Molecular Simulations of Liquid Jet Explosions and Shock Waves Induced by X-Ray Free-Electron LasersX-ray free-electron lasers (XFELs) produce X-ray pulses with high brilliance and short pulse duration. These properties enable structural investigations of biomolecular nanocrystals, and they allow…Leonie Chatzimagas, Jochen S. Hub·Aug 4, 2022SaveLearn
Decay Processes in Cationic Alkali Metals in Microsolvated Clusters: A Complex Absorbing Potential Based Equation-of-Motion Coupled Cluster InvestigationWe have employed the highly accurate complex absorbing potential based ionization potential equation-of-motion coupled cluster singles and doubles (CAP-IP-EOM-CCSD) method to study the various…Ravi Kumar, Aryya Ghosh, Nayana Vaval·Aug 4, 2022SaveLearn
Barrier height prediction by machine learning correction of semiempirical calculationsDifferent machine learning (ML) models are proposed in the present work to predict DFT-quality barrier heights (BHs) from semiempirical quantum-mechanical (SQM) calculations. The ML models include…Xabier García-Andrade, Pablo García Tahoces, Jesús Pérez-Ríos et al.·Aug 3, 2022SaveLearn
Is there evidence for exponential quantum advantage in quantum chemistry?The idea to use quantum mechanical devices to simulate other quantum systems is commonly ascribed to Feynman. Since the original suggestion, concrete proposals have appeared for simulating molecular…Seunghoon Lee, Joonho Lee, Huanchen Zhai et al.·Aug 3, 2022SaveLearn
Effect of Protonation and Deprotonation on Electron Transfer Mediated Decay and Interatomic Coulombic DecayElectronically excited atoms or molecules in an environment are often subject to interatomic/intermolecular Coulombic decay (ICD) and/or electron transfer mediated decay (ETMD) mechanisms. A few of…Ravi Kumar, Dr. Nayana Vaval·Aug 3, 2022SaveLearn
A perturbative approximation to DFT/MRCI: DFT/MRCI(2)We introduce a perturbative approximation to the combined density functional theory and multireference configuration interaction (DFT/MRCI) method. The method, termed DFT/MRCI(2), results from the…Simon P. Neville, Michael S. Schuurman·Aug 3, 2022SaveLearn
Orientation Echoes via Concerted Terahertz and Near-IR excitationA new and efficient method for orientation echo spectroscopy is presented and realized experimentally. The excitation scheme utilizes concerted rotational excitations by both ultrashort terahertz and…Ran Damari, Amit Beer, Sharly Fleischer·Aug 3, 2022SaveLearn
S66x8 Noncovalent Interactions Revisited: New Benchmark and Performance of Composite Localized Coupled-Cluster MethodsThe S66x8 noncovalent interactions benchmark has been re-evaluated at the "sterling silver" level, using explicitly correlated MP2-F12 near the complete basis set limit,…Golokesh Santra, Emmanouil Semidalas, Nisha Mehta et al.·Aug 2, 2022SaveLearn
Twenty Years of Auxiliary-Field Quantum Monte Carlo in Quantum Chemistry: An Overview and Assessment on Main Group Chemistry and Bond-BreakingIn this work, we present an overview of the phaseless auxiliary-field quantum Monte Carlo (ph- AFQMC) approach from a computational quantum chemistry perspective, and present a numerical assessment…Joonho Lee, Hung Q. Pham, David R. Reichman·Aug 2, 2022SaveLearn
Understanding Dynamics in Coarse-Grained Models: II. Coarse-Grained Diffusion Modeled Using Hard Sphere TheoryThe first paper of this series [J. Chem. Phys. 158, 034103 (2023)] demonstrated that excess entropy scaling holds for both fine-grained and corresponding coarse-grained (CG) systems. Despite its…Jaehyeok Jin, Kenneth S. Schweizer, Gregory A. Voth·Aug 2, 2022SaveLearn
Observing Nearby Nuclei on Paramagnetic Trityls and MOFs via DNP and Electron DecouplingDynamic nuclear polarization (DNP) is an NMR sensitivity enhancement technique that mediates polarization transfer from unpaired electrons to NMR-active nuclei. Despite its success in elucidating…Kong Ooi Tan, Luming Yang, Michael Mardini et al.·Aug 2, 2022SaveLearn
Transfer learning for affordable and high quality tunneling splittings from instanton calculationsThe combination of transfer learning (TL) a low level potential energy surface (PES) to a higher level of electronic structure theory together with ring-polymer instanton (RPI) theory is explored and…Silvan Käser, Jeremy O. Richardson, Markus Meuwly·Aug 2, 2022SaveLearn
