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arXiv · 2110.05181

Modification of the Optical Properties of Molecular Chains upon Coupling to Adatoms

Marvin M. Müller·Miriam Kosik·Marta Pelc·Garnett W. Bryant·Andrés Ayuela·Carsten Rockstuhl·Karolina Słowik
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Abstract

Adsorbed atoms (adatoms) coupled to the matrix of solid state host materials as impurities can significantly modify their properties. Especially in low-dimensional materials, such as one-dimensional organic polymer chains or quasi-one-dimensional graphene nanoribbons, intriguing manipulation of the optical properties, such as the absorption cross section, is possible. The most widely used approach to couple quantum emitters to optical antennas is based on the Purcell effect. This formalism, however, does not comprise charge transfer from the emitter to the antenna, but only spontaneous emission of the quantum emitter into the tailored photonic environment, that is evoked by the antenna. To capture such effects, we present a tight-binding formalism to couple an adatom to a finite Su-Schrieffer-Heeger chain, where the former is treated as a two-level system and the latter acts as an optical antenna. We systematically analyze how the coupling strength and the position of the adatom influence the optical properties of the molecular chains in the model. We take into account charge transfer from the adatom to the antenna and vice versa via an inter-system hopping parameter, and also include Coulomb interaction within the antenna as well as between the adatom and the antenna. We show that coupling the adatom to one of the bulk atoms of the linear chain results in a substantial change in optical properties already for comparatively small coupling strengths. We also find that the position of the adatom crucially determines if and how the optical properties of the chains are altered. Therefore, we identify this adatom-chain hybrid system as a tunable platform for light-matter interaction at the nanoscale.

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Marvin M. Müller, Miriam Kosik, Marta Pelc, Garnett W. Bryant, Andrés Ayuela, Carsten Rockstuhl, Karolina Słowik. 2021-10-11. Modification of the Optical Properties of Molecular Chains upon Coupling to Adatoms. https://doi.org/10.1103/physrevb.104.235414

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