Understanding density driven errors for reaction barrier heightsDelocalization errors, such as charge-transfer and some self-interaction errors, plague computationally-efficient and otherwise-accurate density functional approximations (DFAs). Evaluating a…Aaron D. Kaplan, Chandra Shahi, Pradeep Bhetwal et al.·Jul 27, 2022SaveLearn
Sub-promille measurements and calculations of CO (3--0) overtone line intensitiesIntensities of lines in the near-infrared second overtone band (3--0) of 12C16O are measured and calculated to an unprecedented degree of precision and accuracy. Agreement between theory…K. Bielska, A. A. Kyuberis, Z. D. Reed et al.·Jul 27, 2022SaveLearn
A truncated Davidson method for the efficient "chemically accurate" calculation of full configuration interaction wavefunctions without any large matrix diagonalizationThis work develops and illustrates a new method of calculating "chemically accurate" electronic wavefunctions (and energies) via a truncated full configuration interaction (CI) procedure…Stephen J. Cotton·Jul 26, 2022SaveLearn
Transition1x -- a Dataset for Building Generalizable Reactive Machine Learning PotentialsMachine Learning (ML) models have, in contrast to their usefulness in molecular dynamics studies, had limited success as surrogate potentials for reaction barrier search. It is due to the scarcity of…Mathias Schreiner, Arghya Bhowmik, Tejs Vegge et al.·Jul 25, 2022SaveLearn
Coupled charge and energy transfer dynamics in light harvesting complexes from a hybrid hierarchical equations of motion approachWe describe a method for simulating exciton dynamics in protein-pigment complexes, including effects from charge transfer as well as fluorescence. The method combines the hierarchical equations of…Thomas P. Fay, David T. Limmer·Jul 24, 2022SaveLearn
Thermal half-lives of azobenzene derivatives: virtual screening based on intersystem crossing using a machine learning potentialMolecular photoswitches are the foundation of light-activated drugs. A key photoswitch is azobenzene, which exhibits trans-cis isomerism in response to light. The thermal half-life of the cis isomer…Simon Axelrod, Eugene Shakhnovich, Rafael Gomez-Bombarelli·Jul 23, 2022SaveLearn
A new framework for frequency-dependent polarizable force fieldsA frequency-dependent extension of the polarizable force field ``Atom-Condensed Kohn-Sham density functional theory approximated to the second-order'' (ACKS2) [J. Chem. Phys. 141, 194114…YingXing Cheng, Toon Verstraelen·Jul 23, 2022SaveLearn
Direct determination of optimal real-space orbitals for correlated electronic structure of moleculesWe demonstrate how to determine numerically nearly exact orthonormal orbitals that are optimal for evaluation of the energy of arbitrary (correlated) states of atoms and molecules by minimization of…Edward F. Valeev, Robert J. Harrison. Adam A. Holmes, Charles C. Peterson et al.·Jul 22, 2022SaveLearn
Magnetic-Translational Sum Rule and Approximate Models of the Molecular Berry CurvatureThe Berry connection and curvature are key components of electronic structure calculations for atoms and molecules in magnetic fields. They ensure the correct translational behavior of the effective…Laurens D. M. Peters, Tanner Culpitt, Erik I. Tellgren et al.·Jul 22, 2022SaveLearn
A Transferable Recommender Approach for Selecting the Best Density Functional Approximations in Chemical DiscoveryApproximate density functional theory (DFT) has become indispensable owing to its cost-accuracy trade-off in comparison to more computationally demanding but accurate correlated wavefunction theory.…Chenru Duan, Aditya Nandy, Ralf Meyer et al.·Jul 21, 2022SaveLearn
A Semiclassical Framework for Mixed Quantum Classical DynamicsSemiclassical approximations for quantum dynamic simulations in complex chemical systems range from rigorously accurate methods that are computationally expensive to methods that exhibit…Shreyas Malpathak, Matthew S. Church, Nandini Ananth·Jul 21, 2022SaveLearn
Spin-orbit transitions in the N+(3PJA) + H2 → NH+(X2Π, 4Σ-)+ H(2S) reaction, using adiabatic and mixed quantum-adiabatic statistical approachesThe cross section and rate constants for the title reaction are calculated for all the spin-orbit states of N+(3PJA) using two statistical approaches, one purely adiabatic and the other one…Susana Gomez-Carrasco, Daniel Felix-Gonzalez, Alfredo Aguado et al.·Jul 21, 2022SaveLearn
