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Issue 40, 2016
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Open-ended response theory with polarizable embedding: multiphoton absorption in biomolecular systems

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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.

Graphical abstract: Open-ended response theory with polarizable embedding: multiphoton absorption in biomolecular systems

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Publication details

The article was received on 30 Jul 2016, accepted on 19 Sep 2016 and first published on 19 Sep 2016


Article type: Paper
DOI: 10.1039/C6CP05297E
Citation: Phys. Chem. Chem. Phys., 2016,18, 28339-28352
  • Open access: Creative Commons BY license
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    Open-ended response theory with polarizable embedding: multiphoton absorption in biomolecular systems

    A. H. Steindal, M. T. P. Beerepoot, M. Ringholm, N. H. List, K. Ruud, J. Kongsted and J. M. H. Olsen, Phys. Chem. Chem. Phys., 2016, 18, 28339
    DOI: 10.1039/C6CP05297E

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