Ab initio uncertainty quantification in scattering analysis of microscopy

Abstract

Estimating parameters from data is a fundamental problem, customarily done by minimizing a loss function between a model and observed statistics. In scattering-based analysis, researchers often employ their domain expertise to select a specific range of wave vectors for analysis, a choice that can vary depending on the specific case. We introduce another paradigm that defines a probabilistic generative model from the beginning of data processing and propagates the uncertainty for parameter estimation, termed the ab initio uncertainty quantification (AIUQ). As an illustrative example, we demonstrate this approach with differential dynamic microscopy (DDM) that extracts dynamical information through Fourier analysis at a selected range of wave vectors. We first show that the conventional way of estimation in DDM is equivalent to fitting a temporal variogram in the reciprocal space using a latent factor model. Then we derive the maximum marginal likelihood estimator, which optimally weighs the information at all wave vectors, therefore eliminating the need to select the range of wave vectors. Furthermore, we substantially reduce the computational cost by utilizing the generalized Schur algorithm for Toeplitz covariances without approximation. Simulated studies validate that AIUQ improves estimation accuracy and enables model selection with automated analysis. The utility of AIUQ is also demonstrated by three distinct sets of experiments: first in an isotropic Newtonian fluid, pushing limits of optically dense systems compared to multiple particle tracking; next in a system undergoing a sol-gel transition, automating the determination of gelling points and critical exponent; and lastly, in discerning anisotropic diffusive behavior of colloids in a liquid crystal. These outcomes collectively underscore AIUQ's versatility to capture system dynamics in an efficient and automated manner.

23 pages, 9 figures

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