Theoretical proposal of a revolutionary water-splitting photocatalyst: The monolayer of boron phosphideRecently, hydrogen generation by water-splitting photocatalysts is attracting attention as a sustainable and clean energy resource. Photocatalytic hydrogen-generation systems are much simpler,…Tatsuo Suzuki·Apr 4, 2022SaveLearn
Atomistic Global Optimization X: A Python package for optimization of atomistic structuresModelling and understanding properties of materials from first principles require knowledge of the underlying atomistic structure. This entails knowing the individual identity and position of all…Mads-Peter Verner Christiansen, Nikolaj Rønne, Bjørk Hammer·Apr 4, 2022SaveLearn
RE-EDS Using GAFF Topologies: Application to Relative Hydration Free-Energy Calculations for Large Sets of MoleculesFree-energy differences between pairs of end-states can be estimated based on molecular dynamics (MD) simulations using standard pathway-dependent methods such as thermodynamic integration (TI),…Salome R. Rieder, Benjamin Ries, Kay Schaller et al.·Apr 4, 2022SaveLearn
Possible Ribose Synthesis in Carbonaceous PlanetesimalsThe origin of life might be sparked by the polymerization of the first RNA molecules in Darwinian ponds during wet-dry cycles. The key life-building block ribose was found in carbonaceous chondrites.…Klaus Paschek, Kai Kohler, Ben K. D. Pearce et al.·Apr 4, 2022SaveLearn
q-AQUA: a many-body CCSD(T) water potential, including 4-body interactions, demonstrates the quantum nature of water from clusters to the liquid phaseMany model potential energy surfaces (PESs) have been reported for water; however, none are strictly from "first principles". Here we report such a potential, based on a many-body…Qi Yu, Chen Qu, Paul L. Houston et al.·Apr 4, 2022SaveLearn
Wavefunction Embedding for Molecular PolaritonsPolaritonic chemistry relies on the strong light-matter interaction phenomena for altering the chemical reaction rates inside optical cavities. To explain and to understand these processes, the…Fabijan Pavošević, Angel Rubio·Apr 4, 2022SaveLearn
On the Suppression and Enhancement of Thermal Chemical Rates in a CavityThe observed modification of thermal chemical rates in Fabry-Perot cavities remains a poorly understood effect theoretically. Recent breakthroughs explain some of the observations through the…Jing Sun, Oriol Vendrell·Apr 4, 2022SaveLearn
Mixed Chiral and Achiral Character in Substituted Ethane: A Next Generation QTAIM PerspectiveWe use the newly introduced spanning stress tensor trajectory Uσ-space construction within next generation quantum theory of atoms in molecules (NG-QTAIM) for a chirality investigation of singly…Zi Li, Tianlv Xu, Herbert Früchtl et al.·Apr 4, 2022SaveLearn
Leading correction to the local density approximation for exchange in large-Z atomsThe large-Z asymptotic expansion of atomic energies has been useful in determining exact conditions for corrections to the local density approximation in density functional theory. The correction…Nathan Argaman, Jeremy Redd, Antonio C. Cancio et al.·Apr 3, 2022SaveLearn
Reduced-density-matrix-based ab initio cavity quantum electrodynamicsA reduced-density-matrix (RDM)-based approach to ab initio cavity quantum electrodynamics (QED) is developed. The expectation value of the Pauli-Fierz Hamiltonian is expressed in terms of one-…Joel D. Mallory, A. Eugene DePrince·Apr 2, 2022SaveLearn
Understanding the Spin Crossover Dynamical Effects of the Dioxygen Binding and Activation on HOD enzymeFor the cofactor-free 1-H-3-hydroxy-4-oxoquinaldine-2,4-dioxygenase (HOD), the dioxygen (O2) dependent steps are rate-limiting along with a spin state crossover to the singlet spin state. Here, the…Likai Du·Apr 2, 2022SaveLearn
Quantum tunnelling driven H2 formation on grapheneIt is commonly believed that it is unfavourable for adsorbed H atoms on carbonaceous surfaces to form H2 without the help of incident H atoms. Using ring-polymer instanton theory to describe…Erxun Han, Wei Fang, Michail Stamatakis et al.·Apr 2, 2022SaveLearn
Reduced density matrix functional theory from an ab initio seniority-zero wave function: Exact and approximate formulations along adiabatic connection pathsCurrently, there is a growing interest in the development of a new hierarchy of methods based on the concept of seniority, which has been introduced quite recently in quantum chemistry. Despite the…Bruno Senjean, Saad Yalouz, Naoki Nakatani et al.·Apr 1, 2022SaveLearn
