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Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency

Ardalan Armin Orcid Logo, Nasim Zarrabi, Oskar Sandberg Orcid Logo, Christina Kaiser, Stefan Zeiske, Wei Li, Paul Meredith Orcid Logo

Advanced Energy Materials, Volume: 10, Issue: 41, Start page: 2001828

Swansea University Authors: Ardalan Armin Orcid Logo, Oskar Sandberg Orcid Logo, Paul Meredith Orcid Logo

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DOI (Published version): 10.1002/aenm.202001828

Abstract

Free carrier photogeneration in bulk‐heterojunction solar cells composed of blends of acceptor and donor organic semiconductors proceeds via intermolecular charge transfer (CT) states. Non‐adiabatic Marcus theory has proven valid to explain the absorption and emission of these sub‐gap states which h...

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Published in: Advanced Energy Materials
ISSN: 1614-6832 1614-6840
Published: Wiley 2020
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spelling 2021-08-29T14:58:33.6371355 v2 55526 2020-10-27 Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency 22b270622d739d81e131bec7a819e2fd 0000-0002-6129-5354 Ardalan Armin Ardalan Armin true false 9e91512a54d5aee66cd77851a96ba747 0000-0003-3778-8746 Oskar Sandberg Oskar Sandberg true false 31e8fe57fa180d418afd48c3af280c2e 0000-0002-9049-7414 Paul Meredith Paul Meredith true false 2020-10-27 SPH Free carrier photogeneration in bulk‐heterojunction solar cells composed of blends of acceptor and donor organic semiconductors proceeds via intermolecular charge transfer (CT) states. Non‐adiabatic Marcus theory has proven valid to explain the absorption and emission of these sub‐gap states which have extremely weak emission probabilities and absorption cross sections making them difficult to probe directly using optical spectroscopy. Therefore, the CT state parameters involved in the Marcus model are often extracted from fittings on the photovoltaic external quantum efficiency (EQEPV) and electroluminescence. These two spectra are (ideally) interrelated via the so‐called reciprocity principle. In this paper, the limitations of such an approach are demonstrated, in particular the impact of simple low finesse cavity interference effects acting as an uneven spectral filter for emission and absorption. This can produce almost spurious CT state parameterization with, for example, relative errors as large as 90% in absorption coefficients obtained from EQEPV. It is shown how these limitations can be partially lifted using an iterative transfer matrix approach applied to the EQEPV. Journal Article Advanced Energy Materials 10 41 2001828 Wiley 1614-6832 1614-6840 charge transfer states; electroluminescence; external quantum efficiency; organic photovoltaics; reciprocity principle 3 11 2020 2020-11-03 10.1002/aenm.202001828 COLLEGE NANME Physics COLLEGE CODE SPH Swansea University EPSRC, WEFO EP/N020863/1, SER Cymru II 2021-08-29T14:58:33.6371355 2020-10-27T10:19:41.2643981 Faculty of Science and Engineering School of Biosciences, Geography and Physics - Physics Ardalan Armin 0000-0002-6129-5354 1 Nasim Zarrabi 2 Oskar Sandberg 0000-0003-3778-8746 3 Christina Kaiser 4 Stefan Zeiske 5 Wei Li 6 Paul Meredith 0000-0002-9049-7414 7 55526__18506__a4aaaa5b2b0843149cc2ccc722aa6684.pdf aenm.202001828.pdf 2020-10-27T10:21:44.1283217 Output 2918037 application/pdf Version of Record true © 2020 The Authors. Published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License true eng http://creativecommons.org/licenses/by/4.0/
title Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
spellingShingle Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
Ardalan Armin
Oskar Sandberg
Paul Meredith
title_short Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
title_full Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
title_fullStr Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
title_full_unstemmed Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
title_sort Limitations of Charge Transfer State Parameterization Using Photovoltaic External Quantum Efficiency
author_id_str_mv 22b270622d739d81e131bec7a819e2fd
9e91512a54d5aee66cd77851a96ba747
31e8fe57fa180d418afd48c3af280c2e
author_id_fullname_str_mv 22b270622d739d81e131bec7a819e2fd_***_Ardalan Armin
9e91512a54d5aee66cd77851a96ba747_***_Oskar Sandberg
31e8fe57fa180d418afd48c3af280c2e_***_Paul Meredith
author Ardalan Armin
Oskar Sandberg
Paul Meredith
author2 Ardalan Armin
Nasim Zarrabi
Oskar Sandberg
Christina Kaiser
Stefan Zeiske
Wei Li
Paul Meredith
format Journal article
container_title Advanced Energy Materials
container_volume 10
container_issue 41
container_start_page 2001828
publishDate 2020
institution Swansea University
issn 1614-6832
1614-6840
doi_str_mv 10.1002/aenm.202001828
publisher Wiley
college_str Faculty of Science and Engineering
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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
document_store_str 1
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description Free carrier photogeneration in bulk‐heterojunction solar cells composed of blends of acceptor and donor organic semiconductors proceeds via intermolecular charge transfer (CT) states. Non‐adiabatic Marcus theory has proven valid to explain the absorption and emission of these sub‐gap states which have extremely weak emission probabilities and absorption cross sections making them difficult to probe directly using optical spectroscopy. Therefore, the CT state parameters involved in the Marcus model are often extracted from fittings on the photovoltaic external quantum efficiency (EQEPV) and electroluminescence. These two spectra are (ideally) interrelated via the so‐called reciprocity principle. In this paper, the limitations of such an approach are demonstrated, in particular the impact of simple low finesse cavity interference effects acting as an uneven spectral filter for emission and absorption. This can produce almost spurious CT state parameterization with, for example, relative errors as large as 90% in absorption coefficients obtained from EQEPV. It is shown how these limitations can be partially lifted using an iterative transfer matrix approach applied to the EQEPV.
published_date 2020-11-03T04:09:48Z
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