The Role of Molecular Arrangement on the Dispersion in Strongly Coupled Metal-Organic Hybrid Structures

Rödel, Maximilian; Lisinetskaya, Polina G.; Rudloff, Maximilian; Stark, Thomas; Manara, Jochen; Mitrić, Roland; Pflaum, Jens

doi:10.48550/arxiv.2111.09185

Cited by 1 publication

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“…degree of freedom amenable to optimization beyond Fabry-Perot configurations, [6][7][8] and, when the interaction is strong enough, hybrid light-matter modes known as polaritons will form inside the cavity: The optical properties of the joint system can differ significantly from the separate responses of cavity and materials. [10][11][12][13][14][15][16][17][18][19] The choice of MOFs as active materials inside the cavities is motivated by the crystallinity and porosity of this class of reticular compounds, which makes possible a straightforward experimental characterization using X-ray diffraction methods as well as a tuning of the dielectric constant inside the cavity by loading the MOFs with small molecules. Hybrid light-matter states have also been observed in MOFs placed on a plasmonic nanoparticle lattice [20] and even in molecular films on top of substrates.…”

Section: Introductionmentioning

confidence: 99%

A Multi‐Scale Approach for Modeling the Optical Response of Molecular Materials Inside Cavities

et al. 2022

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The recent fabrication advances in nanoscience and molecular materials point toward a new era where material properties are tailored in silico for target applications. To fully realize this potential, accurate and computationally efficient theoretical models are needed for: a) the computer‐aided design and optimization of new materials before their fabrication; and b) the accurate interpretation of experiments. The development of such theoretical models is a challenging multi‐disciplinary problem where physics, chemistry, and material science are intertwined across spatial scales ranging from the molecular to the device level, that is, from ångströms to millimeters. In photonic applications, molecular materials are often placed inside optical cavities. Together with the sought‐after enhancement of light‐molecule interactions, the cavities bring additional complexity to the modeling of such devices. Here, a multi‐scale approach that, starting from ab initio quantum mechanical molecular simulations, can compute the electromagnetic response of macroscopic devices such as cavities containing molecular materials is presented. Molecular time‐dependent density‐functional theory calculations are combined with the efficient transition matrix based solution of Maxwell's equations. Some of the capabilities of the approach are demonstrated by simulating surface metal‐organic frameworks ‐in‐cavity and J‐aggregates‐in‐cavity systems that have been recently investigated experimentally, and providing a refined understanding of the experimental results.

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