Size dependent optical response in coupled systems of plasmons and electron-hole pairs in metallic nanostructures

Masayuki Iio, Tomohiro Yokoyama, Takeshi Inaoka, Hajime Ishihara

Published 2023-12-18, updated 2023-12-21Version 2

In bulk materials, the collective modes and individual modes are orthogonal each other, and no connection occurs if there is no damping processes. In the presence of damping, the collective modes, i.e., plasmons decay into the hot carriers. In finite systems, the collective and individual modes are coupled by the Coulomb interaction. Such couplings by longitudinal (L) field have been intensively investigated, whereas a coupling via transverse (T) field has been poorly studied although the plasmon is excited by an irradiated light on surface and in finite nanostructures. Then, the T field would play a significant role in the coupling between the collective and individual excitations. In this study, we investigate how the T field mediates the coherent coupling. This study is based on the recently developed microscopic nonlocal theory of electronic systems in metals and the results of eigenmode analyses by this theory. To tune the coupling strength in a single nanorod, we examine three parameters: Rod length $L_z$, background refractive index $n_{\rm b}$, and Fermi energy $\varepsilon_{\rm F}$. We discuss the modulation ratio of the spectrum of optical response coefficients to evaluate the coupling by the T field. The T field shifts the collective excitation energy, which causes a finite modulation at both collective excitation and individual excitations. The three parameters can change the energy distance between the collective and individual excitations. Thus, the coherent coupling by the T field is enhanced for a proper tuning of the parameters. The results of the investigation of system parameter dependence would give insight into the guiding principle of designing the materials for highly efficient hot carrier generation.