Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field

Greta Donati; Andrew Wildman; Stefano Caprasecca; David B. Lingerfelt; Filippo Lipparini; Benedetta Mennucci; Xiaosong Li

doi:10.1021/acs.jpclett.7b02320

Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field

Greta Donati
, Andrew Wildman
, Stefano Caprasecca
, David B. Lingerfelt
, Filippo Lipparini
, Benedetta Mennucci
, Xiaosong Li

Research output: Contribution to journal › Review article › peer-review

28 Scopus citations

Abstract

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful tool for obtaining spectroscopic observables and understanding complex, time-dependent properties. Currently, performing RT-TDDFT calculations on large, fully quantum mechanical systems is not computationally feasible. Previously, polarizable mixed quantum mechanical and molecular mechanical (QM/MMPol) models have been successful in providing accurate, yet efficient, approximations to a fully quantum mechanical system. Here we develop a coupling scheme between induced dipole based QM/MMPol and RT-TDDFT. Our approach is validated by comparing calculated spectra with both real-time and linear-response TDDFT calculations. The model developed within provides an accurate method for performing RT-TDDFT calculations on extended systems while accounting for mutual polarization between the quantum mechanical and molecular mechanical regions.

Original language	English
Pages (from-to)	5283-5289
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	8
Issue number	21
DOIs	https://doi.org/10.1021/acs.jpclett.7b02320
State	Published - Nov 2 2017
Externally published	Yes

Funding

The development of the solvated electronic dynamics is funded by the U.S. Department of Energy (DE-SC0006863 to X.L.). The development of ab initio linear response theory is supported by the U.S. National Science Foundation (CHE-1565520 to X.L.). Computations were facilitated through the use of advanced computational, storage, and networking infrastructure provided by the Hyak supercomputer system at the University of Washington, funded by the Student Technology Fee, and the National Science Foundation (MRI-1624430).

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10.1021/acs.jpclett.7b02320

Cite this

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title = "Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field",

abstract = "Real-time time-dependent density functional theory (RT-TDDFT) is a powerful tool for obtaining spectroscopic observables and understanding complex, time-dependent properties. Currently, performing RT-TDDFT calculations on large, fully quantum mechanical systems is not computationally feasible. Previously, polarizable mixed quantum mechanical and molecular mechanical (QM/MMPol) models have been successful in providing accurate, yet efficient, approximations to a fully quantum mechanical system. Here we develop a coupling scheme between induced dipole based QM/MMPol and RT-TDDFT. Our approach is validated by comparing calculated spectra with both real-time and linear-response TDDFT calculations. The model developed within provides an accurate method for performing RT-TDDFT calculations on extended systems while accounting for mutual polarization between the quantum mechanical and molecular mechanical regions.",

author = "Greta Donati and Andrew Wildman and Stefano Caprasecca and Lingerfelt, \{David B.\} and Filippo Lipparini and Benedetta Mennucci and Xiaosong Li",

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doi = "10.1021/acs.jpclett.7b02320",

language = "English",

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T1 - Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field

AU - Donati, Greta

AU - Wildman, Andrew

AU - Caprasecca, Stefano

AU - Lingerfelt, David B.

AU - Lipparini, Filippo

AU - Mennucci, Benedetta

AU - Li, Xiaosong

PY - 2017/11/2

Y1 - 2017/11/2

N2 - Real-time time-dependent density functional theory (RT-TDDFT) is a powerful tool for obtaining spectroscopic observables and understanding complex, time-dependent properties. Currently, performing RT-TDDFT calculations on large, fully quantum mechanical systems is not computationally feasible. Previously, polarizable mixed quantum mechanical and molecular mechanical (QM/MMPol) models have been successful in providing accurate, yet efficient, approximations to a fully quantum mechanical system. Here we develop a coupling scheme between induced dipole based QM/MMPol and RT-TDDFT. Our approach is validated by comparing calculated spectra with both real-time and linear-response TDDFT calculations. The model developed within provides an accurate method for performing RT-TDDFT calculations on extended systems while accounting for mutual polarization between the quantum mechanical and molecular mechanical regions.

AB - Real-time time-dependent density functional theory (RT-TDDFT) is a powerful tool for obtaining spectroscopic observables and understanding complex, time-dependent properties. Currently, performing RT-TDDFT calculations on large, fully quantum mechanical systems is not computationally feasible. Previously, polarizable mixed quantum mechanical and molecular mechanical (QM/MMPol) models have been successful in providing accurate, yet efficient, approximations to a fully quantum mechanical system. Here we develop a coupling scheme between induced dipole based QM/MMPol and RT-TDDFT. Our approach is validated by comparing calculated spectra with both real-time and linear-response TDDFT calculations. The model developed within provides an accurate method for performing RT-TDDFT calculations on extended systems while accounting for mutual polarization between the quantum mechanical and molecular mechanical regions.

UR - https://www.scopus.com/pages/publications/85032786695

U2 - 10.1021/acs.jpclett.7b02320

DO - 10.1021/acs.jpclett.7b02320

M3 - Review article

C2 - 28994290

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EP - 5289

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 21

ER -

Coupling Real-Time Time-Dependent Density Functional Theory with Polarizable Force Field

Abstract

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