Excited States in Solution through Polarizable Embedding

Jógvan Magnus Olsen, Kestutis Aidas, Jacob Kongsted

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

Resumé

We present theory and implementation of an advanced quantum mechanics/molecular mechanics (QM/MM) approach using a fully self-consistent polarizable embedding (PE) scheme. It is a polarizable layered model designed for effective yet accurate inclusion of an anisotropic medium in a quantum mechanical calculation. The polarizable embedding potential is described by an atomistic representation including terms up to localized octupoles and anisotropic polarizabilities. It is generally applicable to any quantum chemical description but is here implemented for the case of Kohn−Sham density functional theory which we denote the PE-DFT method. It has been implemented in combination with time-dependent quantum mechanical linear and nonlinear response techniques, thus allowing for assessment of electronic excitation processes and dynamic ground- and excited-state molecular properties using a nonequilibrium formulation of the environmental response. In our formulation of polarizable embedding we explicitly take into account the full self-consistent many-body environmental response from both ground and excited states. The PE-DFT method can be applied to any molecular system, e.g., proteins, nanoparticles and solute−solvent systems. Here, we present numerical examples of solvent shifts and excited-state properties related to a set of organic molecules in aqueous solution.
OriginalsprogEngelsk
TidsskriftJournal of Chemical Theory and Computation
Vol/bind6
Udgave nummer12
Sider (fra-til)3721-3734
ISSN1549-9618
DOI
StatusUdgivet - 2010

Fingeraftryk

Excited states
embedding
Discrete Fourier transforms
Ground state
excitation
Anisotropic media
Molecular mechanics
Quantum theory
Density functional theory
formulations
ground state
Nanoparticles
molecular properties
anisotropic media
Proteins
Molecules
quantum mechanics
inclusions
density functional theory
aqueous solutions

Citer dette

Olsen, Jógvan Magnus ; Aidas, Kestutis ; Kongsted, Jacob. / Excited States in Solution through Polarizable Embedding. I: Journal of Chemical Theory and Computation. 2010 ; Bind 6, Nr. 12. s. 3721-3734.
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abstract = "We present theory and implementation of an advanced quantum mechanics/molecular mechanics (QM/MM) approach using a fully self-consistent polarizable embedding (PE) scheme. It is a polarizable layered model designed for effective yet accurate inclusion of an anisotropic medium in a quantum mechanical calculation. The polarizable embedding potential is described by an atomistic representation including terms up to localized octupoles and anisotropic polarizabilities. It is generally applicable to any quantum chemical description but is here implemented for the case of Kohn−Sham density functional theory which we denote the PE-DFT method. It has been implemented in combination with time-dependent quantum mechanical linear and nonlinear response techniques, thus allowing for assessment of electronic excitation processes and dynamic ground- and excited-state molecular properties using a nonequilibrium formulation of the environmental response. In our formulation of polarizable embedding we explicitly take into account the full self-consistent many-body environmental response from both ground and excited states. The PE-DFT method can be applied to any molecular system, e.g., proteins, nanoparticles and solute−solvent systems. Here, we present numerical examples of solvent shifts and excited-state properties related to a set of organic molecules in aqueous solution.",
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Excited States in Solution through Polarizable Embedding. / Olsen, Jógvan Magnus; Aidas, Kestutis; Kongsted, Jacob.

I: Journal of Chemical Theory and Computation, Bind 6, Nr. 12, 2010, s. 3721-3734.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

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AU - Aidas, Kestutis

AU - Kongsted, Jacob

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AB - We present theory and implementation of an advanced quantum mechanics/molecular mechanics (QM/MM) approach using a fully self-consistent polarizable embedding (PE) scheme. It is a polarizable layered model designed for effective yet accurate inclusion of an anisotropic medium in a quantum mechanical calculation. The polarizable embedding potential is described by an atomistic representation including terms up to localized octupoles and anisotropic polarizabilities. It is generally applicable to any quantum chemical description but is here implemented for the case of Kohn−Sham density functional theory which we denote the PE-DFT method. It has been implemented in combination with time-dependent quantum mechanical linear and nonlinear response techniques, thus allowing for assessment of electronic excitation processes and dynamic ground- and excited-state molecular properties using a nonequilibrium formulation of the environmental response. In our formulation of polarizable embedding we explicitly take into account the full self-consistent many-body environmental response from both ground and excited states. The PE-DFT method can be applied to any molecular system, e.g., proteins, nanoparticles and solute−solvent systems. Here, we present numerical examples of solvent shifts and excited-state properties related to a set of organic molecules in aqueous solution.

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