Comparing correlation components and approximations in Hartree-Fock and Kohn-Sham theories via an analytical test case studyThe asymmetric Hubbard dimer is a model that allows for explicit expressions of the Hartree-Fock (HF) and Kohn-Sham (KS) states as analytical functions of the external potential, Δv, and of the…Sara Giarrusso, Aurora Pribram-Jones·Apr 25, 2022SaveLearn
Fourier-transform spectroscopy of 13C17O and deperturbation analysis of the A1Π (ν = 0 - 3) levelsThe high-resolution B1Σ+ - A1Π (0, 0) and (0, 3) emission bands of the less-abundant 13C17O isotopologue have been investigated by Fourier-transform spectroscopy in the visible…R. Hakalla, M. L. Niu, R. W. Field et al.·Apr 25, 2022SaveLearn
Catalysis for e-Chemistry: Need and Gaps for a Future De-Fossilized Chemical Production, with Focus on the Role of Complex (Direct) Syntheses by ElectrocatalysisThe prospects, needs and limits in current approaches in catalysis to accelerate the transition to e-chemistry, where this term indicates a fossil fuel-free chemical production, are discussed. It is…Georgia Papanikolaou, Gabriele Centi, Siglinda Perathoner et al.·Apr 24, 2022SaveLearn
Coherent Atomic Orbital Polarization Probes the Geometric Phase in Photodissociation of Polyatomic MoleculesQuantum interference between multiple pathways in molecular photodissociation often results in angular momentum polarization of atomic products and this can give deep insight into fundamental…Chaya Weeraratna, Arthur G. Suits, Oleg S. Vasyutinskii·Apr 23, 2022SaveLearn
Hole-initiated melting process of thin filmsWe perform numerical and experimental studies on the melting process of thin films initiated by a small hole. The presence of a non-trivial capillary surface, namely the liquid/air interface, leads…Chenyu Jin, Hans Riegler·Apr 22, 2022SaveLearn
Density Functionals based on the mathematical structure of the strong-interaction limit of DFTWhile in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering…Stefan Vuckovic, Augusto Gerolin, Timothy J. Daas et al.·Apr 22, 2022SaveLearn
Particle formation in oxymethylene ethers (OMEn, n = 2-4) / ethylene premixed flamesAlternative synthetic fuels can be produced by renewable energy sources and represent a potential route for solving long-term energy storage. Among them, oxygenated fuels have the advantage of…Robert Schmitz, Federica Ferraro, Mariano Sirignano et al.·Apr 22, 2022SaveLearn
Confinement-controlled Water Engenders High Energy Density Electrochemical-double-layer CapacitanceThe renewable energy sector critically needs low-cost and environmentally neutral energy storage solutions throughout the entire device life cycle. However, the limited performance of standard…Svetlana Melnik, Alexander Ryzhov, Alexei Kiselev et al.·Apr 21, 2022SaveLearn
General Time-Dependent Configuration-Interaction Singles I: The Molecular CaseWe present a grid-based implementation of the time-dependent configuration-interaction singles method suitable for computing the strong-field ionization of small gas-phase molecules. After outlining…Stefanos Carlström, Michael Spanner, Serguei Patchkovskii·Apr 21, 2022SaveLearn
Two-particle coalescence conditions revisitedThe notion of the n-th order local energy, generated by the n-th power of the Hamiltonian, has been introduced. The n-th order two-particle coalescence conditions have been derived from the…Jacek Karwowski, Andreas Savin·Apr 21, 2022SaveLearn
Density Functional Theory for Electronic Excited StatesThis chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly…John M. Herbert·Apr 21, 2022SaveLearn
Accurate Molecular-Orbital-Based Machine Learning Energies via Unsupervised Clustering of Chemical SpaceWe introduce an unsupervised clustering algorithm to improve training efficiency and accuracy in predicting energies using molecular-orbital-based machine learning (MOB-ML). This work determines…Lixue Cheng, Jiace Sun, Thomas F. Miller·Apr 21, 2022SaveLearn
The conceptual and mathematical foundations of the MC-QTAIMThe concept of atoms in molecules (AIM) is one of the cornerstones of the structural theory of chemistry however, in contrast to the free atoms a comprehensive quantum mechanical theory of AIM has…Shant Shahbazian·Apr 20, 2022SaveLearn
