Stretching bonds in Density Functional Theory without artificial symmetry breakingAccurate first-principles calculations for the energies, charge distributions, and spin symmetries of many-electron systems are essential to understand and predict the electronic and structural…Yuming Shi, Yi Shi, Adam Wasserman·May 22, 2023SaveLearn
Impact of Electron-Withdrawing Groups on Ion Transport and Structure in Lithium Borate Ionic LiquidsAmong 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…Volodymyr Koverga, Selvaraj S. Chandrasekaran, Anh T. Ngo·May 22, 2023SaveLearn
Effect of framework composition and NH3 on the diffusion of Cu+ in Cu-CHA catalysts predicted by machine-learning accelerated molecular dynamicsCu-exchanged zeolites rely on mobile solvated Cu+ cations for their catalytic activity, but the role of framework composition on transport is not fully understood. Ab initio molecular dynamics…Reisel Millan, Estefania Bello-Jurado, Manual Moliner et al.·May 22, 2023SaveLearn
On De Gennes Narrowing of Fluids Confined at the Molecular Scale in Nanoporous MaterialsBeyond well-documented confinement and surface effects arising from the large internal surface and severely confining porosity of nanoporous hosts, the transport of nanoconfined fluids remains…Wanda Kellouai, Jean-Louis Barrat, Patrick Judeinstein et al.·May 22, 2023SaveLearn
A Non-stochastic Optimization Algorithm for Neural-network Quantum StatesNeural-network quantum states (NQS) employ artificial neural networks to encode many-body wave functions in second quantization through variational Monte Carlo (VMC). They have recently been applied…Xiang Li, Jia-Cheng Huang, Guang-Ze Zhang et al.·May 22, 2023SaveLearn
Stereo-Electronic Factors Influencing the Stability of Hydroperoxyalkyl Radicals: Transferability of Chemical Trends across Hydrocarbons and ab initio MethodsThe hydroperoxyalkyl radicals (.QOOH) are known to play a significant role in combustion and tropospheric processes, yet their direct spectroscopic detection remains challenging. In this study, we…Saurabh Chandra Kandpal, Kgalaletso P. Otukile, Shweta Jindal et al.·May 22, 2023SaveLearn
Corrosion rates under charge-conservation conditionsLaboratory and numerical corrosion experiments impose an electric potential on the metal surface, differing from natural corrosion conditions, where corrosion typically occurs in the absence of…Tim Hageman, Carmen Andrade, Emilio Martínez-Pañeda·May 20, 2023SaveLearn
Coupled Chemical Reactions: Effects of Electric Field, Diffusion and Boundary ControlChemical reactions involve the movement of charges, and this work presents a mathematical model for describing chemical reactions in electrolytes. The model is developed using an energy variational…Shixin Xu, Robert Eisenberg, Zilong Song et al.·May 20, 2023SaveLearn
Data-driven Refinement of Electronic Energies from Two-Electron Reduced-Density-Matrix TheoryThe exponential computational cost of describing strongly correlated electrons can be mitigated by adopting a reduced density-matrix (RDM)-based description of the electronic structure. While…Grier M. Jones, Run. R. Li, A. Eugene DePrince et al.·May 20, 2023SaveLearn
Analytic evaluation of non-adiabatic couplings within the complex absorbing potential equation-of-motion coupled-cluster methodWe present the theory for the evaluation of non-adiabatic couplings (NACs) involving resonance states within the complex absorbing potential equation-of-motion coupled-cluster (CAP-EOM-CC) framework…Koushik Chatterjee, Zsuzsanna Koczor-Benda, Xintian Feng et al.·May 19, 2023SaveLearn
Multi-Fidelity Machine Learning for Excited State Energies of MoleculesThe accurate but fast calculation of molecular excited states is still a very challenging topic. For many applications, detailed knowledge of the energy funnel in larger molecular aggregates is of…Vivin Vinod, Sayan Maity, Peter Zaspel et al.·May 18, 2023SaveLearn
Beyond Cavity Born-Oppenheimer: On Non-Adiabatic Coupling and Effective Ground State Hamiltonians in Vibro-Polaritonic ChemistryThe emerging field of vibro-polaritonic chemistry studies the impact of light-matter hybrid states known as vibrational polaritons on chemical reactivity and molecular properties. Here, we discuss…Eric W. Fischer, Peter Saalfrank·May 18, 2023SaveLearn
Exact tunneling splittings from symmetrized path integralsWe develop a new simulation technique based on path-integral molecular dynamics for calculating ground-state tunneling splitting patterns from ratios of symmetrized partition functions. In…George Trenins, Lars Meuser, Hannah Bertschi et al.·May 18, 2023SaveLearn
