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Near-field scanning optical microscopy of molecular aggregates: The role of light polarization

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Nayak,  Sidhartha
Max Planck Institute for the Physics of Complex Systems, Max Planck Society;

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Zheng,  Fulu
Max Planck Institute for the Physics of Complex Systems, Max Planck Society;

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Eisfeld,  Alexander
Max Planck Institute for the Physics of Complex Systems, Max Planck Society;

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Citation

Nayak, S., Zheng, F., & Eisfeld, A. (2020). Near-field scanning optical microscopy of molecular aggregates: The role of light polarization. The Journal of Chemical Physics, 155(13): 134701. doi:10.1063/5.0064133.


Cite as: https://hdl.handle.net/21.11116/0000-0009-9E9A-8
Abstract
We consider theoretically near-field absorption spectra of molecular aggregates stemming from a scattering scanning near-field optical microscopy type setup. Our focus is on the dependence on the direction and polarization of the incoming electromagnetic radiation, which induces a Hertz dipole with a specific orientation at the tip-apex. Within a simple description, which is based on the eigenstates of the aggregate, absorption spectra are calculated for the near field created by this dipole. We find that the spatial patterns of the spectra have a strong dependence on the orientation of this tip-dipole, which can be understood by considering three basic functions that only depend on the arrangement of the aggregate and the molecule tip distance, but not on the orientation of the tip-dipole. This allows direct access to spatial dependence of the aggregate eigenstates. For the important cases of one- and two-dimensional systems with parallel molecules, we discuss these spectra in detail. The simple numerically efficient approach is validated by a more detailed description where the incoming radiation and the interaction between the tip and molecules are explicitly taken into account.& nbsp;(C) 2021 Author(s).