Kinetic energy density for open-shell systems: Analysis and development of a novel techniqueThe quest for an approximate yet accurate kinetic energy density functional is central to the development of orbital-free density functional theory. While a recipe for closed-shell systems has been…Priya Priya, Mainak Sadhukhan·Aug 1, 2022SaveLearn
Morphological Evolution of NMC Secondary Particles Through in situ electrochemical FIB/SEM experimentMicrostructural evolution of NMC secondary particles during the battery operation drives the electrochemical performance and impacts the Li-ion battery lifetime. In this work, we develop an in situ…François Cadiou, Tuan-Tu Nguyen, Martin Bettge et al.·Aug 1, 2022SaveLearn
Nonadiabatic forward flux sampling for excited-state rare eventsWe present a rare event sampling scheme applicable to coupled electronic excited states. In particular, we extend the forward flux sampling (FFS) method for rare event sampling to a nonadiabatic…Madlen Maria Reiner, Brigitta Bachmair, Maximilian Xaver Tiefenbacher et al.·Aug 1, 2022SaveLearn
Understanding Dynamics in Coarse-Grained Models: I. Universal Excess Entropy Scaling RelationshipCoarse-grained (CG) models facilitate an efficient exploration of complex systems by reducing the unnecessary degrees of freedom of the fine-grained (FG) system while recapitulating major structural…Jaehyeok Jin, Kenneth S. Schweizer, Gregory A. Voth·Jul 29, 2022SaveLearn
Theory of layered-oxide cathode degradation in Li-ion batteries by oxidation-induced cation disorderDisorder-driven degradation phenomena, such as structural phase transformations and surface reconstructions, can significantly reduce the lifetime of Li-ion batteries, especially those with…Debbie Zhuang, Martin Z. Bazant·Jul 29, 2022SaveLearn
Reweighted Manifold Learning of Collective Variables from Enhanced Sampling SimulationsEnhanced sampling methods are indispensable in computational physics and chemistry, where atomistic simulations cannot exhaustively sample the high-dimensional configuration space of dynamical…Jakub Rydzewski, Ming Chen, Tushar K. Ghosh et al.·Jul 29, 2022SaveLearn
Room Temperature DNP of Diamond Powder Using Frequency ModulationDynamic nuclear polarization (DNP) is a method of enhancing NMR signals via the transfer of polarization from electron spins to nuclear spins using on-resonance microwave (MW) irradiation. In most…Daphna Shimon, Kelly A. Cantwell, Linta Joseph et al.·Jul 29, 2022SaveLearn
The Valence-Bond Quantum Monte Carlo MethodThe VB-QMC method is presented in this chapter. It consists of using in quantum Monte Carlo (QMC) approaches with a wave function expressed as a usually short expansion of classical Valence-Bond (VB)…Slavko Radenković, Dominik Domin, Julien Toulouse et al.·Jul 29, 2022SaveLearn
Scalable Hybrid Deep Neural Networks/Polarizable Potentials Biomolecular Simulations including long-range effectsDeep-HP is a scalable extension of the \ multi-GPUs molecular dynamics (MD) package enabling the use of Pytorch/TensorFlow Deep Neural Networks (DNNs) models. Deep-HP increases DNNs MD…Théo Jaffrelot Inizan, Thomas Plé, Olivier Adjoua et al.·Jul 28, 2022SaveLearn
Differentiable quantum chemistry with PySCF for molecules and materials at the mean-field level and beyondWe introduce an extension to the PySCF package which makes it automatically differentiable. The implementation strategy is discussed, and example applications are presented to demonstrate the…Xing Zhang, Garnet Kin-Lic Chan·Jul 28, 2022SaveLearn
Collective response in light-matter interactions: The interplay between strong coupling and local dynamicsA model designed to mimic the implications of the collective optical response of molecular ensembles in optical cavities on molecular vibronic dynamics is investigated. Strong molecule-radiation…Bingyu Cui, Abraham Nitzan·Jul 28, 2022SaveLearn
4-component relativistic Hamiltonian with effective QED potentials for molecular calculationsWe report the implementation of effective QED potentials for all-electron 4-component relativistic molecular calculations using the DIRAC code. The potentials are also available for 2-component…Ayaki Sunaga, Maen Salman, Trond Saue·Jul 28, 2022SaveLearn
LLWP -- A new Loomis-Wood Software at the Example of Acetone-13C1Acetone-13C1 is a complex organic molecule with two internal methyl (-CH3) rotors having relatively low effective barriers to internal rotation of about 249 cm-1. This leads to two low-lying…Luis Bonah, Oliver Zingsheim, Holger S. P. Müller et al.·Jul 28, 2022SaveLearn