Exact two-component TDDFT with simple two-electron picture-change corrections: X-ray absorption spectra near L- and M-edges of four-component quality at two-component costX-ray absorption spectroscopy (XAS) has gained popularity in recent years as it probes matter with high spatial and elemental sensitivity. However, the theoretical modelling of XAS is a challenging…Lukas Konecny, Stanislav Komorovsky, Jan Vicha et al.·Nov 29, 2022SaveLearn
The Interplay between Disorder, Local Relaxation and Collective Behaviors for an ensemble of emitters outside vs inside cavityThe interplay between collective optical response and molecular static and dynamic disorder is studied using simple effective Hamiltonians for an ensemble of two-level emitters inside and outside a…Zeyu Zhou, Hsing-Ta Chen, Joseph E. Subotnik et al.·Nov 29, 2022SaveLearn
Towards Pair Atomic Density Fitting for Correlation Energies with Benchmark AccuracyPair atomic density fitting (PADF) is a promising strategy to reduce the scaling with system size of quantum chemical methods for the calculation of the correlation energy like the direct random…Edoardo Spadetto, Pier Herman Theodoor Philipsen, Arno Förster et al.·Nov 29, 2022SaveLearn
Long-range Corrected Fragment Molecular Orbital Density-Functional Tight-binding Method for Excited States in Large Molecular SystemsHerein, we present a new method to efficiently calculate electronically excited states in large molecular assemblies, consisting of hundreds of molecules. For this purpose, we combine the long-range…Richard Einsele, Joscha Hoche, Roland Mitric·Nov 29, 2022SaveLearn
Jumping kinetic Monte Carlo: Fast and accurate simulations of partially delocalised charge transport in organic semiconductorsDeveloping devices using disordered organic semiconductors requires accurate and practical models of charge transport. In these materials, charge transport occurs through partially delocalised states…Jacob T. Willson, William Liu, Daniel Balzer et al.·Nov 29, 2022SaveLearn
Enhanced chiral-sensitivity of Coulomb-focused electrons in strong field ionizationStrong-field light-matter interactions initiate a wide range of phenomena in which the quantumpaths of electronic wavepackets can be manipulated by tailoring the laser field. Among the…S Rozen, S Larroque, N Dudovich et al.·Nov 29, 2022SaveLearn
Implementation of Bounded Diffusion Impedance in a Model Pyeis to Correctly Simulate Flow Gradient on Channel-Electrode in MicrofluidicsHere, we proposed to test the limits of the bounded diffusion impedance model by using electrochemical impedance spectroscopy (EIS) measurements in a microfluidic device architecture bearing a set of…Rassen Boukraa, Claire Poujouly, Pedro Gonzalez-Losada et al.·Nov 29, 2022SaveLearn
A Mean-Field Treatment of Vacuum Fluctuations in Strong Light-Matter CouplingMean-field mixed quantum--classical dynamics could provide a much-needed means to inexpensively model quantum electrodynamical phenomena, by describing the optical field and its vacuum fluctuations…Ming-Hsiu Hsieh, Alex Krotz, Roel Tempelaar·Nov 29, 2022SaveLearn
EMReact: A Tool for Modelling Electromagnetic Field Induced Effects in Chemical Reactions by Solving the Discrete Stochastic Master EquationThe effects of electromagnetic fields (EMF) have been widely debated concerning their role in chemical reactions. Reactions usually took hours or days to complete, and have been shown to happen a…Kelvin Dsouza, Daryoosh Vashaee·Nov 28, 2022SaveLearn
Analysis and Optimization of Resonance Energies and Widths Using Complex Absorbing PotentialsComplex absorbing potentials (CAPs) are artificial potentials added to electronic Hamiltonians to make the wavefunction of metastable electronic states square-integrable. This makes the electronic…Jerryman A. Gyamfi, Thomas -C. Jagau·Nov 28, 2022SaveLearn
The role of symmetric vibrational modes in the dehoherence of correlation-driven charge migrationDue to the electron correlation, a fast removal of an electron from a molecule may create a coherent superposition of cationic states and in this way initiate pure electronic dynamics in which the…J. Vester, V. Despré, A. I. Kuleff·Nov 28, 2022SaveLearn
Characterizing Reaction Route Map of Realistic Molecular Reactions based on Weight Rank Clique Filtration of Persistent HomologyA reaction route map (RRM) constructed using the GRRM program is a collection of elementary reaction pathways, each of which comprises two equilibrium (EQ) geometries and one transition state (TS)…Burai Murayama, Masato Kobayashi, Masamitsu Aoki et al.·Nov 28, 2022SaveLearn