Machine learning interatomic potentials for reactive hydrogen dynamics at metal surfaces based on iterative refinement of reaction probabilitiesReactive chemistry of molecular hydrogen at surfaces, notably dissociative sticking and hydrogen evolution, plays a crucial role in energy storage and fuel cells. Theoretical studies can help to…Wojciech G. Stark, Julia Westermayr, Oscar A. Douglas-Gallardo et al.·May 18, 2023SaveLearn
Accurate Fourth-Generation Machine Learning Potentials by Electrostatic EmbeddingIn recent years, significant progress has been made in the development of machine learning potentials (MLPs) for atomistic simulations with applications in many fields from chemistry to materials…Tsz Wai Ko, Jonas A. Finkler, Stefan Goedecker et al.·May 18, 2023SaveLearn
Prompt Engineering for Transformer-based Chemical Similarity Search Identifies Structurally Distinct Functional AnaloguesChemical similarity searches are widely used in-silico methods for identifying new drug-like molecules. These methods have historically relied on structure-based comparisons to compute molecular…Clayton W. Kosonocky, Aaron L. Feller, Claus O. Wilke et al.·May 17, 2023SaveLearn
Interatomic and intermolecular Coulombic decay rates from equation-of-motion coupled-cluster theory with complex basis functionsWhen a vacancy is created in an inner-valence orbital of a dimer of atoms or molecules, the resulting species can undergo interatomic/intermolecular Coulombic decay (ICD): the hole is filled through…Valentina Parravicini, Thomas-C. Jagau·May 17, 2023SaveLearn
Manipulation of Charge Delocalization in a Bulk Heterojunction Material Using a Mid-Infrared Push PulseIn organic bulk heterojunction materials, charge delocalization has been proposed to play a vital role in the generation of free carriers by reducing the Coulomb attraction via an interfacial charge…Angela Montanaro, Kyu Hyung Park, Francesca Fassioli et al.·May 17, 2023SaveLearn
Self-interaction and transport of solvated electrons in molten saltsThe dynamics of (few) electrons dissolved in an ionic fluid--as when a small amount of metal is added to a solution while upholding its electronic insulation--manifests interesting properties that…Paolo Pegolo, Stefano Baroni, Federico Grasselli·May 17, 2023SaveLearn
Low-data deep quantum chemical learning for accurate MP2 and coupled-cluster correlationsAccurate ab-initio prediction of electronic energies is very expensive for macromolecules by explicitly solving post-Hartree-Fock equations. We here exploit the physically justified local correlation…Wai-Pan Ng, Qiujiang Liang, Jun Yang·May 17, 2023SaveLearn
Riemannian Trust Region Method for Minimization of Fourth Central Moment for Localized Molecular OrbitalsThe importance of Localized Molecular Orbitals in correlation treatments beyond mean-field calculation and in the illustration of chemical bonding can hardly be overstated. However, generation of…Aliakbar Sepehri, Run R. Li, Mark R. Hoffmann·May 16, 2023SaveLearn
Mller-Plesset and density-fixed adiabatic connections for a model diatomic system at different correlation regimesIn recent years, Adiabatic Connection Interpolations developed within Density Functional Theory (DFT) have been found to provide satisfactory performances in the calculation of interaction energies…Sara Giarrusso, Aurora Pribram-Jones·May 16, 2023SaveLearn
Cavity Click Chemistry: Cavity-Catalyzed Azide-Alkyne CycloadditionClick chemistry, which refers to chemical reactions that are fast, selective, and with high product yields, has become a powerful approach in organic synthesis and chemical biology. Due to the…Fabijan Pavosevic, Robert L. Smith, Angel Rubio·May 16, 2023SaveLearn
Fully First-Principles Surface Spectroscopy with Machine LearningOur current understanding of the structure and dynamics of aqueous interfaces at the molecular level has grown substantially in the last few decades due to the continuous development of…Yair Litman, Jinggang Lan, Yuki Nagata et al.·May 16, 2023SaveLearn
Orientation dependent etching of silicon by fluorine molecules: a quantum chemistry computational studyAnisotropic etching is a widely used process in semiconductor manufacturing, in particular for micro- and nano-scale texturing of silicon surfaces for black silicon production. The typical process of…Omesh Dhar Dwivedi, Yuri Barsukov, Sierra Jubin et al.·May 15, 2023SaveLearn