ACS Publications. Most Trusted. Most Cited. Most Read
My Activity
CONTENT TYPES

Figure 1Loading Img

Increases in the Charge Separation Barrier in Organic Solar Cells Due to Delocalization

  • Adam Gluchowski
    Adam Gluchowski
    School of Mathematics and Physics and Centre for Engineered Quantum Systems, The University of Queensland, St. Lucia, QLD 4072, Australia
  • Katherine L. G. Gray
    Katherine L. G. Gray
    School of Mathematics and Physics and Centre for Engineered Quantum Systems, The University of Queensland, St. Lucia, QLD 4072, Australia
  • Samantha N. Hood
    Samantha N. Hood
    School of Mathematics and Physics and Centre for Engineered Quantum Systems, The University of Queensland, St. Lucia, QLD 4072, Australia
  • , and 
  • Ivan Kassal*
    Ivan Kassal
    School of Chemistry and the University of Sydney Nano Institute, The University of Sydney, Sydney, NSW 2006, Australia
    *E-mail: [email protected]
    More by Ivan Kassal
Cite this: J. Phys. Chem. Lett. 2018, 9, 6, 1359–1364
Publication Date (Web):March 1, 2018
https://doi.org/10.1021/acs.jpclett.8b00292
Copyright © 2018 American Chemical Society

    Article Views

    1079

    Altmetric

    -

    Citations

    LEARN ABOUT THESE METRICS
    Other access options

    Abstract

    Abstract Image

    Because of the low dielectric constant, charges in organic solar cells must overcome a strong Coulomb attraction in order to separate. It has been widely argued that intermolecular delocalization would assist charge separation by increasing the effective initial electron–hole separation in a charge-transfer state, thus decreasing their barrier to separation. Here we show that this is not the case: including more than a small amount of delocalization in models of organic solar cells leads to an increase in the free-energy barrier to charge separation. Therefore, if delocalization were to improve the charge separation efficiency, it would have to do so through nonequilibrium kinetic effects that are not captured by a thermodynamic treatment of the barrier height.

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. You can change your affiliated institution below.

    Cited By

    This article is cited by 17 publications.

