Open-ended response theory with polarizable embedding

Multiphoton absorption in biomolecular systems

Arnfinn Hykkerud Steindal, Maarten T P Beerepoot, Magnus Ringholm, Nanna Holmgaard List, Kenneth Ruud, Jacob Kongsted, Jógvan Magnus Haugaard Olsen*

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Resumé

We present the theory and implementation of an open-ended framework for electric response properties at the level of Hartree-Fock and Kohn-Sham density functional theory that includes effects from the molecular environment modeled by the polarizable embedding (PE) model. With this new state-of-the-art multiscale functionality, electric response properties to any order can be calculated for molecules embedded in polarizable atomistic molecular environments ranging from solvents to complex heterogeneous macromolecules such as proteins. In addition, environmental effects on multiphoton absorption (MPA) properties can be studied by evaluating single residues of the response functions. The PE approach includes mutual polarization effects between the quantum and classical parts of the system through induced dipoles that are determined self-consistently with respect to the electronic density. The applicability of our approach is demonstrated by calculating MPA strengths up to four-photon absorption for the green fluorescent protein. We show how the size of the quantum region, as well as the treatment of the border between the quantum and classical regions, is crucial in order to obtain reliable MPA predictions.

OriginalsprogEngelsk
TidsskriftPhysical Chemistry Chemical Physics
Vol/bind18
Udgave nummer40
Sider (fra-til)28339-28352
ISSN1463-9076
DOI
StatusUdgivet - 2016

Fingeraftryk

multiphoton absorption
Green Fluorescent Proteins
Macromolecules
embedding
Density functional theory
Environmental impact
Photons
Polarization
Molecules
proteins
Proteins
borders
macromolecules
dipoles
density functional theory
photons
polarization
predictions
electronics
molecules

Citer dette

Steindal, A. H., Beerepoot, M. T. P., Ringholm, M., List, N. H., Ruud, K., Kongsted, J., & Olsen, J. M. H. (2016). Open-ended response theory with polarizable embedding: Multiphoton absorption in biomolecular systems. Physical Chemistry Chemical Physics, 18(40), 28339-28352. https://doi.org/10.1039/c6cp05297e
Steindal, Arnfinn Hykkerud ; Beerepoot, Maarten T P ; Ringholm, Magnus ; List, Nanna Holmgaard ; Ruud, Kenneth ; Kongsted, Jacob ; Olsen, Jógvan Magnus Haugaard. / Open-ended response theory with polarizable embedding : Multiphoton absorption in biomolecular systems. I: Physical Chemistry Chemical Physics. 2016 ; Bind 18, Nr. 40. s. 28339-28352.
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abstract = "We present the theory and implementation of an open-ended framework for electric response properties at the level of Hartree-Fock and Kohn-Sham density functional theory that includes effects from the molecular environment modeled by the polarizable embedding (PE) model. With this new state-of-the-art multiscale functionality, electric response properties to any order can be calculated for molecules embedded in polarizable atomistic molecular environments ranging from solvents to complex heterogeneous macromolecules such as proteins. In addition, environmental effects on multiphoton absorption (MPA) properties can be studied by evaluating single residues of the response functions. The PE approach includes mutual polarization effects between the quantum and classical parts of the system through induced dipoles that are determined self-consistently with respect to the electronic density. The applicability of our approach is demonstrated by calculating MPA strengths up to four-photon absorption for the green fluorescent protein. We show how the size of the quantum region, as well as the treatment of the border between the quantum and classical regions, is crucial in order to obtain reliable MPA predictions.",
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Open-ended response theory with polarizable embedding : Multiphoton absorption in biomolecular systems. / Steindal, Arnfinn Hykkerud; Beerepoot, Maarten T P; Ringholm, Magnus; List, Nanna Holmgaard; Ruud, Kenneth; Kongsted, Jacob; Olsen, Jógvan Magnus Haugaard.

I: Physical Chemistry Chemical Physics, Bind 18, Nr. 40, 2016, s. 28339-28352.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Open-ended response theory with polarizable embedding

T2 - Multiphoton absorption in biomolecular systems

AU - Steindal, Arnfinn Hykkerud

AU - Beerepoot, Maarten T P

AU - Ringholm, Magnus

AU - List, Nanna Holmgaard

AU - Ruud, Kenneth

AU - Kongsted, Jacob

AU - Olsen, Jógvan Magnus Haugaard

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N2 - We present the theory and implementation of an open-ended framework for electric response properties at the level of Hartree-Fock and Kohn-Sham density functional theory that includes effects from the molecular environment modeled by the polarizable embedding (PE) model. With this new state-of-the-art multiscale functionality, electric response properties to any order can be calculated for molecules embedded in polarizable atomistic molecular environments ranging from solvents to complex heterogeneous macromolecules such as proteins. In addition, environmental effects on multiphoton absorption (MPA) properties can be studied by evaluating single residues of the response functions. The PE approach includes mutual polarization effects between the quantum and classical parts of the system through induced dipoles that are determined self-consistently with respect to the electronic density. The applicability of our approach is demonstrated by calculating MPA strengths up to four-photon absorption for the green fluorescent protein. We show how the size of the quantum region, as well as the treatment of the border between the quantum and classical regions, is crucial in order to obtain reliable MPA predictions.

AB - We present the theory and implementation of an open-ended framework for electric response properties at the level of Hartree-Fock and Kohn-Sham density functional theory that includes effects from the molecular environment modeled by the polarizable embedding (PE) model. With this new state-of-the-art multiscale functionality, electric response properties to any order can be calculated for molecules embedded in polarizable atomistic molecular environments ranging from solvents to complex heterogeneous macromolecules such as proteins. In addition, environmental effects on multiphoton absorption (MPA) properties can be studied by evaluating single residues of the response functions. The PE approach includes mutual polarization effects between the quantum and classical parts of the system through induced dipoles that are determined self-consistently with respect to the electronic density. The applicability of our approach is demonstrated by calculating MPA strengths up to four-photon absorption for the green fluorescent protein. We show how the size of the quantum region, as well as the treatment of the border between the quantum and classical regions, is crucial in order to obtain reliable MPA predictions.

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