Beyond the electric-dipole approximation: A formulation and implementation of molecular response theory for the description of absorption of electromagnetic field radiation
| Autor: | Joanna Kauczor, Nanna Holmgaard List, Patrick Norman, Hans Jørgen Aagaard Jensen, Trond Saue |
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| Přispěvatelé: | University of Southern Denmark (SDU), Groupe Méthodes et outils de la chimie quantique (LCPQ) (GMO), Laboratoire de Chimie et Physique Quantiques (LCPQ), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Linköping University (LIU), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse) |
| Jazyk: | angličtina |
| Rok vydání: | 2015 |
| Předmět: |
Electromagnetic field
Models Molecular Photon Molecular Conformation General Physics and Astronomy Electron Polyenes Electromagnetic Fields Metals Alkaline Earth Magnesium Physical and Theoretical Chemistry ComputingMilieux_MISCELLANEOUS Physics Photons Linear polarization Propagator Absorption Radiation Kemi Models Theoretical Polarization (waves) [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry Dipole Electric dipole moment Chemical Sciences Quantum Theory Atomic physics |
| Zdroj: | Journal of Chemical Physics Journal of Chemical Physics, American Institute of Physics, 2015, 142 (24), pp.244111. ⟨10.1063/1.4922697⟩ List, N H, Kauzcor, J, Saue, T, Jensen, H J A & Norman, P 2015, ' Beyond the electric-dipole approximation: A formulation and implementation of molecular response theory for the description of absorption of electromagnetic field radiation ', The Journal of Chemical Physics, vol. 142, 244111 . https://doi.org/10.1063/1.4922697 |
| ISSN: | 0021-9606 1089-7690 |
| DOI: | 10.1063/1.4922697⟩ |
| Popis: | We present a formulation of molecular response theory for the description of a quantum mechanical molecular system in the presence of a weak, monochromatic, linearly polarized electromagnetic field without introducing truncated multipolar expansions. The presentation focuses on a description of linear absorption by adopting the energy-loss approach in combination with the complex polarization propagator formulation of response theory. Going beyond the electric-dipole approximation is essential whenever studying electric-dipole-forbidden transitions, and in general, non-dipolar effects become increasingly important when addressing spectroscopies involving higher-energy photons. These two aspects are examined by our study of the near K-edge X-ray absorption fine structure of the alkaline earth metals (Mg, Ca, Sr, Ba, and Ra) as well as the trans-polyenes. In following the series of alkaline earth metals, the sizes of non-dipolar effects are probed with respect to increasing photon energies and a detailed assessment of results is made in terms of studying the pertinent transition electron densities and in particular their spatial extension in comparison with the photon wavelength. Along the series of trans-polyenes, the sizes of non-dipolar effects are probed for X-ray spectroscopies on organic molecules with respect to the spatial extension of the chromophore. Funding Agencies|Lundbeck Foundation; Danish Council for Independent Research; Knut and Alice Wallenberg Foundation [KAW-2013.0020]; Swedish Research Council [621-2014-4646] |
| Databáze: | OpenAIRE |
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