Implementation of time-dependent Hartree-Fock in real spaceTime-dependent Hartree-Fock (TDHF) is one of the fundamental post-Hartree-Fock (HF) methods to describe excited states. In its Tamm-Dancoff form, equivalent to Configuration Interaction Singles, it…Uday Panta, David A. Strubbe·May 2, 2024SaveLearn
FeNNol: an Efficient and Flexible Library for Building Force-field-enhanced Neural Network PotentialsNeural network interatomic potentials (NNPs) have recently proven to be powerful tools to accurately model complex molecular systems while bypassing the high numerical cost of ab-initio molecular…Thomas Plé, Olivier Adjoua, Louis Lagardère et al.·May 2, 2024SaveLearn
Scalable Ab Initio Electronic Structure Methods with Near Chemical Accuracy for Main Group ChemistryThis study evaluates the precision of widely recognized quantum chemical methodologies, CCSD(T), DLPNO-CCSD(T) and localized ph-AFQMC, for determining the thermochemistry of main group elements.…Yujing Wei, Sibali Debnath, John L. Weber et al.·May 2, 2024SaveLearn
Benchmarking DFT-based excited-state methods for intermolecular charge-transfer excitationsIntermolecular charge-transfer is a highly important process in biology and energy-conversion applications where generated charges need to be transported over several moieties. However, its…Nicola Bogo, Christopher J. Stein·May 2, 2024SaveLearn
High-frequency tails in spectral densitiesRecent advances in numerically exact quantum dynamics methods have brought the dream of accurately modeling the dynamics of chemically complex open systems within reach. Path-integral-based methods,…Roman Korol, Xinxian Chen, Ignacio Franco·May 2, 2024SaveLearn
High repetition rate ultrafast electron diffraction with direct electron detectionUltrafast electron diffraction (UED) instruments typically operate at kHz or lower repetition rates and rely on indirect detection of electrons. However, these experiments encounter limitations…Fernando Rodriguez Diaz, Mark Mero, Kasra Amini·May 2, 2024SaveLearn
Molecular Insights into the Water Dissociation and Proton Dynamics at the β-TaON (100)/Water InterfaceUnderstanding the dynamic nature of the semiconductor-water interface is crucial for developing efficient photoelectrochemical water splitting catalysts, as it governs reactivity through charge and…Sagarmoy Mandal, Tushar Kanti Ghosh·May 1, 2024SaveLearn
Electronic Coherences in Molecules: The Projected Nuclear Quantum Momentum as a Hidden AgentElectronic coherences are key to understanding and controlling photo-induced molecular transformations. We identify a crucial quantum-mechanical feature of electron-nuclear correlation, the projected…Evaristo Villaseco Arribas, Neepa T. Maitra·May 1, 2024SaveLearn
Quantum rates in dissipative systems with spatially varying frictionWe investigate whether making the friction spatially dependent on the reaction coordinate introduces quantum effects into the thermal reaction rates for dissipative reactions. Quantum rates are…Oliver Bridge, Paolo Lazzaroni, Rocco Martinazzo et al.·May 1, 2024SaveLearn
Canonized then Minimized RMSD for Three-Dimensional StructuresExisting molecular canonization algorithms typically operate on one-dimensional (1D) string representations or two-dimensional (2D) connectivity graphs of a molecule and are not able to differentiate…Jie Li, Qian Chen, Jingwei Weng et al.·May 1, 2024SaveLearn
Beyond a Richardson-Gaudin mean-field: Slater-Condon rules and perturbation theoryRichardson-Gaudin states provide a basis of the Hilbert space for strongly correlated electrons. In this study, optimal expressions for the transition density matrix elements between…Paul A. Johnson·May 1, 2024SaveLearn
Thawed Gaussian wavepacket dynamics with -machine learned potentialsA method for performing variable-width (thawed) Gaussian wavepacket (GWP) variational dynamics on machine-learned potentials is presented. Instead of fitting the potential energy surface (PES), the…Rami Gherib, Ilya G. Ryabinkin, Scott N. Genin·Apr 30, 2024SaveLearn
