Abstract

Characterization of nanoparticle aggregates from observed scattered light leads to a highly complex inverse problem. Even the forward model is so complex that it prohibits the use of classical likelihood-based inference methods. In this study, we compare four so-called likelihood-free methods based on approximate Bayesian computation (ABC) that requires only numeric simulation of the forward model without the need of evaluating a likelihood. In particular, rejection, Markov chain Monte Carlo, population Monte Carlo, and adaptive population Monte Carlo (APMC) are compared in terms of accuracy. In the current model, we assume that the nanoparticle aggregates are mutually well separated and made up of particles of same size. Filippov’s particle-cluster algorithm is used to generate aggregates, and discrete dipole approximation is used to estimate scattering behavior. It is found that the APMC algorithm is superior to others in terms of time and acceptance rates, although all algorithms produce similar posterior distributions. Using ABC techniques and utilizing unpolarized light experiments at 266 nm wavelength, characterization of soot aggregates is performed with less than 2 nm deviation in nanoparticle radius and 3–4 deviation in number of nanoparticles forming the monodisperse aggregates. Promising results are also observed for the polydisperse aggregate with log-normal particle size distribution.

© 2017 Optical Society of America

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