Regensburg 2019 – wissenschaftliches Programm
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CPP: Fachverband Chemische Physik und Polymerphysik
CPP 3: Molecular Electronics and Excited State Properties
CPP 3.10: Vortrag
Montag, 1. April 2019, 12:15–12:30, H13
Interplay between intra- and inter-molecular charge transfer in the optical excitations of J-aggregates — •Michele Guerrini1,2,3, Caterina Cocchi2, Arrigo Calzolari3, Daniele Varsano3, and Stefano Corni3,4 — 1Dept. FIM, Univ. of Modena and Reggio Emilia, Italy — 2Dept. of Physics and IRIS Adlershof, Humboldt Universität zu-Berlin, Germany — 3CNR Nano, Centro S3, Modena, Italy — 4Dept. Chem. Scienc., Univ. of Padova, Italy
Molecular J-aggregates formed by push-pull chromophores have appealing optical properties which are dominated by collective and supramolecular effects, as recently demonstrated from first principles [1]. Here, we investigate the character of the optical excitations from many-body perturbation theory, focusing on the interplay between intra- and inter-molecular interactions. We find that the most intense excitation which dominates the spectral onset (the so-called J-band) exhibits a combination of intra-molecular charge transfer, coming from the push-pull character of the constituting dyes, and inter-molecular charge-transfer, due to the dense molecular packing which favors wave-function delocalization. Within the J-band we also reveal the presence of a pure inter-molecular charge-transfer excitation. Our results [2] shed light into the microscopic character of optical excitations in J-aggregates and offer new perspectives for understanding the nature of collective excitations in organic molecular solids.
[1] M. Guerrini; A. Calzolari; S. Corni ACS Omega 2018, 3 (9), 10481-10486. [2] M. Guerrini; C. Cocchi; A. Calzolari; D. Varsano; S. Corni submitted (2018).