Quantifying noise effects in optical measures of excited state transport.

Abstract

Time-resolved microscopy is a widely used approach for imaging and quantifying charge and energy transport in functional materials. While it is generally recognized that resolving small diffusion lengths is limited by measurement noise, the impacts of noise have not been systematically assessed or quantified. This article reports modeling efforts to elucidate the impact of noise on optical probes of transport. Excited state population distributions, modeled as Gaussians with additive white noise typical of experimental conditions, are subject to decay and diffusive evolution. Using a conventional composite least-squares fitting algorithm, the resulting diffusion constant estimates are compared with the model input parameter. The results show that heteroscedasticity (i.e., time-varying noise levels), insufficient spatial and/or temporal resolution, and small diffusion lengths relative to the magnitude of noise lead to a surprising degree of imprecision under moderate experimental parameters. Moreover, the compounding influence of low initial contrast and small diffusion length leads to systematic overestimation of diffusion coefficients. Each of these issues is quantitatively analyzed herein, and experimental approaches to mitigate them are proposed. General guidelines for experimentalists to rapidly assess measurement precision are provided, as is an open-source tool for customizable evaluation of noise effects on time-resolved microscopy transport measurements.