CO2 (scCO2) is a promising candidate due to its non-toxicity and the potential for reusing CO2…Mohamed Houssein Mohamed, Luc Belloni, Daniel Borgis et al.·Oct 23, 2023SaveLearn
Elastic and inelastic diffraction of fast neon atoms on a LiF surfaceGrazing incidence fast atom diffraction has mainly been investigated with helium atoms, considered as the best possible choice for surface analysis. This article presents experimental diffraction…Maxime Debiossac, Peng Pan, Philippe Roncin·Oct 23, 2023SaveLearn
What to Make of Zero: Resolving the Statistical Noise from Conformational Reorganization in Alchemical Binding Free Energy Estimates with Metadynamics SamplingWe introduce the self-Relative Binding Free Energy (self-RBFE) approach to evaluate the intrinsic statistical variance of dual-topology alchemical binding free energy estimators. The self-RBFE is the…Sheenam Khuttan, Emilio Gallicchio·Oct 22, 2023SaveLearn
Boundary homogenization for target search problemsIn this review, we describe several approximations in the theory of Laplacian transport near complex or heterogeneously reactive boundaries. This phenomenon, governed by the Laplace operator, is…Denis S. Grebenkov, Alexei T. Skvortsov·Oct 22, 2023SaveLearn
Kubo-Anderson theory of polariton lineshapeWe apply the Kubo-Anderson stochastic theory of molecular spectral lineshape to the case of polaritons formed in the collective strong coupling regime. We investigate both the fast and slow limits of…Clàudia Climent, Joseph E. Subotnik, Abraham Nitzan·Oct 20, 2023SaveLearn
Learning Interatomic Potentials at Multiple ScalesThe need to use a short time step is a key limit on the speed of molecular dynamics (MD) simulations. Simulations governed by classical potentials are often accelerated by using a multiple-time-step…Xiang Fu, Albert Musaelian, Anders Johansson et al.·Oct 20, 2023SaveLearn
Excited-State Downfolding Using Ground-State FormalismsDownfolding coupled cluster (CC) techniques are powerful tools for reducing the dimensionality of many-body quantum problems. This work investigates how ground-state downfolding formalisms can target…Nicholas P. Bauman·Oct 20, 2023SaveLearn
Beyond power density: unexpected scaling laws in scale up of characterization of reverse-electro-dialysis membranesBlue energy represents a large reservoir of renewable osmotic energy that can be converted into electricity by reverse electrodialysis (RED). This method is based on ion-exchange membrane. Before…Timothee Derkenne, Annie Colin, Corentin Tregouet·Oct 20, 2023SaveLearn
Variational Lang-Firsov approach plus Mller-Plesset perturbation theory with applications to ab initio polariton chemistryWe apply the Lang-Firsov (LF) transformation to electron-boson coupled Hamiltonians and variationally optimize the transformation parameters and molecular orbital coefficients to determine the ground…Zhi-Hao Cui, Arkajit Mandal, David R. Reichman·Oct 19, 2023SaveLearn