Explicit models of motions to understand protein side-chain dynamicsNuclear magnetic relaxation is widely used to probe protein dynamics. For decades, most analyses of relaxation in proteins have relied successfully on the model-free approach, forgoing mechanistic…Nicolas Bolik-Coulon, Olivier Languin-Cattoën, Diego Carnevale et al.·Apr 12, 2022SaveLearn
Sub-percent accuracy for the intensity of a near infrared water line at 10670 cm-1: experiment and analysisLaser measurements of the intensity of (201) 322 -- (000) 221 near-infrared water absorption line at 10670.1 \ are made using three different Herriott cells. These measurements determine…Tom M. Rubin, Marian Sarrazin, Nikolai F. Zobov et al.·Apr 12, 2022SaveLearn
Dimerization of dehydrogenated polycyclic aromatic hydrocarbons on grapheneDimerization of polycyclic aromatic hydrocarbons (PAHs) is an important, yet poorly understood, step in the on-surface synthesis of graphene (nanoribbon), soot formation, and growth of carbonaceous…Zeyuan Tang, Bjørk Hammer·Apr 12, 2022SaveLearn
Janus van der Waals equations for real molecules with two-sided phase transitionsWe obtain families of generalised van der Waals equations characterised by an even number n=2,4,6 and a continuous free parameter which is tunable for a critical compressibility factor. Each…Jihwan Kim, Do-Hyun Kim, Jeong-Hyuck Park·Apr 12, 2022SaveLearn
Multidimensional quantum calculation of the infrared spectra under polaritonic vibrational strong and ultrastrong couplingRecent experiments and theory demonstrate that the the ground state properties and chemical reactivity of molecules can be modified inside an optical cavity. The vibrational strong or ultrastrong…Qi Yu·Apr 12, 2022SaveLearn
Transition-Potential Coupled Cluster II: Optimization of the Core Orbital Occupation NumberThe issue of orbital relaxation in computational core-hole spectroscopy, specifically x-ray absorption, has been a major problem for methods such as equation-of-motion coupled cluster with singles…Megan Simons, Devin A. Matthews·Apr 11, 2022SaveLearn
Systematically Improvable Generalization of Self-Interaction Corrected Density Functional TheoryPerdew-Zunger self-interaction correction (PZSIC) reintroduces an exact constraint to approximate density functional theory (DFT), but can paradoxically degrade performance and is not systematically…Benjamin G. Janesko·Apr 11, 2022SaveLearn
Reference Energies for Cyclobutadiene: Automerization and Excited StatesCyclobutadiene is a well-known playground for theoretical chemists and is particularly suitable to test ground- and excited-state methods. Indeed, due to its high spatial symmetry, especially at the…Enzo Monino, Martial Boggio-Pasqua, Anthony Scemama et al.·Apr 11, 2022SaveLearn
Gliding on ice in search of accurate and cost-effective computational methods for astrochemistry on grains: the puzzling case of the HCN isomerizationThe isomerization of hydrogen cyanide to hydrogen isocyanide on icy grain surfaces is investigated by an accurate composite method (jun-Cheap) rooted in the coupled cluster ansatz and by density…Carmen Baiano, Jacopo Lupi, Vincenzo Barone et al.·Apr 10, 2022SaveLearn
Self-Consistent Equations for Nonempirical Tight Binding TheoryA new reference state for density functional theory, termed the independent atom ansatz, is introduced in this work. This ansatz allows for the exact representation of electron density in terms of…Alexander V. Mironenko·Apr 9, 2022SaveLearn
Spectral signatures of excess-proton waiting and transfer-path dynamics in aqueous hydrochloric acid solutionsSignatures of solvated excess protons in infrared difference absorption spectra, such as the continuum band between the water bend and stretch bands, have been experimentally known for a long time,…Florian N. Brünig, Manuel Rammler, Ellen M. Adams et al.·Apr 9, 2022SaveLearn
Explicit models of motions to analyze NMR relaxation data in proteinsNuclear Magnetic Resonance (NMR) is a tool of choice to characterize molecular motions. In biological macromolecules, pico- to nano-second motions, in particular, can be probed by nuclear spin…Nicolas Bolik-Coulon, Fabien Ferrage·Apr 8, 2022SaveLearn
Improved proton-transfer barriers with van der Waals density functionals: Role of repulsive non-local correlationProton-transfer (PT) between organic complexes is a common and important biochemical process. Unfortunately, PT energy barriers are difficult to accurately predict using density functional theory…S. Seyedraoufi, Kristian Berland·Apr 8, 2022SaveLearn
Exact two-component Hamiltonians for relativistic quantum chemistry: Two-electron picture-change corrections made simpleBased on self-consistent field (SCF) atomic mean-field (amf) quantities, we present two simple, yet computationally efficient and numerically accurate matrix-algebraic approaches to correct both…Stefan Knecht, Michal Repisky, Hans Jørgen Aagaard Jensen et al.·Apr 8, 2022SaveLearn
Optical Signatures of the Coupling between Excitons and Charge Transfer States in Linear Molecular AggregatesCharge Transfer (CT) has enjoyed continuous interest due to increasing experimental control over molecular structure leading to applications in, for example, photovoltaics and hydrogen production. In…Marìck Manrho, Thomas L. C. Jansen, Jasper Knoester·Apr 8, 2022SaveLearn
MP2-F12 basis set convergence near the complete basis set limit: are h functions sufficient?We have investigated the title question for the W4-08 thermochemical benchmark using partial-wave truncations of a large reference (REF) basis set, as well as for standard F12-optimized basis sets.…Nisha Mehta, Jan M. L. Martin·Apr 7, 2022SaveLearn
The coupling of the hydrated proton to its first solvation shellThe transfer of a hydrated proton between water molecules in aqueous solution is accompanied by the large-scale structural reorganization of the environment as the proton relocates, giving rise to…Markus Schröder, Fabien Gatti, David Lauvergnat et al.·Apr 7, 2022SaveLearn
Secondary kinetic peak in the Kohn-Sham potential and its connection to the response stepWe consider a prototypical 1D model Hamiltonian for a stretched heteronuclear molecule and construct individual components of the corresponding KS potential, namely: the kinetic, the N - 1, and the…Sara Giarrusso, Roeland Neugarten, Evert Jan Baerends et al.·Apr 6, 2022SaveLearn
Solid-state heteronuclear multiple-quantum spectroscopy under a magic-angle spinning frequency of 150 kHzWe hereby demonstrate that 1H detected 15N-1H heteronuclear multiple-quantum spectroscopy can be carried out at a magic angle spinning frequency of 150 kHz. While the 15N-1H multiple-quantum…Eric Chung-Yueh Yuan, Po-Wen Chen, Shing-Jong Huang et al.·Apr 6, 2022SaveLearn
δ44/40Ca-δ88/86Sr multi-proxy constrains primary origin of Marinoan cap carbonatesThe Neoproterozoic Earth experienced at least two global-scale glaciations termed Snowball Earth events. 'Cap carbonates' were widely deposited after the events, but controversy surrounds…Jiuyuan Wang, Andrew D. Jacobson, Bradley B. Sageman et al.·Apr 6, 2022SaveLearn
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