$\mathcal{T}$-matrix method for computation of second-harmonic generation upon optical wave scattering from clusters of arbitrary particles: Application to nonlinear optical interaction of bound states in the continuum

TL;DR

This paper introduces a versatile and efficient $ ext{T}$-matrix formalism for calculating second-harmonic generation in arbitrarily shaped particle clusters, accounting for complex nonlinear sources and material dispersion.

Contribution

The authors develop a novel $ ext{T}$-matrix approach that handles nonlinear optical scattering from arbitrary particle shapes and compositions, including bulk and surface nonlinearities.

Findings

Method is faster and more memory-efficient than existing techniques.

Applicable to particles of arbitrary shape and material dispersion.

Enables analysis of nonlinear optical interactions in complex particle clusters.

Abstract

We derive the $\mathcal{T}$-matrix formalism tailored for numerical analysis of second-harmonic (SH) generation from arbitrarily shaped particles made of centrosymmetric optical materials. First, the transfer matrix of a single particle is computed via the extended boundary condition method, in which the electromagnetic fields both at fundamental frequency and SH are expanded in vector spherical wave functions, and the integral formulation is satisfied away from the surface of the scatterer. We allow for the accurate physical description of the SH sources by taking into account both local surface and nonlocal bulk polarization contributions to the nonlinear polarization density source responsible for the generation of the SH signal by a particle. This single-particle formalism is then extended to arbitrary distributions of particles by incorporating into the formalism linear and nonlinear electromagnetic wave scattering from the particles in the cluster. Importantly from a practical point of view, our method can be applied to particles of arbitrary shape made of optical materials characterized by general frequency-dispersion relations, so that it can describe the linear and nonlinear optical response of clusters of metallic, semiconductor, or polaritonic particles, as well as mixtures of such particles. The approach proposed here is faster and more memory-efficient than well-established numerical techniques, especially in the analysis of spheroidal particles, due to the favorable symmetries of spherical wave basis functions used in the wave scattering analysis.