Solvent Induced Proton Polarization within the Nuclear–Electronic Orbital Framework

Lambros, Eleftherios; Link, Benjamin; Chow, Mathew; Hammes-Schiffer, Sharon; Li, Xiaosong

doi:10.1021/acs.jpclett.3c00471

Solvent Induced Proton Polarization within the Nuclear–Electronic Orbital Framework

Journal Article · Tue Mar 21 00:00:00 EDT 2023 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.3c00471· OSTI ID:1974722

Lambros, Eleftherios ^[1]; Link, Benjamin ^[2]; Chow, Mathew ^[3]; ^[3]; ^[2]

University of Washington, Seattle, WA (United States); Yale University
University of Washington, Seattle, WA (United States)
Yale University, New Haven, CT (United States)

To explicitly account for nuclear quantum effects and solvent environments in simulations of chemical processes, the nuclear-electronic orbital approach is coupled with a polarizable continuum model (PCM). This NEO–PCM approach is used to explore the influence of solvation on nuclear polarization through applications to a water dimer and a set of protonated water tetramers. Nuclear polarization in these species is analyzed in terms of changes in proton density and oxygen–hydrogen bond length. Solvation is shown to enhance nuclear polarization with increasing dielectric constant. For the water dimer, the internal, hydrogen-bonded proton is shown to polarize more than the external, free proton. Moreover, proton quantization leads to greater solvent polarization through their mutual polarization. Furthermore, these calculations highlight the complex interplay among electronic, nuclear, and solvent polarization in chemical systems.

View Accepted Manuscript (DOE)

Research Organization:: Yale University, New Haven, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0023284

