Molecules in (fancy) cavities

Zerulla, Benedikt; Krstić, Marjan; Beutel, Dominik; Holzer, Christof; Rockstuhl, Carsten; Fernandez‐Corbaton, Ivan

doi:10.1117/12.2620691

Cited by 1 publication

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“…In a very recent study, the method has already been applied to disclose the origin of the surface SHG signal of molecular films and its quantification. [ 36 ] In that study, every layer is described by a different second‐order nonlinearity, which can be simulated with the presented approach but not with an approach based on homogenization. The first hyperpolarizability of each layer can be calculated by embedding the quantum region within the field of partial charges, simulating the effects of the interface between the molecular film and the surrounding.…”

Section: Introductionmentioning

confidence: 99%

A Multi‐Scale Approach to Simulate the Nonlinear Optical Response of Molecular Nanomaterials

Zerulla,

Beutel,

Holzer

et al. 2023

Advanced Materials

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Nonlinear optics is essential for many recent photonic technologies. Here, a novel multi‐scale approach is introduced to simulate the nonlinear optical response of molecular nanomaterials combining ab initio quantum‐chemical and classical Maxwell‐scattering computations. In this approach, the first hyperpolarizability tensor is computed with time‐dependent density‐functional theory and incorporated into a multi‐scattering formalism that considers the optical interaction between neighboring molecules. Such incorporation is achieved by a novel object: the Hyper‐Transition(T)‐matrix. With this object at hand, the nonlinear optical response from single molecules and also from entire photonic devices can be computed, including the full tensorial and dispersive nature of the optical response of the molecules, as well as the optical interaction between different molecules as, for example, in the lattice of a molecular crystal. To demonstrate the applicability of the novel approach, the generation of a second‐harmonic signal from a thin film of an Urea molecular crystal is computed and compared to more traditional simulations. Furthermore, an optical cavity is designed, which enhances the second‐harmonic response of the molecular film up to more than two orders of magnitude. This approach is highly versatile and accurate and can be the working horse for the future exploration of nonlinear photonic molecular materials in structured photonic environments.

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Section: Introductionmentioning

confidence: 99%