Challenges for variational reduced-density-matrix theory: Total angular momentum constraintsThe variational two-electron reduced density matrix (v2RDM) method is generalized for the description of total angular momentum (J) and projection of total angular momentum (MJ) states in…Run R. Li, Nicholas C. Rubin, A. Eugene DePrince·Apr 18, 2022SaveLearn
The generality of uncooperative and cooperative effects in elementary hydrogen-bonded systemsThe cooperative effect plays a significant role in understanding the intermolecular donor-acceptor interactions of hydrogen bonds (H-bonds, D-H...A). Herein, using the benchmark method of…Rui Liu, Rui Wang, Danhui Li et al.·Apr 16, 2022SaveLearn
Homonuclear J-Coupling Spectroscopy using J-Synchronized Echo DetectionIn the strong coupling regime with J-coupling much larger than chemical shift differences, J-coupling spectroscopy enables spectral identification of molecules even when conventional NMR fails. While…Stephen J. DeVience, Matthew S. Rosen·Apr 16, 2022SaveLearn
Ultra-fast Spectroscopy for High-Throughput and Interactive Quantum ChemistryWe present ultra-fast quantum chemical methods for the calculation of infrared and ultraviolet-visible spectra designed to provide fingerprint information during autonomous and interactive…Francesco Bosia, Thomas Weymuth, Markus Reiher·Apr 15, 2022SaveLearn
Automatic generation of complementary auxiliary basis sets (CABS) for explicitly correlated methodsExplicitly correlated calculations, aside from the orbital basis set, typically require three auxiliary basis sets: JK (Coulomb-exchange fitting), RI-MP2 (resolution of the identity MP2), and CABS…Emmanouil Semidalas, Jan M. L. Martin·Apr 14, 2022SaveLearn
Assessment of the second-order statically screened exchange correction to the random phase approximation for correlation energiesWith increasing inter-electronic distance, the screening of the electron-electron interaction by the presence of other electrons becomes the dominant source of electron correlation. This effect is…Arno Förster·Apr 14, 2022SaveLearn
Benchmarking an improved statistical adiabatic channel model for competing inelastic and reactive processesInelastic collisions and elementary chemical reactions proceeding through the formation and subsequent decay of an intermediate collision complex, with an associated deep well on the potential energy…Maarten Konings, Benjamin Desrousseaux, François Lique et al.·Apr 14, 2022SaveLearn
Computational Vibrational SpectroscopyVibrational spectroscopy is a powerful technique to characterize the near-equilibrium dynamics of molecules in the gas- and the condensed-phase. This contribution summarizes efforts from…Markus Meuwly·Apr 14, 2022SaveLearn
Hard X-ray helical dichroism of disordered molecular mediaChirality is a structural property of molecules lacking mirror symmetry that has strong implications in diverse fields, ranging from life to materials sciences. Established spectroscopic methods that…Jeremy R. Rouxel, Benedikt Rosner, Dmitry Karpov et al.·Apr 14, 2022SaveLearn
Benchmarking CASPT3 Vertical Excitation EnergiesBased on 280 reference vertical transition energies of various natures (singlet, triplet, valence, Rydberg, nπ*, ππ*, and double excitations) extracted from the QUEST database, we assess…Martial Boggio-Pasqua, Denis Jacquemin, Pierre-François Loos·Apr 13, 2022SaveLearn
A methane line list with sub-MHz accuracy in the 1250 to 1380 cm-1 range from optical frequency comb Fourier transform spectroscopyWe use a Fourier transform spectrometer based on a difference frequency generation optical frequency comb to measure high-resolution, low-pressure, room-temperature spectra of methane in the 1250 -…Matthias Germann, Adrian Hjältén, Vincent Boudon et al.·Apr 13, 2022SaveLearn
LED-based photo-CIDNP hyperpolarization enables 19F MR imaging and 19F NMR spectroscopy of 3-fluoro-DL-tyrosine at 0.6 TAlthough 19F has high potential to serve as a background-free molecular marker in bioimaging, the molar amount of marker substance is often too small to enable 19F MR imaging or 19F NMR spectroscopy…Johannes Bernarding, Christian Bruns, Isabell Prediger et al.·Apr 13, 2022SaveLearn