OSTI ID:: 1974722

Alternate ID(s):: OSTI ID: 2554027

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 12 Vol. 14; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Medium effects on the properties of chemical systems: An overview of recent formulations in the polarizable continuum model (PCM) Tomasi, Jacopo; Cammi, Roberto; Mennucci, Benedetta International Journal of Quantum Chemistry, Vol. 75, Issue 4-5 https://doi.org/10.1002/(SICI)1097-461X(1999)75:4/5<783::AID-QUA44>3.0.CO;2-G	journal	January 1999
Energies, structures, and electronic properties of molecules in solution with the C-PCM solvation model Cossi, Maurizio; Rega, Nadia; Scalmani, Giovanni Journal of Computational Chemistry, Vol. 24, Issue 6 https://doi.org/10.1002/jcc.10189	journal	April 2003
UCSF Chimera?A visualization system for exploratory research and analysis Pettersen, Eric F.; Goddard, Thomas D.; Huang, Conrad C. Journal of Computational Chemistry, Vol. 25, Issue 13 https://doi.org/10.1002/jcc.20084	journal	January 2004
How to make continuum solvation incredibly fast in a few simple steps: A practical guide to the domain decomposition paradigm for the conductor-like screening model Stamm, Benjamin; Lagardère, Louis; Scalmani, Giovanni International Journal of Quantum Chemistry, Vol. 119, Issue 1 https://doi.org/10.1002/qua.25669	journal	August 2018
Polarizable continuum model: Polarizable continuum model Mennucci, Benedetta Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 3 https://doi.org/10.1002/wcms.1086	journal	January 2012
The Chronus Quantum software package Williams‐Young, David B.; Petrone, Alessio; Sun, Shichao WIREs Computational Molecular Science, Vol. 10, Issue 2 https://doi.org/10.1002/wcms.1436	journal	August 2019
Dielectric continuum methods for quantum chemistry Herbert, John M. WIREs Computational Molecular Science, Vol. 11, Issue 4 https://doi.org/10.1002/wcms.1519	journal	March 2021
Electrostatic interaction of a solute with a continuum. A direct utilizaion of AB initio molecular potentials for the prevision of solvent effects Miertuš, S.; Scrocco, E.; Tomasi, J. Chemical Physics, Vol. 55, Issue 1 https://doi.org/10.1016/0301-0104(81)85090-2	journal	February 1981
Alternative formulation of many-body perturbation theory for electron–proton correlation Swalina, Chet; Pak, Michael V.; Hammes-Schiffer, Sharon Chemical Physics Letters, Vol. 404, Issue 4-6 https://doi.org/10.1016/j.cplett.2005.01.115	journal	March 2005
Direct Dynamics with Nuclear–Electronic Orbital Density Functional Theory Tao, Zhen; Yu, Qi; Roy, Saswata Accounts of Chemical Research, Vol. 54, Issue 22 https://doi.org/10.1021/acs.accounts.1c00516	journal	November 2021
Multicomponent Quantum Chemistry: Integrating Electronic and Nuclear Quantum Effects via the Nuclear–Electronic Orbital Method Pavošević, Fabijan; Culpitt, Tanner; Hammes-Schiffer, Sharon Chemical Reviews, Vol. 120, Issue 9 https://doi.org/10.1021/acs.chemrev.9b00798	journal	April 2020
Solvated Nuclear–Electronic Orbital Structure and Dynamics Wildman, Andrew; Tao, Zhen; Zhao, Luning Journal of Chemical Theory and Computation, Vol. 18, Issue 3 https://doi.org/10.1021/acs.jctc.1c01285	journal	February 2022
Benchmark Electronic Structure Calculations for H ₃ O ⁺ (H ₂ O) _n , n = 0–5, Clusters and Tests of an Existing 1,2,3-Body Potential Energy Surface with a New 4-Body Correction Heindel, Joseph P.; Yu, Qi; Bowman, Joel M. Journal of Chemical Theory and Computation, Vol. 14, Issue 9 https://doi.org/10.1021/acs.jctc.8b00598	journal	August 2018
Multicomponent Coupled Cluster Singles and Doubles Theory within the Nuclear-Electronic Orbital Framework Pavošević, Fabijan; Culpitt, Tanner; Hammes-Schiffer, Sharon Journal of Chemical Theory and Computation, Vol. 15, Issue 1 https://doi.org/10.1021/acs.jctc.8b01120	journal	November 2018
Simultaneous Optimization of Nuclear–Electronic Orbitals Liu, Aodong; Chow, Mathew; Wildman, Andrew The Journal of Physical Chemistry A, Vol. 126, Issue 39 https://doi.org/10.1021/acs.jpca.2c05172	journal	September 2022
Real-Time Time-Dependent Nuclear−Electronic Orbital Approach: Dynamics beyond the Born–Oppenheimer Approximation Zhao, Luning; Tao, Zhen; Pavošević, Fabijan The Journal of Physical Chemistry Letters, Vol. 11, Issue 10 https://doi.org/10.1021/acs.jpclett.0c00701	journal	April 2020
Excited State Intramolecular Proton Transfer with Nuclear-Electronic Orbital Ehrenfest Dynamics Zhao, Luning; Wildman, Andrew; Pavošević, Fabijan The Journal of Physical Chemistry Letters, Vol. 12, Issue 14 https://doi.org/10.1021/acs.jpclett.1c00564	journal	April 2021
Multicomponent Density Functional Theory: Impact of Nuclear Quantum Effects on Proton Affinities and Geometries Brorsen, Kurt R.; Yang, Yang; Hammes-Schiffer, Sharon The Journal of Physical Chemistry Letters, Vol. 8, Issue 15 https://doi.org/10.1021/acs.jpclett.7b01442	journal	July 2017
Proton-Coupled Electron Transfer Weinberg, David R.; Gagliardi, Christopher J.; Hull, Jonathan F. Chemical Reviews, Vol. 112, Issue 7 https://doi.org/10.1021/cr200177j	journal	April 2012
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
Improving Generalized Born Models by Exploiting Connections to Polarizable Continuum Models. I. An Improved Effective Coulomb Operator Lange, Adrian W.; Herbert, John M. Journal of Chemical Theory and Computation, Vol. 8, Issue 6 https://doi.org/10.1021/ct300111m	journal	May 2012
Improving Generalized Born Models by Exploiting Connections to Polarizable Continuum Models. II. Corrections for Salt Effects Lange, Adrian W.; Herbert, John M. Journal of Chemical Theory and Computation, Vol. 8, Issue 11 https://doi.org/10.1021/ct300493y	journal	September 2012
Describing Noncovalent Interactions beyond the Common Approximations: How Accurate Is the “Gold Standard,” CCSD(T) at the Complete Basis Set Limit? Řezáč, Jan; Hobza, Pavel Journal of Chemical Theory and Computation, Vol. 9, Issue 5 https://doi.org/10.1021/ct400057w	journal	April 2013
