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Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited

Elisa Collado-Fregoso, Samantha N. Hood, Safa Shoaee, Bob C. Schroeder, Iain McCulloch, Ivan Kassal, Dieter Neher, James Durrant Orcid Logo

The Journal of Physical Chemistry Letters, Volume: 8, Issue: 17, Pages: 4061 - 4068

Swansea University Author: James Durrant Orcid Logo

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Abstract

In this Letter, we study the role of the donor:acceptor interface nanostructure upon charge separation and recombination in organic photovoltaic devices and blend films, using mixtures of PBTTT and two different fullerene derivatives (PC70BM and ICTA) as models for intercalated and nonintercalated m...

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Published in: The Journal of Physical Chemistry Letters
ISSN: 1948-7185
Published: 2017
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URI: https://cronfa.swan.ac.uk/Record/cronfa35633
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spelling 2017-10-09T10:24:05.0044001 v2 35633 2017-09-25 Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2017-09-25 MTLS In this Letter, we study the role of the donor:acceptor interface nanostructure upon charge separation and recombination in organic photovoltaic devices and blend films, using mixtures of PBTTT and two different fullerene derivatives (PC70BM and ICTA) as models for intercalated and nonintercalated morphologies, respectively. Thermodynamic simulations show that while the completely intercalated system exhibits a large free-energy barrier for charge separation, this barrier is significantly lower in the nonintercalated system and almost vanishes when energetic disorder is included in the model. Despite these differences, both femtosecond-resolved transient absorption spectroscopy (TAS) and time-delayed collection field (TDCF) exhibit extensive first-order losses in both systems, suggesting that geminate pairs are the primary product of photoexcitation. In contrast, the system that comprises a combination of fully intercalated polymer:fullerene areas and fullerene-aggregated domains (1:4 PBTTT:PC70BM) is the only one that shows slow, second-order recombination of free charges, resulting in devices with an overall higher short-circuit current and fill factor. This study therefore provides a novel consideration of the role of the interfacial nanostructure and the nature of bound charges and their impact upon charge generation and recombination. Journal Article The Journal of Physical Chemistry Letters 8 17 4061 4068 1948-7185 31 12 2017 2017-12-31 10.1021/acs.jpclett.7b01571 https://spiral.imperial.ac.uk:8443/handle/10044/1/51582 COLLEGE NANME Materials Science and Engineering COLLEGE CODE MTLS Swansea University 2017-10-09T10:24:05.0044001 2017-09-25T14:26:01.7884661 College of Engineering Engineering Elisa Collado-Fregoso 1 Samantha N. Hood 2 Safa Shoaee 3 Bob C. Schroeder 4 Iain McCulloch 5 Ivan Kassal 6 Dieter Neher 7 James Durrant 0000-0001-8353-7345 8
title Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
spellingShingle Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
James Durrant
title_short Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
title_full Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
title_fullStr Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
title_full_unstemmed Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
title_sort Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Elisa Collado-Fregoso
Samantha N. Hood
Safa Shoaee
Bob C. Schroeder
Iain McCulloch
Ivan Kassal
Dieter Neher
James Durrant
format Journal article
container_title The Journal of Physical Chemistry Letters
container_volume 8
container_issue 17
container_start_page 4061
publishDate 2017
institution Swansea University
issn 1948-7185
doi_str_mv 10.1021/acs.jpclett.7b01571
college_str College of Engineering
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hierarchy_top_id collegeofengineering
hierarchy_top_title College of Engineering
hierarchy_parent_id collegeofengineering
hierarchy_parent_title College of Engineering
department_str Engineering{{{_:::_}}}College of Engineering{{{_:::_}}}Engineering
url https://spiral.imperial.ac.uk:8443/handle/10044/1/51582
document_store_str 0
active_str 0
description In this Letter, we study the role of the donor:acceptor interface nanostructure upon charge separation and recombination in organic photovoltaic devices and blend films, using mixtures of PBTTT and two different fullerene derivatives (PC70BM and ICTA) as models for intercalated and nonintercalated morphologies, respectively. Thermodynamic simulations show that while the completely intercalated system exhibits a large free-energy barrier for charge separation, this barrier is significantly lower in the nonintercalated system and almost vanishes when energetic disorder is included in the model. Despite these differences, both femtosecond-resolved transient absorption spectroscopy (TAS) and time-delayed collection field (TDCF) exhibit extensive first-order losses in both systems, suggesting that geminate pairs are the primary product of photoexcitation. In contrast, the system that comprises a combination of fully intercalated polymer:fullerene areas and fullerene-aggregated domains (1:4 PBTTT:PC70BM) is the only one that shows slow, second-order recombination of free charges, resulting in devices with an overall higher short-circuit current and fill factor. This study therefore provides a novel consideration of the role of the interfacial nanostructure and the nature of bound charges and their impact upon charge generation and recombination.
published_date 2017-12-31T03:56:56Z
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