Analytical theory for three wave-mixing processes in a slightly deformed cylinder

TL;DR

This paper develops an analytical theory to understand the second order optical response of slightly deformed noncentrosymmetric cylinders made of centrosymmetric materials, revealing complex resonant behaviors and contributions from multiple multipolar sources.

Contribution

It introduces a perturbative analytical framework for the nonlinear optical response of deformed cylindrical nanoparticles, highlighting the interplay of various multipolar contributions.

Findings

Strong competition between dipolar and quadrupolar contributions.

Resonant features in the nonlinear response functions.

Deformation influences the efficiency of quadratic optical processes.

Abstract

The second order optical response of centrosymmetric materials manifests itself mostly at their surface, being strongly suppressed in their bulk. However, the overall surface response is also suppressed in nanoparticles with a centrosymmetric geometry subjected to homogeneous fields. Nevertheless, nanoparticles with a noncentrosymmetric geometry do exhibit second order optical properties. We develop an analytical theory to investigate the second order optical response of a noncentrosymmetric thin cylinder with a slightly deformed cross-section made up of a centrosymmetric material subjected to two monochromatic fields. We calculate the linear and nonlinear near fields perturbatively using the extent of the deformation away from a circular cross-section as the perturbation parameter. We obtain expressions for the quadratic hyperpolarizabilities in terms of the linear response evaluated at the three frequencies involved. We analyze the spectral features of the nonlinear response functions and explore their resonant structure for a model dielectric cylinder. Furthermore, we evaluate the second order radiated fields, the radiation patterns and efficiency of the different quadratic processes. We obtain a strong competition between electric dipolar, magnetic dipolar and electric quadrupolar contributions even for very small deformations.