Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Sundararaman, Ravishankar; Schwarz, Kathleen A.; Letchworth-Weaver, Kendra; Arias, T. A.

doi:10.1063/1.4906828

Title: Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Journal Article · Sat Feb 07 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4906828· OSTI ID:22416063

Sundararaman, Ravishankar; Schwarz, Kathleen A.; Letchworth-Weaver, Kendra; Arias, T. A. ^[1]

Department of Physics, Cornell University, Ithaca, New York 14853 (United States)

Continuum solvation models enable electronic structure calculations of systems in liquid environments, but because of the large number of empirical parameters, they are limited to the class of systems in their fit set (typically organic molecules). Here, we derive a solvation model with no empirical parameters for the dielectric response by taking the linear response limit of a classical density functional for molecular liquids. This model directly incorporates the nonlocal dielectric response of the liquid using an angular momentum expansion, and with a single fit parameter for dispersion contributions it predicts solvation energies of neutral molecules with a RMS error of 1.3 kcal/mol in water and 0.8 kcal/mol in chloroform and carbon tetrachloride. We show that this model is more accurate for strongly polar and charged systems than previous solvation models because of the parameter-free electric response, and demonstrate its suitability for ab initio solvation, including self-consistent solvation in quantum Monte Carlo calculations.

Cite

Export

Save

OSTI ID:: 22416063

Journal Information:: Journal of Chemical Physics, Vol. 142, Issue 5; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606

Country of Publication:: United States

Language:: English

References (41)

Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
The implementation of density functional theory within the polarizable continuum model for solvation Fortunelli, Alessandro; Tomasi, Jacopo Chemical Physics Letters, Vol. 231, Issue 1 https://doi.org/10.1016/0009-2614(94)01253-9	journal	December 1994
The radial distribution functions of water and ice from 220 to 673 K and at pressures up to 400 MPa Soper, A. K. Chemical Physics, Vol. 258, Issue 2-3 https://doi.org/10.1016/s0301-0104(00)00179-8	journal	August 2000
Quantum Mechanical Continuum Solvation Models Tomasi, Jacopo; Mennucci, Benedetta; Cammi, Roberto Chemical Reviews, Vol. 105, Issue 8 https://doi.org/10.1021/cr9904009	journal	August 2005
Field-Extremum Model for Short-Range Contributions to Hydration Free Energy Pomogaeva, Anna; Chipman, Daniel M. Journal of Chemical Theory and Computation, Vol. 7, Issue 12 https://doi.org/10.1021/ct200575c	journal	October 2011
Self-Consistent Reaction Field Model for Aqueous and Nonaqueous Solutions Based on Accurate Polarized Partial Charges Marenich, Aleksandr V.; Olson, Ryan M.; Kelly, Casey P. Journal of Chemical Theory and Computation, Vol. 3, Issue 6 https://doi.org/10.1021/ct7001418	journal	October 2007
General parameterized SCF model for free energies of solvation in aqueous solution Cramer, Christopher J.; Truhlar, Donald G. Journal of the American Chemical Society, Vol. 113, Issue 22 https://doi.org/10.1021/ja00022a017	journal	October 1991
Accurate First Principles Calculation of Molecular Charge Distributions and Solvation Energies from Ab Initio Quantum Mechanics and Continuum Dielectric Theory Tannor, David J.; Marten, Bryan; Murphy, Robert Journal of the American Chemical Society, Vol. 116, Issue 26 https://doi.org/10.1021/ja00105a030	journal	December 1994
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 Kelly, Casey P.; Cramer, Christopher J.; Truhlar, Donald G. The Journal of Physical Chemistry B, Vol. 110, Issue 32 https://doi.org/10.1021/jp063552y	journal	August 2006
Universal Solvation Model Based on Solute Electron Density and on a Continuum Model of the Solvent Defined by the Bulk Dielectric Constant and Atomic Surface Tensions Marenich, Aleksandr V.; Cramer, Christopher J.; Truhlar, Donald G. The Journal of Physical Chemistry B, Vol. 113, Issue 18, p. 6378-6396 https://doi.org/10.1021/jp810292n	journal	May 2009
Consistent van der Waals Radii for the Whole Main Group Mantina, Manjeera; Chamberlin, Adam C.; Valero, Rosendo The Journal of Physical Chemistry A, Vol. 113, Issue 19 https://doi.org/10.1021/jp8111556	journal	May 2009
New Model for Calculation of Solvation Free Energies: Correction of Self-Consistent Reaction Field Continuum Dielectric Theory for Short-Range Hydrogen-Bonding Effects Marten, Bryan; Kim, Kyungsun; Cortis, Christian The Journal of Physical Chemistry, Vol. 100, Issue 28 https://doi.org/10.1021/jp953087x	journal	January 1996
Self-Consistent-Field Calculation of Pauli Repulsion and Dispersion Contributions to the Solvation Free Energy in the Polarizable Continuum Model Amovilli, Claudio; Mennucci, Benedetta The Journal of Physical Chemistry B, Vol. 101, Issue 6 https://doi.org/10.1021/jp9621991	journal	February 1997
Evaluation of Solvent Effects in Isotropic and Anisotropic Dielectrics and in Ionic Solutions with a Unified Integral Equation Method: Theoretical Bases, Computational Implementation, and Numerical Applications Mennucci, B.; Cancès, E.; Tomasi, J. The Journal of Physical Chemistry B, Vol. 101, Issue 49 https://doi.org/10.1021/jp971959k	journal	December 1997
Towards an assessment of the accuracy of density functional theory for first principles simulations of water Grossman, Jeffrey C.; Schwegler, Eric; Draeger, Erik W. The Journal of Chemical Physics, Vol. 120, Issue 1 https://doi.org/10.1063/1.1630560	journal	January 2004
Norm-conserving Hartree–Fock pseudopotentials and their asymptotic behavior Trail, J. R.; Needs, R. J. The Journal of Chemical Physics, Vol. 122, Issue 1 https://doi.org/10.1063/1.1829049	journal	January 2005
Smooth relativistic Hartree–Fock pseudopotentials for H to Ba and Lu to Hg Trail, J. R.; Needs, R. J. The Journal of Chemical Physics, Vol. 122, Issue 17 https://doi.org/10.1063/1.1888569	journal	May 2005
Continuous surface charge polarizable continuum models of solvation. I. General formalism Scalmani, Giovanni; Frisch, Michael J. The Journal of Chemical Physics, Vol. 132, Issue 11 https://doi.org/10.1063/1.3359469	journal	March 2010
Revised self-consistent continuum solvation in electronic-structure calculations Andreussi, Oliviero; Dabo, Ismaila; Marzari, Nicola The Journal of Chemical Physics, Vol. 136, Issue 6 https://doi.org/10.1063/1.3676407	journal	February 2012
