Quantum mechanical analysis of nonlinear optical response of interacting graphene nanoflakes

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Abstract

We propose a distant-neighbor quantum-mechanical (DNQM) approach to study the linear and nonlinear optical properties of graphene nanoflakes (GNFs). In contrast to the widely used tight-binding description of the electronic states that considers only the nearest-neighbor coupling between the atoms, our approach is more accurate and general, as it captures the electron-core interactions between all atoms in the structure. Therefore, as we demonstrate, the DNQM approach enables the investigation of the optical coupling between two closely separated but chemically unbound GNFs. We also find that the optical response of GNFs depends crucially on their shape, size, and symmetry properties. Specifically, increasing the size of nanoflakes is found to shift their accommodated quantum plasmon oscillations to lower frequency. Importantly, we show that by embedding a cavity into GNFs, one can change their symmetry properties, tune their optical properties, or enable otherwise forbidden second-harmonic generation processes.

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Deng, H., Manrique, D. Z., Chen, X., Panoiu, N. C., & Ye, F. (2018). Quantum mechanical analysis of nonlinear optical response of interacting graphene nanoflakes. APL Photonics, 3(1). https://doi.org/10.1063/1.5009600

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