Theoretical Investigation of The X-Ray Stark Effect in Small MoleculesWe have studied the Stark effect in the soft x-ray region for various small molecules by calculating the field-dependent x-ray absorption spectra. This effect is explained in terms of the response of…Avdhoot Datar, Catherine Wright, Devin A. Matthews·Nov 27, 2022SaveLearn
High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validationQuantum chemical calculations on atomistic systems have evolved into a standard approach to study molecular matter. These calculations often involve a significant amount of manual input and expertise…Jan P. Unsleber, Hongbin Liu, Leopold Talirz et al.·Nov 27, 2022SaveLearn
Ultra-Fast Semi-Empirical Quantum Chemistry for High-Throughput Computational Campaigns with SparrowSemi-empirical quantum chemical approaches are known to compromise accuracy for feasibility of calculations on huge molecules. However, the need for ultrafast calculations in interactive quantum…Francesco Bosia, Peikun Zheng, Alain Vaucher et al.·Nov 25, 2022SaveLearn
Understanding the anomalously low dielectric constant of confined water: an ab initio studyRecent experiments have shown that the out-of-plane dielectric constant of water confined in nanoslits of graphite and hexagonal boron nitride (hBN) is vanishingly small. Despite extensive effort…Thomas Dufils, Christoph Schran, Ji Chen et al.·Nov 25, 2022SaveLearn
A Self-Attention Ansatz for Ab-initio Quantum ChemistryWe present a novel neural network architecture using self-attention, the Wavefunction Transformer (Psiformer), which can be used as an approximation (or Ansatz) for solving the many-electron…Ingrid von Glehn, James S. Spencer, David Pfau·Nov 24, 2022SaveLearn
Twisted carotenoids do not support efficient intramolecular singlet fission in the orange carotenoid proteinSinglet exciton fission is the spin-allowed generation of two triplet electronic excited states from a singlet state. Intramolecular singlet fission has been suggested to occur on individual…George A. Sutherland, James P. Pidgeon, Harrison Ka Hin Lee et al.·Nov 24, 2022SaveLearn
Enhanced Sampling for Free Energy Profiles with Post-Transition-State BifurcationsWe present a method to explore the free energy landscapes of chemical reactions with post-transition-state bifurcations using an enhanced sampling method based on well-tempered metadynamics.…Juno Nam, YounJoon Jung·Nov 24, 2022SaveLearn
Long-range interactions of aromatic molecules with alkali-metal and alkaline-earth-metal atomsThe isotropic and anisotropic coefficients Cl,mn of the long-range spherical expansion 1/Rn (R -- the intermolecular distance) of the dispersion and inductions intermolecular energies…Leonid Shirkov, Michał Tomza·Nov 23, 2022SaveLearn
Supervised Pretraining for Molecular Force Fields and Properties PredictionMachine learning approaches have become popular for molecular modeling tasks, including molecular force fields and properties prediction. Traditional supervised learning methods suffer from scarcity…Xiang Gao, Weihao Gao, Wenzhi Xiao et al.·Nov 23, 2022SaveLearn
Triple excitations in Green's function coupled cluster solver for studies of strongly correlated systems in the framework of self-energy embedding theoryEmbedding theories became important approaches used for accurate calculations of both molecules and solids. In these theories, a small chosen subset of orbitals is treated with an accurate method,…Avijit Shee, Chia-Nan Yeh, Bo Peng et al.·Nov 23, 2022SaveLearn
Molecular Dynamics Study of Plasmon-Mediated Chemical TransformationsHeterogeneous catalysis of adsorbates on metallic surfaces mediated by plasmon has potential high photoelectric conversion efficiency and controllable reaction selectivity. Theoretical modeling of…Xiaoyan Wu, Tammo van der Heide, Thomas Frauenheim et al.·Nov 22, 2022SaveLearn
The role of steric effects on hydrogen atom transfer reactionsWe explored how steric effects influence the rate of hydrogen atom transfer (HAT) reactions between oxyradicals and alkanes. Quantum chemical computations of transition states show that activation…Yi Sun, Jacob N. Sanders, K. N. Houk·Nov 22, 2022SaveLearn
How to validate machine-learned interatomic potentialsMachine learning (ML) approaches enable large-scale atomistic simulations with near-quantum-mechanical accuracy. With the growing availability of these methods there arises a need for careful…Joe D. Morrow, John L. A. Gardner, Volker L. Deringer·Nov 22, 2022SaveLearn