A new definition of cavities for the computation of solvation free energies by the polarizable continuum model Barone, Vincenzo; Cossi, Maurizio; Tomasi, Jacopo The Journal of Chemical Physics, Vol. 107, Issue 8 https://doi.org/10.1063/1.474671	journal	August 1997
Self-consistent continuum solvation (SCCS): The case of charged systems Dupont, C.; Andreussi, O.; Marzari, N. The Journal of Chemical Physics, Vol. 139, Issue 21 https://doi.org/10.1063/1.4832475	journal	December 2013
A recipe for free-energy functionals of polarizable molecular fluids Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Arias, T. A. The Journal of Chemical Physics, Vol. 140, Issue 14 https://doi.org/10.1063/1.4870653	journal	April 2014
Weighted-density functionals for cavity formation and dispersion energies in continuum solvation models Sundararaman, Ravishankar; Gunceler, Deniz; Arias, T. A. The Journal of Chemical Physics, Vol. 141, Issue 13 https://doi.org/10.1063/1.4896827	journal	October 2014
Continuum variational and diffusion quantum Monte Carlo calculations Needs, R. J.; Towler, M. D.; Drummond, N. D. Journal of Physics: Condensed Matter, Vol. 22, Issue 2 https://doi.org/10.1088/0953-8984/22/2/023201	journal	December 2009
The importance of nonlinear fluid response in joint density-functional theory studies of battery systems Gunceler, Deniz; Letchworth-Weaver, Kendra; Sundararaman, Ravishankar Modelling and Simulation in Materials Science and Engineering, Vol. 21, Issue 7 https://doi.org/10.1088/0965-0393/21/7/074005	journal	October 2013
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/physrev.140.a1133	journal	November 1965
Inhomogeneous Electron Gas Rajagopal, A. K.; Callaway, J. Physical Review B, Vol. 7, Issue 5 https://doi.org/10.1103/physrevb.7.1912	journal	March 1973
Joint density-functional theory for electronic structure of solvated systems Petrosyan, S. A.; Briere, Jean-Francois; Roundy, David Physical Review B, Vol. 75, Issue 20 https://doi.org/10.1103/physrevb.75.205105	journal	May 2007
Framework for solvation in quantum Monte Carlo Schwarz, Kathleen A.; Sundararaman, Ravishankar; Letchworth-Weaver, Kendra Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/physrevb.85.201102	journal	May 2012
Joint density functional theory of the electrode-electrolyte interface: Application to fixed electrode potentials, interfacial capacitances, and potentials of zero charge Letchworth-Weaver, Kendra; Arias, T. A. Physical Review B, Vol. 86, Issue 7 https://doi.org/10.1103/physrevb.86.075140	journal	August 2012
Nuclear Quantum Effects in Water Morrone, Joseph A.; Car, Roberto Physical Review Letters, Vol. 101, Issue 1 https://doi.org/10.1103/physrevlett.101.017801	journal	July 2008
Workhorse Semilocal Density Functional for Condensed Matter Physics and Quantum Chemistry Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 103, Issue 2 https://doi.org/10.1103/physrevlett.103.026403	journal	July 2009
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/physrevlett.77.3865	journal	October 1996
Van der Waals Density Functional for General Geometries Dion, M.; Rydberg, H.; Schröder, E. Physical Review Letters, Vol. 92, Issue 24 https://doi.org/10.1103/physrevlett.92.246401	journal	June 2004
Quantum Mechanical Continuum Solvation Models Tomasi, Jacopo; Menucci, Benedetta; Cammi, Roberto ChemInform, Vol. 36, Issue 42 https://doi.org/10.1002/chin.200542292	journal	October 2005
Nuclear quantum effects in water Morrone, Joseph A.; Car, Roberto arXiv https://doi.org/10.48550/arxiv.0803.3635	text	January 2008
Workhorse Semilocal Density Functional for Condensed Matter Physics and Quantum Chemistry Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gabor I. arXiv https://doi.org/10.48550/arxiv.0906.5029	preprint	January 2009
Framework for solvation in quantum Monte Carlo Schwarz, Kathleen A.; Sundararaman, Ravishankar; Letchworth-Weaver, Kendra arXiv https://doi.org/10.48550/arxiv.1204.6330	text	January 2012
The importance of nonlinear fluid response in joint density-functional theory studies of battery systems Gunceler, Deniz; Letchworth-Weaver, Kendra; Sundararaman, Ravishankar arXiv https://doi.org/10.48550/arxiv.1301.6189	text	January 2013
A recipe for free-energy functionals of polarizable molecular fluids Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Arias, T. A. arXiv https://doi.org/10.48550/arxiv.1402.3237	text	January 2014
Weighted-density functionals for cavity formation and dispersion energies in continuum solvation models Sundararaman, Ravishankar; Gunceler, Deniz; Arias, T. A. arXiv https://doi.org/10.48550/arxiv.1407.4011	text	January 2014

