Large-Z atoms in the strong-interaction limit of DFT: Implications for gradient expansions and for the Lieb-Oxford boundWe study numerically the strong-interaction limit of the exchange-correlation functional for neutral atoms and for Bohr atoms as the number of electrons increases. Using a compact representation, we…Kimberly J. Daas, Derk P. Kooi, Tarik Benyahia et al.·Nov 14, 2022SaveLearn
Quadripartite bond length rule applied to two prototypical aromatic and antiaromatic moleculesIn 2000, a remarkably simple relationship was introduced, which connected the calculated geometries of isomolecular states of three different multiplicities. These encompass a ground singlet state,…Lukasz Wolanski, Wojciech Grochala·Nov 14, 2022SaveLearn
Berry Population Analysis: Atomic Charges from the Berry Curvature in a Magnetic FieldThe Berry curvature is essential in Born-Oppenheimer molecular dynamics, describing the screening of the nuclei by the electrons in a magnetic field. Parts of the Berry curvature can be understood…Laurens D. M. Peters, Tanner Culpitt, Erik I. Tellgren et al.·Nov 14, 2022SaveLearn
Using Machine Learning Hamiltonians To Compute Molecular Motor Barrier HeightsMachine Learning Inter-atomic Potentials (MLIPs) have become a common tool in use by computational chemists due to their combination of accuracy and speed. Yet, it is still not clear how well these…Aaron Philip, Guoqing Zhou, Benjamin Nebgen·Nov 14, 2022SaveLearn
Photoionization and core resonances from range-separated time-dependent density-functional theory for open-shell states: Example of the lithium atomWe consider the calculations of photoionization spectra and core resonances of open-shell systems using range-separated time-dependent density-functional theory. Specifically, we use the…Julien Toulouse, Karno Schwinn, Felipe Zapata et al.·Nov 14, 2022SaveLearn
Machine Learning Diffusion Monte Carlo ForcesDiffusion Monte Carlo (DMC) is one of the most accurate techniques available for calculating the electronic properties of molecules and materials, yet it often remains a challenge to economically…Cancan Huang, Brenda M. Rubenstein·Nov 14, 2022SaveLearn
Applications of the Spectral Theory of Chemical Bonding to Simple HydrocarbonsThe finite-basis, pair formulation of the Spectral Theory of chemical bonding is briefly surveyed. Solutions of the Born-Oppenheimer polyatomic Hamiltonian totally antisymmetric in electron exchange…Jeffrey D. Mills·Nov 13, 2022SaveLearn
Self-diffusion and shear viscosity for the TIP4P/Ice water modelWith an ever-increasing interest in water properties, many intermolecular force fields have been proposed to describe the behavior of water. Unfortunately, good models for liquid water usually cannot…Łukasz Baran, Wojciech Rżysko, Luis G. MacDowell·Nov 12, 2022SaveLearn
Adaptive Basis Sets for Practical Quantum ComputingElectronic structure calculations on small systems such as H2, H2O, LiH, and BeH2 with chemical accuracy are still a challenge for the current generation of the noisy intermediate-scale…Hyuk-Yong Kwon, Gregory M. Curtin, Zachary Morrow et al.·Nov 11, 2022SaveLearn
Understanding and eliminating spurious modes in variational Monte Carlo using collective variablesThe use of neural network parametrizations to represent the ground state in variational Monte Carlo (VMC) calculations has generated intense interest in recent years. However, as we demonstrate in…Huan Zhang, Robert J. Webber, Michael Lindsey et al.·Nov 11, 2022SaveLearn
Simulating Spin-Orbit Coupling With Quasidegenerate N-Electron Valence Perturbation TheoryWe present the first implementation of spin-orbit coupling effects in fully internally contracted second-order quasidegenerate N-electron valence perturbation theory (SO-QDNEVPT2). The SO-QDNEVPT2…Rajat Majumder, Alexander Yu. Sokolov·Nov 11, 2022SaveLearn
Potential curves illustrating a dissipative self-assembly system and the meaning of away-from-equilibriumDissipative self-assembly is a recently proposed concept in the field of non-equilibrium systems. This concept catches the reader's attention owing to its relationship with life phenomena. Recently,…Yoshiyuki Kageyama, Goro Maruta·Nov 11, 2022SaveLearn
Vibropolaritonic Reaction Rates in the Collective Strong Coupling Regime: Pollak-Grabert-H\"anggi TheoryFollowing experimental evidence that vibrational polaritons, formed from collective vibrational strong coupling (VSC) in optical microcavities, can modify ground-state reaction rates, a spate of…Matthew Du, Yong Rui Poh, Joel Yuen-Zhou·Nov 10, 2022SaveLearn
