Non-negatively constrained least squares and parameter choice by the residual periodogram for the inversion of electrochemical impedance spectroscopy data

Jakob K. Hansen, Jarom D. Hogue, Grant K. Sander, Rosemary Renaut, Sudeep C. Popat

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

The inverse problem associated with electrochemical impedance spectroscopy requiring the solution of a Fredholm integral equation of the first kind is considered. If the underlying physical model is not clearly determined, the inverse problem needs to be solved using a regularized linear least squares problem that is obtained from the discretization of the integral equation. For this system, it is shown that the model error can be made negligible by a change of variables and by extending the effective range of quadrature. This change of variables serves as a right preconditioner that significantly improves the condition of the system. Still, to obtain feasible solutions the additional constraint of non-negativity is required. Simulations with artificial, but realistic, data demonstrate that the use of non-negatively constrained least squares with a smoothing norm provides higher quality solutions than those obtained without the non-negative constraint. Using higher-order smoothing norms also reduces the error in the solutions. The L-curve and residual periodogram parameter choice criteria, which are used for parameter choice with regularized linear least squares, are successfully adapted to be used for the non-negatively constrained Tikhonov least squares problem. Although these results have been verified within the context of the analysis of electrochemical impedance spectroscopy, there is no reason to suppose that they would not be relevant within the broader framework of solving Fredholm integral equations for other applications.

Original languageEnglish (US)
Pages (from-to)52-74
Number of pages23
JournalJournal of Computational and Applied Mathematics
Volume278
DOIs
StatePublished - Apr 15 2015

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Constrained Least Squares
Periodogram
Linear Least Squares
Change of Variables
Least Squares Problem
Fredholm Integral Equation
Electrochemical impedance spectroscopy
Impedance
Smoothing
Spectroscopy
Inversion
Inverse Problem
L-curve
Integral equations
Norm
Model Error
Nonnegativity
Physical Model
Inverse problems
Quadrature

Keywords

  • Ill-posed
  • Inverse problem
  • Non-negative least squares
  • Regularization
  • Residual periodogram

ASJC Scopus subject areas

  • Computational Mathematics
  • Applied Mathematics

Cite this

Non-negatively constrained least squares and parameter choice by the residual periodogram for the inversion of electrochemical impedance spectroscopy data. / Hansen, Jakob K.; Hogue, Jarom D.; Sander, Grant K.; Renaut, Rosemary; Popat, Sudeep C.

In: Journal of Computational and Applied Mathematics, Vol. 278, 15.04.2015, p. 52-74.

Research output: Contribution to journalArticle

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