Exploring the role of mean-field potentials and short-range wave function behavior in the adiabatic connectionIn this article, we explore the construction of Hamiltonians with long-range interactions and their corrections using the short-range behavior of the wave function. A key aspect of our investigation…Anthony Scemama, Andreas Savin·Apr 30, 2024SaveLearn
Unveiling the effects of Cu doping on the H2 activation by CeO2 surface frustrated Lewis pairsRecently, the solid-state frustrated Lewis pairs (FLPs) on the surface of CeO2 have been demonstrated to effectively catalyze the selective hydrogenation of unsaturated substrates, hence, the…Tongtong Liu, Xinyi Wu, Kaisi Liu et al.·Apr 30, 2024SaveLearn
Striking the Right Balance of Encoding Electron Correlation in the Hamiltonian and the Wavefunction AnsatzMulti-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from…Kalman Szenes, Maximilian Moerchen, Paul Fischill et al.·Apr 30, 2024SaveLearn
SCN as a Local Probe of Protein Structural DynamicsThe dynamics of lysozyme is probed by attaching -SCN to all alanine-residues. The 1-dimensional infrared spectra exhibit frequency shifts in the position of the maximum absorption by 4 cm-1…Sena Aydin, Seyedeh Maryam Salehi, Kai Töpfer et al.·Apr 29, 2024SaveLearn
High-Energy Reaction Dynamics of N3The atom-exchange and atomization dissociation dynamics for the N(4S) + N2(1 g+) reaction is studied using a reproducing kernel Hilbert space (RKHS)-based, global potential…JingChun Wang, Juan Carlos San Vicente Veliz, Markus Meuwly·Apr 29, 2024SaveLearn
Understanding Radicals via Orbital ParitiesWe introduce analysis of orbital parities as a concept and a tool for understanding radicals. Based on fundamental reduced one- and two-electron density matrices, our approach allows us to evaluate a…Reza G. Shirazi, Benedikt M. Schoenauer, Peter Schmitteckert et al.·Apr 29, 2024SaveLearn
A general framework for active space embedding methods: applications in quantum computingWe developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of…Stefano Battaglia, Max Rossmannek, Vladimir V. Rybkin et al.·Apr 29, 2024SaveLearn
Efficient Random Phase Approximation for DiradicalsWe apply the analytically solvable model of two electrons in two orbitals to diradical molecules, characterized by two unpaired electrons. The effect of the doubly occupied and empty orbitals is…Reza G. Shirazi, Vladimir V. Rybkin, Michael Marthaler et al.·Apr 29, 2024SaveLearn
Excimer Formation in Zinc-phthalocyanine Revealed using Ultrafast Electron DiffractionThe formation of excited dimer states, so called excimers, is an important phenomenon in many organic molecular semiconductors. In contrast to Frenkel exciton-polaron excited states, an excimer is…Sebastian Hammer, Tristan L. Britt, Laurenz Kremeyer et al.·Apr 28, 2024SaveLearn
Tensor hypercontraction for fully self-consistent imaginary-time GF2 and GWSOX methods: theory, implementation, and role of the Green's function second-order exchange for intermolecular interactionsWe apply tensor hypercontraction (THC) to reduce the computational scaling of expensive fully self-consistent Green's function methods. We present an efficient MPI-parallel algorithm and its…Pavel Pokhilko, Chia-Nan Yeh, Miguel A. Morales et al.·Apr 27, 2024SaveLearn
Vibrational coherences in half-broadband 2D electronic spectroscopy: spectral filtering to identify excited state displacementsVibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat…Dale Green, Giovanni Bressan, Ismael A. Heisler et al.·Apr 26, 2024SaveLearn
Isotope effect in the Morse approximation of the ground state term of hydrogen molecule nH2, n = 1-7. Herzberg anomaly and anharmonicityThe influence of the reduced mass on the results of the approximation by the Morse function of the ground electronic state term potential U(r) of hydrogen molecule nH2 for seven symmetrical…Gleb S. Denisov, Edem R. Chakalov, Peter M. Tolstoy·Apr 26, 2024SaveLearn
Converging TDDFT calculations in 5 iterations with minimal auxiliary preconditioningEigenvalue problems and linear systems of equations involving large symmetric matrices are commonly solved in quantum chemistry using Krylov space methods, such as the Davidson algorithm. The…Zehao Zhou, Shane M. Parker·Apr 26, 2024SaveLearn