Fast Domain Decomposition Algorithm for Continuum Solvation Models: Energy and First Derivatives Lipparini, Filippo; Stamm, Benjamin; Cancès, Eric Journal of Chemical Theory and Computation, Vol. 9, Issue 8 https://doi.org/10.1021/ct400280b	journal	July 2013
Density Functional Theory Treatment of Electron Correlation in the Nuclear−Electronic Orbital Approach Pak, Michael V.; Chakraborty, Arindam; Hammes-Schiffer, Sharon The Journal of Physical Chemistry A, Vol. 111, Issue 20 https://doi.org/10.1021/jp0704463	journal	May 2007
Performance Test of Multicomponent Quantum Mechanical Calculation with Polarizable Continuum Model for Proton Chemical Shift Kanematsu, Yusuke; Tachikawa, Masanori The Journal of Physical Chemistry A, Vol. 119, Issue 20 https://doi.org/10.1021/jp512877a	journal	May 2015
Quantum Calculation of Molecular Energies and Energy Gradients in Solution by a Conductor Solvent Model Barone, Vincenzo; Cossi, Maurizio The Journal of Physical Chemistry A, Vol. 102, Issue 11 https://doi.org/10.1021/jp9716997	journal	March 1998
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
New applications of integral equations methods for solvation continuum models: ionic solutions and liquid crystals Cancès, Eric; Mennucci, Benedetta Journal of Mathematical Chemistry, Vol. 23, Issue 3/4, p. 309-326 https://doi.org/10.1023/A:1019133611148	journal	January 1998
COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient Klamt, A.; Schüürmann, G. J. Chem. Soc., Perkin Trans. 2, Issue 5 https://doi.org/10.1039/P29930000799	journal	January 1993
Multiconfigurational nuclear-electronic orbital approach: Incorporation of nuclear quantum effects in electronic structure calculations Webb, Simon P.; Iordanov, Tzvetelin; Hammes-Schiffer, Sharon The Journal of Chemical Physics, Vol. 117, Issue 9 https://doi.org/10.1063/1.1494980	journal	September 2002
New formulation and implementation for volume polarization in dielectric continuum theory Chipman, Daniel M. The Journal of Chemical Physics, Vol. 124, Issue 22 https://doi.org/10.1063/1.2203068	journal	June 2006
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen Dunning, Thom H. The Journal of Chemical Physics, Vol. 90, Issue 2 https://doi.org/10.1063/1.456153	journal	January 1989
Treatment of the outlying charge in continuum solvation models Klamt, Andreas; Jonas, Volker The Journal of Chemical Physics, Vol. 105, Issue 22 https://doi.org/10.1063/1.472829	journal	December 1996
A new integral equation formalism for the polarizable continuum model: Theoretical background and applications to isotropic and anisotropic dielectrics Cancès, E.; Mennucci, B.; Tomasi, J. The Journal of Chemical Physics, Vol. 107, Issue 8 https://doi.org/10.1063/1.474659	journal	August 1997
Toward reliable density functional methods without adjustable parameters: The PBE0 model Adamo, Carlo; Barone, Vincenzo The Journal of Chemical Physics, Vol. 110, Issue 13 https://doi.org/10.1063/1.478522	journal	April 1999
Simulation of volume polarization in reaction field theory Chipman, Daniel M. The Journal of Chemical Physics, Vol. 110, Issue 16 https://doi.org/10.1063/1.478729	journal	April 1999
Solvent effect on vertical electronic transitions by the polarizable continuum model Cossi, Maurizio; Barone, Vincenzo The Journal of Chemical Physics, Vol. 112, Issue 5 https://doi.org/10.1063/1.480808	journal	February 2000
Development of multicomponent hybrid density functional theory with polarizable continuum model for the analysis of nuclear quantum effect and solvent effect on NMR chemical shift Kanematsu, Yusuke; Tachikawa, Masanori The Journal of Chemical Physics, Vol. 140, Issue 16 https://doi.org/10.1063/1.4872006	journal	April 2014
Quantum, classical, and hybrid QM/MM calculations in solution: General implementation of the ddCOSMO linear scaling strategy Lipparini, Filippo; Scalmani, Giovanni; Lagardère, Louis The Journal of Chemical Physics, Vol. 141, Issue 18 https://doi.org/10.1063/1.4901304	journal	November 2014
Perspective: Polarizable continuum models for quantum-mechanical descriptions Lipparini, Filippo; Mennucci, Benedetta The Journal of Chemical Physics, Vol. 144, Issue 16 https://doi.org/10.1063/1.4947236	journal	April 2016
Development of a practical multicomponent density functional for electron-proton correlation to produce accurate proton densities Yang, Yang; Brorsen, Kurt R.; Culpitt, Tanner The Journal of Chemical Physics, Vol. 147, Issue 11 https://doi.org/10.1063/1.4996038	journal	September 2017
Development of nuclear basis sets for multicomponent quantum chemistry methods Yu, Qi; Pavošević, Fabijan; Hammes-Schiffer, Sharon The Journal of Chemical Physics, Vol. 152, Issue 24 https://doi.org/10.1063/5.0009233	journal	June 2020
Nuclear–electronic orbital Ehrenfest dynamics Zhao, Luning; Wildman, Andrew; Tao, Zhen The Journal of Chemical Physics, Vol. 153, Issue 22 https://doi.org/10.1063/5.0031019	journal	December 2020
Software for the frontiers of quantum chemistry: An overview of developments in the Q-Chem 5 package Epifanovsky, Evgeny; Gilbert, Andrew T. B.; Feng, Xintian The Journal of Chemical Physics, Vol. 155, Issue 8 https://doi.org/10.1063/5.0055522	journal	August 2021
Matplotlib: A 2D Graphics Environment Hunter, John D. Computing in Science & Engineering, Vol. 9, Issue 3 https://doi.org/10.1109/MCSE.2007.55	journal	January 2007
Modern Theoretical Approaches to Modeling the Excited-State Intramolecular Proton Transfer: An Overview Jankowska, Joanna; Sobolewski, Andrzej L. Molecules, Vol. 26, Issue 17 https://doi.org/10.3390/molecules26175140	journal	August 2021

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Solvent Induced Proton Polarization within the Nuclear–Electronic Orbital Framework

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