Towards chemical accuracy using the Jastrow correlated antisymmetrized geminal power ansatzHerein, we report accurate atomization energy calculations for 55 molecules in the Gaussian-2 (G2) set using lattice regularized diffusion Monte Carlo (LRDMC). We compare the Jastrow-Slater…Abhishek Raghav, Ryo Maezono, Kenta Hongo et al.·Nov 10, 2022SaveLearn
Proton transfer at subkelvin temperaturesWe demonstrate a novel method to ionize molecules or molecular clusters by proton transfer at temperatures below 1 K. The method yields nascent ions and largely eliminates secondary reactions, even…Lukas Tiefenthaler, Siegfried Kollotzek, Andrew M. Ellis et al.·Nov 10, 2022SaveLearn
Uncertainties in the Transport Properties of Helium Gas at Cryogenic Temperatures Determined Using Molecular Dynamics SimulationIn this study, the transport properties, such as diffusivity, viscosity, and thermal conductivity, of 4He at the gaseous phase are computed for state points in the temperature range of 10 K to 150 K…Kaanapuli Ramkumar, Swati Swagatika Mishra, Sudeep Bhattacharjee·Nov 9, 2022SaveLearn
Robust inversion of time-resolved data via forward-optimisation in a trajectory basisAn inversion method for time-resolved data from ultrafast experiments is introduced, based on forward-optimisation in a trajectory basis. The method is applied to experimental data from x-ray…Kyle Acheson, Adam Kirrander·Nov 9, 2022SaveLearn
Experimental Characterization of the Energetics of Low-temperature Surface ReactionsAstrochemical surface reactions are thought to be responsible for the formation of complex organic molecules, which are of potential importance for the origin of life. In a situation, when the…Thomas K. Henning, Serge A. Krasnokutski·Nov 8, 2022SaveLearn
Electron Diffraction of Water in No Man's LandA generally accepted understanding of the anomalous properties of water will only emerge if it becomes possible to systematically characterize water in the deeply supercooled regime, from where the…Constantin R. Krüger, Nathan J. Mowry, Gabriele Bongiovanni et al.·Nov 8, 2022SaveLearn
Crumbling Crystals: On the Dissolution Mechanism of NaCl in WaterLife on Earth depends upon the dissolution of ionic salts in water, particularly NaCl. However, an atomistic scale understanding of the process remains elusive. Simulations lend themselves…Niamh O'Neill, Christoph Schran, Stephen J. Cox et al.·Nov 8, 2022SaveLearn
Ground- and Excited-State Dipole Moments and Oscillator Strengths of Full Configuration Interaction QualityWe report ground- and excited-state dipole moments and oscillator strengths (computed in different ``gauges'' or representations) of full configuration interaction (FCI) quality using the selected…Yann Damour, Raúl Quintero-Monsebaiz, Michel Caffarel et al.·Nov 8, 2022SaveLearn
Spin-state Gaps and Self-Interaction-Corrected Density Functional Approximations: Octahedral Fe(II) Complexes as Case StudyAccurate prediction of spin-state energy difference is crucial for understanding the spin crossover (SCO) phenomena and is very challenging for the density functional approximations, especially for…Selim Romero, Tunna Baruah, Rajendra R. Zope·Nov 8, 2022SaveLearn
Self-consistent implementation of locally scaled self-interaction-correction methodRecently proposed local self-interaction correction (LSIC) method [Zope, R. R. et al., J. Chem. Phys. 151, 214108 (2019)] is a one-electron self-interaction-correction (SIC) method that uses an…Yoh Yamamoto, Tunna Baruah, Po-Hao Chang et al.·Nov 8, 2022SaveLearn
Multi-site Reaction Dynamics Through Multi-fragment Density Matrix EmbeddingThe practical description of disordered chemical reactions, where reactions involve multiple species at multiple sites, is presently challenge using correlated electronic structure methods. Here we…Chenghan Li, Junjie Yang, Xing Zhang et al.·Nov 7, 2022SaveLearn
Non-adiabatic Ring Polymer Molecular Dynamics in the Phase Space of the SU(N) Lie GroupWe derive the non-adiabatic ring polymer molecular dynamics (RPMD) approach in the phase space of the SU(N) Lie Group. This method, which we refer to as the spin mapping non-adiabatic RPMD…Duncan Bossion, Sutirtha N. Chowdhury, Pengfei Huo·Nov 7, 2022SaveLearn