Cited By (17)

Simulation of Many-Electron Systems That Exchange Matter with the Environment: Simulation of Many-Electron Systems That Exchange Matter with the Environment Delle Site, Luigi Advanced Theory and Simulations, Vol. 1, Issue 10 https://doi.org/10.1002/adts.201800056	journal	August 2018
Computational Insights into Materials and Interfaces for Capacitive Energy Storage Zhan, Cheng; Lian, Cheng; Zhang, Yu Advanced Science, Vol. 4, Issue 7 https://doi.org/10.1002/advs.201700059	journal	April 2017
Development of reaction–diffusion DFT and its application to catalytic oxidation of NO in porous materials Liu, Yu; Liu, Honglai AIChE Journal, Vol. 66, Issue 2 https://doi.org/10.1002/aic.16824	journal	November 2019
Computational Approaches to Photoelectrode Design through Molecular Functionalization for Enhanced Photoelectrochemical Water Splitting Iyer, Ashwathi; Kearney, Kara; Ertekin, Elif ChemSusChem, Vol. 12, Issue 9 https://doi.org/10.1002/cssc.201802514	journal	November 2018
Continuum embeddings in condensed-matter simulations Andreussi, Oliviero; Fisicaro, Giuseppe International Journal of Quantum Chemistry, Vol. 119, Issue 1 https://doi.org/10.1002/qua.25725	journal	October 2018
Modelling heterogeneous interfaces for solar water splitting Pham, Tuan Anh; Ping, Yuan; Galli, Giulia Nature Materials, Vol. 16, Issue 4 https://doi.org/10.1038/nmat4803	journal	January 2017
Computational optimization of electric fields for better catalysis design Welborn, Valerie Vaissier; Ruiz Pestana, Luis; Head-Gordon, Teresa Nature Catalysis, Vol. 1, Issue 9 https://doi.org/10.1038/s41929-018-0109-2	journal	September 2018
Formic acid oxidation on platinum: a simple mechanistic study Schwarz, Kathleen A.; Sundararaman, Ravishankar; Moffat, Thomas P. Physical Chemistry Chemical Physics, Vol. 17, Issue 32 https://doi.org/10.1039/c5cp03045e	journal	January 2015
The charge-asymmetric nonlocally determined local-electric (CANDLE) solvation model Sundararaman, Ravishankar; Goddard, William A. The Journal of Chemical Physics, Vol. 142, Issue 6 https://doi.org/10.1063/1.4907731	journal	February 2015
First-principles electrostatic potentials for reliable alignment at interfaces and defects Sundararaman, Ravishankar; Ping, Yuan The Journal of Chemical Physics, Vol. 146, Issue 10 https://doi.org/10.1063/1.4978238	journal	March 2017
Grand canonical electronic density-functional theory: Algorithms and applications to electrochemistry Sundararaman, Ravishankar; Goddard, William A.; Arias, Tomas A. The Journal of Chemical Physics, Vol. 146, Issue 11 https://doi.org/10.1063/1.4978411	journal	March 2017
Substrate effects on charged defects in two-dimensional materials Wang, Dan; Sundararaman, Ravishankar Physical Review Materials, Vol. 3, Issue 8 https://doi.org/10.1103/physrevmaterials.3.083803	journal	August 2019
First-principles identification of localized trap states in polymer nanocomposite interfaces Shandilya, Abhishek; Schadler, Linda S.; Sundararaman, Ravishankar Journal of Materials Research, Vol. 35, Issue 8 https://doi.org/10.1557/jmr.2020.18	journal	February 2020
First-principles electrostatic potentials for reliable alignment at interfaces and defects Sundararaman, Ravishankar; Ping, Yuan arXiv https://doi.org/10.48550/arxiv.1612.01671	text	January 2016
Grand canonical electronic density-functional theory: algorithms and applications to electrochemistry Sundararaman, Ravishankar; Goddard, William A.; Arias, Tomas A. arXiv https://doi.org/10.48550/arxiv.1701.04490	text	January 2017
Solvent-Aware Interfaces in Continuum Solvation Andreussi, Oliviero; Hörmann, Nicolas Georg; Nattino, Francesco Journal of Chemical Theory and Computation, Vol. 15, Issue 3 https://doi.org/10.1021/acs.jctc.8b01174	journal	January 2019
The charge-asymmetric nonlocally-determined local-electric (CANDLE) solvation model Sundararaman, Ravishankar; Goddard, William A. arXiv https://doi.org/10.48550/arxiv.1410.2922	text	January 2014

Similar Records

Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Journal Article · Tue Feb 03 00:00:00 EST 2015 · Journal of Chemical Physics · OSTI ID:22416063

Sundararaman, Ravishankar; Schwarz, Kathleen A.; Letchworth-Weaver, Kendra; +1 more

Weighted-density functionals for cavity formation and dispersion energies in continuum solvation models

Journal Article · Fri Oct 03 00:00:00 EDT 2014 · Journal of Chemical Physics · OSTI ID:22416063

Sundararaman, Ravishankar; Gunceler, Deniz; Arias, T. A.

Weighted-density functionals for cavity formation and dispersion energies in continuum solvation models

Journal Article · Tue Oct 07 00:00:00 EDT 2014 · Journal of Chemical Physics · OSTI ID:22416063

Sundararaman, Ravishankar; Gunceler, Deniz; Arias, T. A.

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ANGULAR MOMENTUM
CARBON TETRACHLORIDE
CHLOROFORM
DENSITY FUNCTIONAL METHOD
DIELECTRIC MATERIALS
ELECTRONIC STRUCTURE
EXPANSION
LIQUIDS
MOLECULES
MONTE CARLO METHOD
SOLVATION
SPHERICAL CONFIGURATION
WATER

Title: Spicing up continuum solvation models with SaLSA: The spherically averaged liquid susceptibility ansatz

Citation Formats

References (41)

Cited By (17)

Similar Records

Related Subjects