    1. Waldemar Kaiser, Veljko Janković, Nenad Vukmirović, Alessio Gagliardi. Nonequilibrium Thermodynamics of Charge Separation in Organic Solar Cells. The Journal of Physical Chemistry Letters 2021, 12 (27) , 6389-6397. https://doi.org/10.1021/acs.jpclett.1c01817
    2. Meera Madhu, Remya Ramakrishnan, Vishnu Vijay, Mahesh Hariharan. Free Charge Carriers in Homo-Sorted π-Stacks of Donor–Acceptor Conjugates. Chemical Reviews 2021, 121 (13) , 8234-8284. https://doi.org/10.1021/acs.chemrev.1c00078
    3. Márcio T. do N. Varella, Ljiljana Stojanović, Van Quan Vuong, Stephan Irle, Thomas A. Niehaus, Mario Barbatti. How the Size and Density of Charge-Transfer Excitons Depend on Heterojunction’s Architecture. The Journal of Physical Chemistry C 2021, 125 (10) , 5458-5474. https://doi.org/10.1021/acs.jpcc.0c10762
    4. Chengqiang Lu, Qi Liu, Qiming Sun, Chang-Yu Hsieh, Shengyu Zhang, Liang Shi, Chee-Kong Lee. Deep Learning for Optoelectronic Properties of Organic Semiconductors. The Journal of Physical Chemistry C 2020, 124 (13) , 7048-7060. https://doi.org/10.1021/acs.jpcc.0c00329
    5. Stavros Athanasopoulos, Heinz Bässler, Anna Köhler. Disorder vs Delocalization: Which Is More Advantageous for High-Efficiency Organic Solar Cells?. The Journal of Physical Chemistry Letters 2019, 10 (22) , 7107-7112. https://doi.org/10.1021/acs.jpclett.9b02866
    6. Frank-Julian Kahle, Christina Saller, Selina Olthof, Cheng Li, Jenny Lebert, Sebastian Weiß, Eva M. Herzig, Sven Hüttner, Klaus Meerholz, Peter Strohriegl, Anna Köhler. Does Electron Delocalization Influence Charge Separation at Donor–Acceptor Interfaces in Organic Photovoltaic Cells?. The Journal of Physical Chemistry C 2018, 122 (38) , 21792-21802. https://doi.org/10.1021/acs.jpcc.8b06429
    7. Daniel Balzer, Ivan Kassal. Delocalisation enables efficient charge generation in organic photovoltaics, even with little to no energetic offset. Chemical Science 2024, 15 (13) , 4779-4789. https://doi.org/10.1039/D3SC05409H
    8. Marios Maimaris, Allan J. Pettipher, Mohammed Azzouzi, Daniel J. Walke, Xijia Zheng, Andrei Gorodetsky, Yifan Dong, Pabitra Shakya Tuladhar, Helder Crespo, Jenny Nelson, John W. G. Tisch, Artem A. Bakulin. Sub-10-fs observation of bound exciton formation in organic optoelectronic devices. Nature Communications 2022, 13 (1) https://doi.org/10.1038/s41467-022-32478-8
    9. Daniel Balzer, Ivan Kassal. Even a little delocalization produces large kinetic enhancements of charge-separation efficiency in organic photovoltaics. Science Advances 2022, 8 (32) https://doi.org/10.1126/sciadv.abl9692
    10. Yangjun Yan, Yajie Zhang, Waqar Ali Memon, Mengni Wang, Xinghua Zhang, Zhixiang Wei. The Role of Entropy Gains in the Exciton Separation in Organic Solar Cells. Macromolecular Rapid Communications 2022, 43 (16) https://doi.org/10.1002/marc.202100903
    11. Francesco Campaioli, Jared H Cole. Exciton transport in amorphous polymers and the role of morphology and thermalisation. New Journal of Physics 2021, 23 (11) , 113038. https://doi.org/10.1088/1367-2630/ac37c7
    12. Daniel Balzer, Thijs J. A. M. Smolders, David Blyth, Samantha N. Hood, Ivan Kassal. Delocalised kinetic Monte Carlo for simulating delocalisation-enhanced charge and exciton transport in disordered materials. Chemical Science 2021, 12 (6) , 2276-2285. https://doi.org/10.1039/D0SC04116E
    13. Sebastian Wilken. Charge Recombination in Organic Solar Cells. 2020, 5-1-5-32. https://doi.org/10.1063/9780735422414_005
    14. Hyojung Cha, Yizhen Zheng, Yifan Dong, Hyun Hwi Lee, Jiaying Wu, Helen Bristow, Jiangbin Zhang, Harrison Ka Hin Lee, Wing C. Tsoi, Artem A. Bakulin, Iain McCulloch, James R. Durrant. Exciton and Charge Carrier Dynamics in Highly Crystalline PTQ10:IDIC Organic Solar Cells. Advanced Energy Materials 2020, 10 (38) https://doi.org/10.1002/aenm.202001149
    15. Lifeng Zheng, Yang Meng, Xiangqian Wang, Chun Zhu, Jin-Xia Liang. Screening metal-dicorrole-based dyes with excellent photoelectronic properties for dye-sensitized solar cells by density functional calculations. Journal of Porphyrins and Phthalocyanines 2020, 24 (08) , 1003-1012. https://doi.org/10.1142/S1088424620500145
    16. Jens Wehner, Björn Baumeier. Multiscale simulations of singlet and triplet exciton dynamics in energetically disordered molecular systems based on many-body Green's functions theory. New Journal of Physics 2020, 22 (3) , 033033. https://doi.org/10.1088/1367-2630/ab7a04
    17. Veaceslav Coropceanu, Xian-Kai Chen, Tonghui Wang, Zilong Zheng, Jean-Luc Brédas. Charge-transfer electronic states in organic solar cells. Nature Reviews Materials 2019, 4 (11) , 689-707. https://doi.org/10.1038/s41578-019-0137-9

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    You’ve supercharged your research process with ACS and Mendeley!

    STEP 1:
    Click to create an ACS ID

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    MENDELEY PAIRING EXPIRED
    Your Mendeley pairing has expired. Please reconnect