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Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems

[Image: see text] Intensity-modulated photocurrent spectroscopy (IMPS) has been largely employed in semiconductor characterization for solar energy conversion devices to probe the operando behavior with widely available facilities. However, the implementation of IMPS data analysis to complex structu...

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Autores principales: Piccioni, Alberto, Vecchi, Pierpaolo, Vecchi, Lorenzo, Grandi, Silvia, Caramori, Stefano, Mazzaro, Raffaello, Pasquini, Luca
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10166235/
https://www.ncbi.nlm.nih.gov/pubmed/37181327
http://dx.doi.org/10.1021/acs.jpcc.3c00770
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author Piccioni, Alberto
Vecchi, Pierpaolo
Vecchi, Lorenzo
Grandi, Silvia
Caramori, Stefano
Mazzaro, Raffaello
Pasquini, Luca
author_facet Piccioni, Alberto
Vecchi, Pierpaolo
Vecchi, Lorenzo
Grandi, Silvia
Caramori, Stefano
Mazzaro, Raffaello
Pasquini, Luca
author_sort Piccioni, Alberto
collection PubMed
description [Image: see text] Intensity-modulated photocurrent spectroscopy (IMPS) has been largely employed in semiconductor characterization for solar energy conversion devices to probe the operando behavior with widely available facilities. However, the implementation of IMPS data analysis to complex structures, whether based on the physical rate constant model (RCM) or the assumption-free distribution of relaxation times (DRT), is generally limited to a semi-quantitative description of the charge carrier kinetics of the system. In this study, a new algorithm for the analysis of IMPS data is developed, providing unprecedented time resolution to the investigation of μs to s charge carrier dynamics in semiconductor-based systems used in photoelectrochemistry and photovoltaics. The algorithm, based on the previously developed DRT analysis, is herein modified with a Lasso regression method and available to the reader free of charge. A validation of this new algorithm is performed on a α-Fe(2)O(3) photoanode for photoelectrochemical water splitting, identified as a standard platform in the field, highlighting multiple potential-dependent charge transfer paths, otherwise hidden in the conventional IMPS data analysis.
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spelling pubmed-101662352023-05-09 Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems Piccioni, Alberto Vecchi, Pierpaolo Vecchi, Lorenzo Grandi, Silvia Caramori, Stefano Mazzaro, Raffaello Pasquini, Luca J Phys Chem C Nanomater Interfaces [Image: see text] Intensity-modulated photocurrent spectroscopy (IMPS) has been largely employed in semiconductor characterization for solar energy conversion devices to probe the operando behavior with widely available facilities. However, the implementation of IMPS data analysis to complex structures, whether based on the physical rate constant model (RCM) or the assumption-free distribution of relaxation times (DRT), is generally limited to a semi-quantitative description of the charge carrier kinetics of the system. In this study, a new algorithm for the analysis of IMPS data is developed, providing unprecedented time resolution to the investigation of μs to s charge carrier dynamics in semiconductor-based systems used in photoelectrochemistry and photovoltaics. The algorithm, based on the previously developed DRT analysis, is herein modified with a Lasso regression method and available to the reader free of charge. A validation of this new algorithm is performed on a α-Fe(2)O(3) photoanode for photoelectrochemical water splitting, identified as a standard platform in the field, highlighting multiple potential-dependent charge transfer paths, otherwise hidden in the conventional IMPS data analysis. American Chemical Society 2023-04-20 /pmc/articles/PMC10166235/ /pubmed/37181327 http://dx.doi.org/10.1021/acs.jpcc.3c00770 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Piccioni, Alberto
Vecchi, Pierpaolo
Vecchi, Lorenzo
Grandi, Silvia
Caramori, Stefano
Mazzaro, Raffaello
Pasquini, Luca
Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title_full Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title_fullStr Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title_full_unstemmed Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title_short Distribution of Relaxation Times Based on Lasso Regression: A Tool for High-Resolution Analysis of IMPS Data in Photoelectrochemical Systems
title_sort distribution of relaxation times based on lasso regression: a tool for high-resolution analysis of imps data in photoelectrochemical systems
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10166235/
https://www.ncbi.nlm.nih.gov/pubmed/37181327
http://dx.doi.org/10.1021/acs.jpcc.3c00770
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