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A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors

Austin Kay, DREW RILEY, Paul Meredith Orcid Logo, Ardalan Armin, Oskar Sandberg Orcid Logo

The Journal of Physical Chemistry Letters, Volume: 15, Issue: 16, Pages: 4416 - 4421

Swansea University Authors: Austin Kay, DREW RILEY, Paul Meredith Orcid Logo, Ardalan Armin, Oskar Sandberg Orcid Logo

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DOI (Published version): 10.1021/acs.jpclett.4c00218

Abstract

Recombination of free charges is a key loss mechanism limiting the performance of organic semiconductor-based photovoltaics such as solar cells and photodetectors. The carrier density-dependence of the rate of recombination and the associated rate coefficients are often estimated using transient cha...

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Published in: The Journal of Physical Chemistry Letters
ISSN: 1948-7185 1948-7185
Published: American Chemical Society (ACS) 2024
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URI: https://cronfa.swan.ac.uk/Record/cronfa66033
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The carrier density-dependence of the rate of recombination and the associated rate coefficients are often estimated using transient charge extraction (CE) experiments. These experiments, however, often neglect the effect of recombination during the transient extraction process. In this work, the validity of the CE experiment for low-mobility devices, such as organic semiconductor-based photovoltaics, is investigated using transient drift-diffusion simulations. We find that recombination leads to incomplete CE, resulting in carrier density-dependent recombination rate constants and overestimated recombination orders; an effect that depends on both the charge carrier mobilities and the resistance–capacitance time constant. 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spelling v2 66033 2024-04-11 A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors 0d9126cbd038113f697c252762b4f053 Austin Kay Austin Kay true false 341d608c40b518bfe3c715d6687175ed DREW RILEY DREW RILEY true false 31e8fe57fa180d418afd48c3af280c2e 0000-0002-9049-7414 Paul Meredith Paul Meredith true false 22b270622d739d81e131bec7a819e2fd Ardalan Armin Ardalan Armin true false 9e91512a54d5aee66cd77851a96ba747 0000-0003-3778-8746 Oskar Sandberg Oskar Sandberg true false 2024-04-11 BGPS Recombination of free charges is a key loss mechanism limiting the performance of organic semiconductor-based photovoltaics such as solar cells and photodetectors. The carrier density-dependence of the rate of recombination and the associated rate coefficients are often estimated using transient charge extraction (CE) experiments. These experiments, however, often neglect the effect of recombination during the transient extraction process. In this work, the validity of the CE experiment for low-mobility devices, such as organic semiconductor-based photovoltaics, is investigated using transient drift-diffusion simulations. We find that recombination leads to incomplete CE, resulting in carrier density-dependent recombination rate constants and overestimated recombination orders; an effect that depends on both the charge carrier mobilities and the resistance–capacitance time constant. To overcome this intrinsic limitation of the CE experiment, we present an analytical model that accounts for charge carrier recombination, validate it using numerical simulations, and employ it to correct the carrier density-dependence observed in experimentally determined bimolecular recombination rate constants. Journal Article The Journal of Physical Chemistry Letters 15 16 4416 4421 American Chemical Society (ACS) 1948-7185 1948-7185 Carrier dynamics, Electrical properties, Kinetic parameters, Light, Recombination 25 4 2024 2024-04-25 10.1021/acs.jpclett.4c00218 COLLEGE NANME Biosciences Geography and Physics School COLLEGE CODE BGPS Swansea University SU Library paid the OA fee (TA Institutional Deal) Research Council of Finland - 357196; Engineering and Physical Sciences Research Council - EP/T028513/1; Llywodraeth Cymru; European Regional Development Fund; Research England; Swansea University 2024-05-31T12:19:05.4416064 2024-04-11T10:47:12.4601579 Faculty of Science and Engineering School of Biosciences, Geography and Physics - Physics Austin Kay 1 DREW RILEY 2 Paul Meredith 0000-0002-9049-7414 3 Ardalan Armin 4 Oskar Sandberg 0000-0003-3778-8746 5 66033__30414__e2ef7a5215164fd0ab36671bdd813d7c.pdf 66033.VOR.pdf 2024-05-20T16:49:00.6271941 Output 1951408 application/pdf Version of Record true This publication is licensed under a Creative Commons Attribution CC-BY 4.0 Licence. true eng https://creativecommons.org/licenses/by/4.0/
title A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
spellingShingle A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
Austin Kay
DREW RILEY
Paul Meredith
Ardalan Armin
Oskar Sandberg
title_short A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
title_full A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
title_fullStr A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
title_full_unstemmed A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
title_sort A New Framework for Understanding Recombination-Limited Charge Extraction in Disordered Semiconductors
author_id_str_mv 0d9126cbd038113f697c252762b4f053
341d608c40b518bfe3c715d6687175ed
31e8fe57fa180d418afd48c3af280c2e
22b270622d739d81e131bec7a819e2fd
9e91512a54d5aee66cd77851a96ba747
author_id_fullname_str_mv 0d9126cbd038113f697c252762b4f053_***_Austin Kay
341d608c40b518bfe3c715d6687175ed_***_DREW RILEY
31e8fe57fa180d418afd48c3af280c2e_***_Paul Meredith
22b270622d739d81e131bec7a819e2fd_***_Ardalan Armin
9e91512a54d5aee66cd77851a96ba747_***_Oskar Sandberg
author Austin Kay
DREW RILEY
Paul Meredith
Ardalan Armin
Oskar Sandberg
author2 Austin Kay
DREW RILEY
Paul Meredith
Ardalan Armin
Oskar Sandberg
format Journal article
container_title The Journal of Physical Chemistry Letters
container_volume 15
container_issue 16
container_start_page 4416
publishDate 2024
institution Swansea University
issn 1948-7185
1948-7185
doi_str_mv 10.1021/acs.jpclett.4c00218
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
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hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Biosciences, Geography and Physics - Physics{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Biosciences, Geography and Physics - Physics
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description Recombination of free charges is a key loss mechanism limiting the performance of organic semiconductor-based photovoltaics such as solar cells and photodetectors. The carrier density-dependence of the rate of recombination and the associated rate coefficients are often estimated using transient charge extraction (CE) experiments. These experiments, however, often neglect the effect of recombination during the transient extraction process. In this work, the validity of the CE experiment for low-mobility devices, such as organic semiconductor-based photovoltaics, is investigated using transient drift-diffusion simulations. We find that recombination leads to incomplete CE, resulting in carrier density-dependent recombination rate constants and overestimated recombination orders; an effect that depends on both the charge carrier mobilities and the resistance–capacitance time constant. To overcome this intrinsic limitation of the CE experiment, we present an analytical model that accounts for charge carrier recombination, validate it using numerical simulations, and employ it to correct the carrier density-dependence observed in experimentally determined bimolecular recombination rate constants.
published_date 2024-04-25T12:19:04Z
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score 11.013731

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