Determination of the recombination coefficient in electrolytic solutions from impedance spectroscopy measurementsThe dependence of the actual/effective ionic concentration on the nominal salt concentration is experimentally investigated for aqueous solutions of NaCl and KCl. The actual ionic bulk density is…G. Barbero, N. G. Fytas, I. Lelidis et al.·Apr 1, 2022SaveLearn
Ab initio machine learning of phase space averagesEquilibrium structures determine material properties and biochemical functions. We propose to machine learn phase-space averages, conventionally obtained by ab initio or force-field based…Jan Weinreich, Dominik Lemm, Guido Falk von Rudorff et al.·Mar 31, 2022SaveLearn
Exchange energies with forces in density-functional theoryWe propose exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation…Nicolas Tancogne-Dejean, Markus Penz, Andre Laestadius et al.·Mar 31, 2022SaveLearn
Surface microlenses for much more efficient photodegradation in water treatmentThe global need for clean water requires sustainable technology for purifying contaminated water. Highly efficient solar-driven photodegradation is a sustainable strategy for wastewater treatment. In…Qiuyun Lu, Qiwei Xu, Jia Meng et al.·Mar 31, 2022SaveLearn
SELFIES and the future of molecular string representationsArtificial intelligence (AI) and machine learning (ML) are expanding in popularity for broad applications to challenging tasks in chemistry and materials science. Examples include the prediction of…Mario Krenn, Qianxiang Ai, Senja Barthel et al.·Mar 31, 2022SaveLearn
Automatic Identification of Chemical MoietiesIn recent years, the prediction of quantum mechanical observables with machine learning methods has become increasingly popular. Message-passing neural networks (MPNNs) solve this task by…Jonas Lederer, Michael Gastegger, Kristof T. Schütt et al.·Mar 30, 2022SaveLearn
On the Origins of Life's Homochirality: Inducing Enantiomeric Excess with Spin-Polarized ElectronsLife as we know it is homochiral, but the origins of biological homochirality on early Earth remain elusive. Shallow closed-basin lakes are a plausible prebiotic environment on early Earth, and most…S. Furkan Ozturk, Dimitar D. Sasselov·Mar 30, 2022SaveLearn
Can second-order perturbation theory accurately predict electron density of open-shell molecules? The importance of self-consistencyElectron density distribution plays an essential role in predicting molecular properties. It is also a simple observable from which machine-learning models for molecular electronic structure can be…Lan Nguyen Tran·Mar 30, 2022SaveLearn
A Continuum of Physics-Based Lithium-Ion Battery Models ReviewedPhysics-based electrochemical battery models derived from porous electrode theory are a very powerful tool for understanding lithium-ion batteries, as well as for improving their design and…Ferran Brosa Planella, Weilong Ai, Adam M. Boyce et al.·Mar 30, 2022SaveLearn
Benchmarking Structural Evolution Methods for Training of Machine Learned Interatomic PotentialsWhen creating training data for machine-learned interatomic potentials (MLIPs), it is common to create initial structures and evolve them using molecular dynamics to sample a larger configuration…Michael J. Waters, James M. Rondinelli·Mar 30, 2022SaveLearn
Accurate Deep Learning-aided Density-free Strategy for Many-Body Dispersion-corrected Density Functional TheoryUsing a Deep Neuronal Network model (DNN) trained on the large ANI-1 data set of small organic molecules, we propose a transferable density-free many-body dispersion model (DNN-MBD). The DNN strategy…Pier Paolo Poier, Théo Jaffrelot Inizan, Olivier Adjoua et al.·Mar 29, 2022SaveLearn
Quantum Machine Learning Corrects Classical Force Fields: Stretching DNA Base Pairs in Explicit SolventIn order to improve the accuracy of molecular dynamics simulations, classical force fields are supplemented with a kernel-based machine learning method trained on quantum-mechanical fragment…Joshua T. Berryman, Amirhossein Taghavi, Florian Mazur et al.·Mar 29, 2022SaveLearn