The probabilistic deconvolution of the distribution of relaxation times with finite Gaussian processes

Abstract

Electrochemical impedance spectroscopy (EIS) is a tool widely used to study the properties of electrochemical systems. The distribution of relaxation times (DRT) has emerged as one of the main methods for the analysis of EIS spectra. Gaussian processes can be used to regress EIS data, quantify uncertainty, and deconvolve the DRT. However, previously developed DRT models based on Gaussian processes do not constrain the DRT to be non-negative and can only use the imaginary part of EIS spectra. Herein, we overcome both issues by using a finite Gaussian process approximation to develop a new framework called the finite Gaussian process distribution of relaxation times (fGP-DRT). The analysis on artificial EIS data shows that the fGP-DRT method consistently recovers exact DRT from noise-corrupted EIS spectra while accurately regressing experimental data. Furthermore, the fGP-DRT framework is used as a machine learning tool to provide probabilistic estimates of the impedance at unmeasured frequencies. The method is further validated against experimental data from fuel cells and batteries. In short, this work develops a novel probabilistic approach for the analysis of EIS data based on Gaussian process, opening a new stream of research for the deconvolution of DRT.