Journal ArticleDOI
Absolute Hydration Free Energy of the Proton from First-Principles Electronic Structure Calculations
Chang-Guo Zhan,David A. Dixon +1 more
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In this paper, a first-principles determination of the absolute hydration free energy of the proton ΔGhyd298(H+) by using the latest developments in electronic structure theory including solvation effects is reported.Abstract:
The absolute hydration free energy of the proton, ΔGhyd298(H+), is one of the fundamental quantities for the thermodynamics of aqueous systems. Its exact value remains unknown despite extensive experimental and computational efforts. We report a first-principles determination of ΔGhyd298(H+) by using the latest developments in electronic structure theory including solvation effects. High level ab initio calculations have been performed with a supermolecule-continuum approach based on a recently developed self-consistent reaction field model known as surface and volume polarization for electrostatic interaction (SVPE) or fully polarizable continuum model (FPCM). In the supermolecule-continuum approach, part of the solvent surrounding the solute is treated quantum mechanically and the remaining bulk solvent is approximated by a dielectric continuum medium. With this approach, the calculated results can systematically be improved by increasing the number of quantum mechanically treated solvent molecules. ΔGh...read more
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Aqueous solvation free energies of ions and ion-water clusters based on an accurate value for the absolute aqueous solvation free energy of the proton.
TL;DR: Using the same set of ions that was recently used to develop the SM6 continuum solvation model, SM6 retains its previously determined high accuracy; indeed, in most cases the mean unsigned error improves when it is tested against the more accurate reference data.
Journal ArticleDOI
Calculation of Solvation Free Energies of Charged Solutes Using Mixed Cluster/Continuum Models
TL;DR: A consistent approach is derived for predicting the solvation free energies of charged solutes in the presence of implicit and explicit solvents because of the incorrect accounting of the standard state corrections for water molecules or water clusters present in the thermodynamic cycle.
Journal ArticleDOI
Role of water in electron-initiated processes and radical chemistry: issues and scientific advances.
Bruce C. Garrett,David A. Dixon,Donald M. Camaioni,Daniel M. Chipman,Mark A. Johnson,Charles D. Jonah,Gregory A. Kimmel,John H. Miller,Thomas N. Rescigno,Peter J. Rossky,Sotiris S. Xantheas,Steven D. Colson,Allan H. Laufer,Douglas Ray,Paul F. Barbara,David M. Bartels,Kurt Becker,Kit H. Bowen,Stephen E. Bradforth,Ian Carmichael,James V. Coe,L. René Corrales,James P. Cowin,Michel Dupuis,Kenneth B. Eisenthal,James A. Franz,Maciej Gutowski,Kenneth D. Jordan,Bruce D. Kay,Jay A. LaVerne,Sergei V. Lymar,Theodore E. Madey,C. William McCurdy,Dan Meisel,Shaul Mukamel,Anders Nilsson,Thomas M. Orlando,Nikolay G. Petrik,Simon M. Pimblott,James R. Rustad,Gregory K. Schenter,Sherwin J. Singer,Andrei Tokmakoff,Lai-Sheng Wang,Curt Wettig,Timothy S. Zwier +45 more
TL;DR: Chemical Science Division, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352; Department of Chemistry, ShelbyHall, University of Alabama, Box 870336, Tuscaloosa, Alabama 35487-0336; Notre Dame Radiation Laboratory, Universityof Notre Dame,Notre Dame, Indiana 46556.
Journal ArticleDOI
Rational Design of Particle Mesh Ewald Compatible Lennard-Jones Parameters for +2 Metal Cations in Explicit Solvent.
TL;DR: This work systematically designed LJ parameters for 24 +2 metal (M(II) cations to reproduce different experimental properties appropriate for the Lorentz-Berthelot combining rules and PME simulations to represent the best possible compromise that can be achieved using the nonbonded model for the ions in combination with simple water models.
Journal ArticleDOI
Ion Solvation Thermodynamics from Simulation with a Polarizable Force Field
TL;DR: The results indicate that calculations with a polarizable force field can capture the thermodynamics of ion solvation and that the solvation free energies of the individual ions differ by several kilocalories from commonly cited values.
References
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Journal ArticleDOI
Density‐functional thermochemistry. III. The role of exact exchange
TL;DR: In this article, a semi-empirical exchange correlation functional with local spin density, gradient, and exact exchange terms was proposed. But this functional performed significantly better than previous functionals with gradient corrections only, and fits experimental atomization energies with an impressively small average absolute deviation of 2.4 kcal/mol.
Journal ArticleDOI
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
TL;DR: Numerical calculations on a number of atoms, positive ions, and molecules, of both open- and closed-shell type, show that density-functional formulas for the correlation energy and correlation potential give correlation energies within a few percent.
Journal ArticleDOI
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen
TL;DR: In this paper, a detailed study of correlation effects in the oxygen atom was conducted, and it was shown that primitive basis sets of primitive Gaussian functions effectively and efficiently describe correlation effects.
Journal ArticleDOI
General atomic and molecular electronic structure system
Michael W. Schmidt,Kim K. Baldridge,Jerry A. Boatz,Steven T. Elbert,Mark S. Gordon,Jan H. Jensen,Shiro Koseki,Nikita Matsunaga,Kiet A. Nguyen,Shujun Su,Theresa L. Windus,Michel Dupuis,John A. Montgomery +12 more
TL;DR: A description of the ab initio quantum chemistry package GAMESS, which can be treated with wave functions ranging from the simplest closed‐shell case up to a general MCSCF case, permitting calculations at the necessary level of sophistication.
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Electron affinities of the first-row atoms revisited. Systematic basis sets and wave functions
TL;DR: In this paper, a reliable procedure for calculating the electron affinity of an atom and present results for hydrogen, boron, carbon, oxygen, and fluorine (hydrogen is included for completeness).