Franck-Condon spectra of unbound and imaginary-frequency vibrations via correlation functions: a branch-cut free, numerically stable derivationMolecular electronic spectra can be represented in the time domain as auto-correlation functions of the initial vibrational wavepacket. We present a derivation of the harmonic vibrational…P. Bryan Changala, Nadav Genossar, Joshua H. Baraban·Jul 21, 2022SaveLearn
Exploring the configurational space of amorphous graphene with machine-learned atomic energiesTwo-dimensionally extended amorphous carbon ("amorphous graphene") is a prototype system for disorder in 2D, showing a rich and complex configurational space that is yet to be fully understood. Here…Zakariya El-Machachi, Mark Wilson, Volker L. Deringer·Jul 19, 2022SaveLearn
Faster Exact Exchange for Solids via occ-RI-K: Application to Combinatorially Optimized Range-Separated Hybrid Functionals for Simple Solids with Pseudopotentials Near the Basis Set LimitIn this work, we developed and showcased the occ-RI-K algorithm to compute the exact exchange contribution in density functional calculations of solids near the basis set limit. Within the gaussian…Joonho Lee, Adam Rettig, Xintian Feng et al.·Jul 19, 2022SaveLearn
Spectroscopy from Machine Learning by Accurately Representing the Atomic Polar TensorVibrational spectroscopy is a key technique to elucidate microscopic structure and dynamics. Without the aid of theoretical approaches, it is however, often difficult to understand such spectra at a…Philipp Schienbein·Jul 18, 2022SaveLearn
A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and BenchmarkWe present the theory and the implementation of a low-cost four-component relativistic equation of motion coupled cluster method for ionized states based on frozen natural spinors. A single threshold…Kshitijkumar Surjuse, Somesh Chamoli, Malaya K. Nayak et al.·Jul 18, 2022SaveLearn
Active Spaces and Non-Orthogonal Configuration Interaction Approaches for Investigating Molecules on Metal SurfacesWe test a set of multiconfigurational wavefunction approaches for calculating the ground state electron population for a two-site Anderson model representing a molecule on a metal surface. In…Junhan Chen, Wenjie Dou, Joseph Subotnik·Jul 18, 2022SaveLearn
Long-Lived States of Methylene Protons in Achiral MoleculesIt is shown that long-lived states (LLS) involving pairs of methylene protons in nuclear magnetic resonance (NMR) can be readily excited in common molecules that contain two or more neighboring…Anna Sonnefeld, Aiky Razanahoera, Geoffrey Bodenhausen et al.·Jul 18, 2022SaveLearn
Structure, Organization and Heterogeneity of Water-Containing Deep Eutectic SolventsThe spectroscopy and structural dynamics of a deep eutectic mixture (KSCN/acetamide) with varying water content is investigated from 2D IR (with the C-N stretch vibration of the SCN- anions as the…Kai Töpfer, Andrea Pasti, Anuradha Das et al.·Jul 18, 2022SaveLearn
Molecular-orbital-based Machine Learning for Open-shell and Multi-reference Systems with Kernel Addition Gaussian Process RegressionWe introduce a novel machine learning strategy, kernel addition Gaussian process regression (KA-GPR), in molecular-orbital-based machine learning (MOB-ML) to learn the total correlation energies of…Lixue Cheng, Jiace Sun, J. Emiliano Deustua et al.·Jul 17, 2022SaveLearn
Echo-enhanced molecular orientation at high temperaturesUltrashort laser pulses are widely used for transient field-free molecular orientation -- a phenomenon important in chemical reaction dynamics, ultrafast molecular imaging, high harmonics generation,…Ilia Tutunnikov, Long Xu, Yehiam Prior et al.·Jul 17, 2022SaveLearn
Observation of Structure Evolution and Reaction Intermediates at the Gate-tunable Suspended Graphene/Electrolyte InterfaceGraphene serves as an ideal platform to investigate the microscopic structure and reaction kinetics at the graphitic electrode interfaces. However, graphene is susceptible to various extrinsic…Ying Xu, You-Bo Ma, Feng Gu et al.·Jul 17, 2022SaveLearn
Comment on 'Ultradense protium p(0) and deuterium D(0) and their relation to ordinary Rydberg matter: a review' 2019 Physica Scripta 94, 075005The article by Holmlid and Zeiner-Gundersen (2019, Physica Scripta, vol. 94, 075005) contains a number of claims that explicitly or implicitly contradict fundamental knowledge of modern science. Some…Klavs Hansen, Jos Engelen·Jul 17, 2022SaveLearn
Learning inducing points and uncertainty on molecular data by scalable variational Gaussian processesUncertainty control and scalability to large datasets are the two main issues for the deployment of Gaussian process (GP) models within the autonomous machine learning-based prediction pipelines in…Mikhail Tsitsvero, Mingoo Jin, Andrey Lyalin·Jul 16, 2022SaveLearn