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Résumé
In this work, expressions for the third-harmonic scattering optical activity (THS-OA) spectroscopic responses are derived by combining molecular quantum electrodynamics (QED) and response theory, allowing their computational implementation. The QED theory of THS-OA presented here is meant to be an extension of a previous study by Andrews [Symmetry 12, 1466 (2020)]. In particular, the THS-OA phenomena are described within the Power-Zienau-Woolley multipolar Hamiltonian by including the electric-dipole, magnetic-dipole, and electric-quadrupole interactions for the absorption as well as the emission processes between the dynamic electromagnetic field (the photons) and matter. Moreover, we derive the expressions for the differential scattering ratios as a function of the scattering angle defined by the wavevectors of the incident and scattered photons. We show how the pure and mixed second hyperpolarizabilities can be obtained in the framework of response theory as specific cases of a generic cubic response function, thus enabling the computational implementation of THS-OA spectroscopy. We prove the origin-independence of the theory for exact wavefunctions. Preliminary computations on a prototype chiral molecule (methyloxirane) are considered together with an analysis of the basis set convergence and of the origin-dependence.
langue originale | Anglais |
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Numéro d'article | 114107 |
journal | The Journal of chemical physics |
Volume | 159 |
Numéro de publication | 11 |
Les DOIs | |
Etat de la publication | Publié - 21 sept. 2023 |
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Examiner les sujets de recherche de « Third-harmonic scattering optical activity: QED theory, symmetry considerations, and quantum chemistry applications in the framework of response theory ». Ensemble, ils forment une empreinte digitale unique.Projets
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Renouvellement d’équipements pour le Consortium des Equipements de Calcul Intensif (CECI)
Bontempi, G. (Responsable du Projet), CHAMPAGNE, B. (CoPI), Geuzaine , C. (CoPI), RIGNANESE, G. M. (CoPI) & Lazzaroni, R. (CoPI)
1/01/22 → 31/12/23
Projet: Recherche
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Helices oligomériques fonctionnelles comme matériaux moléculaires chiraux polyvalents pour l'optique et la chiroptique non linéaire du deuxième ordre
CHAMPAGNE, B. (Responsable du Projet)
1/01/22 → 31/12/23
Projet: Recherche
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Plateforme Technologique Calcul Intensif
Champagne, B. (!!Manager)
Plateforme technologique Calcul intensifEquipement/installations: Plateforme technolgique
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University of Namur Researcher Describes Research in Chemical Physics (Third-harmonic scattering optical activity: QED theory, symmetry considerations, and quantum chemistry applications in the framework of response theory)
3/10/23
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