Approximate T-matrix and optical properties of spheroidal particles to third order in size parameter

TL;DR

This paper derives a third-order size parameter expansion of the T-matrix for spheroidal particles, enabling efficient optical property calculations beyond Rayleigh limits with validated accuracy up to 200nm particles at 400nm wavelength.

Contribution

It introduces a third-order Taylor expansion of the T-matrix for spheroids, including radiative corrections, providing a computationally efficient alternative to exact methods.

Findings

Valid within 1% error for particles up to 200nm at 400nm wavelength.

Expansion includes multipoles up to octupoles (order 3).

Provides simple formulas for orientation-averaged optical cross-sections.

Abstract

We here calculate the series expansion of the T-matrix for a spheroidal particle in the small-size/long-wavelength limit, up to third lowest order with respect to the size parameter, X, which we will define rigorously for a non-spherical particle. T is calculated from the standard extended boundary condition method with a linear system involving two infinite matrices P and Q, whose matrix elements are integrals on the particle surface. We show that the limiting form of the P- and Q-matrices, which is different in the special case of spheroid, ensures that this Taylor expansion can be obtained by considering only multipoles of order 3 or less (i.e. dipoles, quadrupoles, and octupoles). This allows us to obtain self-contained expressions for the Taylor expansion of T(X). The lowest order is O(X^3) and equivalent to the quasi-static limit or Rayleigh approximation. Expressions to order O(X^5) are obtained by Taylor expansion of the integrals in P and Q followed by matrix inversion. We then apply a radiative correction scheme, which makes the resulting expressions valid up to order O(X^6). Orientation-averaged extinction, scattering, and absorption cross-sections are then derived. All results are compared to the exact T-matrix predictions to confirm the validity of our expressions and assess their range of applicability. For a wavelength of 400nm, the new approximation remains valid (within 1% error) up to particle dimensions of the order of 100-200nm depending on the exact parameters (aspect ratio and material). These results provide a relatively simple and computationally-friendly alternative to the standard T-matrix method for spheroidal particles smaller than the wavelength, in a size range much larger than for the commonly-used Rayleigh approximation.