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

Figure 1Loading Img

Tuning Spin Dynamics in Crystalline Tetracene

  • Sam L. Bayliss
    Sam L. Bayliss
    Berlin Joint EPR Lab, Fachbereich Physik, Freie Universität Berlin, D-14195 Berlin, Germany
  • Felix Kraffert
    Felix Kraffert
    Berlin Joint EPR Lab, Fachbereich Physik, Freie Universität Berlin, D-14195 Berlin, Germany
  • Rui Wang
    Rui Wang
    National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China
    More by Rui Wang
  • Chunfeng Zhang
    Chunfeng Zhang
    National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China
    Synergetic Innovation Center in Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
  • Robert Bittl
    Robert Bittl
    Berlin Joint EPR Lab, Fachbereich Physik, Freie Universität Berlin, D-14195 Berlin, Germany
    More by Robert Bittl
  • , and 
  • Jan Behrends*
    Jan Behrends
    Berlin Joint EPR Lab, Fachbereich Physik, Freie Universität Berlin, D-14195 Berlin, Germany
    *E-mail: [email protected]
    More by Jan Behrends
Cite this: J. Phys. Chem. Lett. 2019, 10, 8, 1908–1913
Publication Date (Web):April 2, 2019
https://doi.org/10.1021/acs.jpclett.9b00356
Copyright © 2019 American Chemical Society

    Article Views

    1871

    Altmetric

    -

    Citations

    LEARN ABOUT THESE METRICS
    Other access options
    Supporting Info (1)»

    Abstract

    Abstract Image

    Tetracene is an archetypal material undergoing singlet fission—the generation of a pair of triplet excitons from one singlet exciton. Here, using time-resolved electron spin resonance, we show how the spin dynamics in tetracene crystals are influenced by temperature and morphology. Upon cooling from 300 to 200 K, we observe a switch between singlet fission and intersystem crossing generated triplets, manifesting as an inversion in transient spin polarization. We extract a spin dephasing time of approximately 40 ns for fission-generated triplets at room temperature, nearly 100 times shorter than the dephasing time that we measure for triplets localized on isolated tetracene molecules. These results highlight the importance of morphology and thermal activation in singlet fission systems.

    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.

    Supporting Information

    ARTICLE SECTIONS
    Jump To

    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.9b00356.

    • Methods, assignment of spin polarization, fluence dependence, kinetics comparison at 200 and 300 K, trESR kinetic simulations, comparison with cw experiments, additional tetracene in para-terphenyl data, and orientation-dependent line widths (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 15 publications.

    1. Daniel Vong, Farahnaz Maleki, Eric C. Novak, Luke L. Daemen, Adam J. Moulé. Measuring Intermolecular Excited State Geometry for Favorable Singlet Fission in Tetracene. The Journal of Physical Chemistry Letters 2024, 15 (5) , 1188-1194. https://doi.org/10.1021/acs.jpclett.3c02343
    2. Jonathan R. Palmer, Malik L. Williams, Ryan M. Young, Kathryn R. Peinkofer, Brian T. Phelan, Matthew D. Krzyaniak, Michael R. Wasielewski. Oriented Triplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular Donor–Acceptor Single Cocrystal. Journal of the American Chemical Society 2024, 146 (1) , 1089-1099. https://doi.org/10.1021/jacs.3c12277
    3. Kanad Majumder, Soham Mukherjee, Naitik A. Panjwani, Jieun Lee, Robert Bittl, Woojae Kim, Satish Patil, Andrew J. Musser. Controlling Intramolecular Singlet Fission Dynamics via Torsional Modulation of Through-Bond versus Through-Space Couplings. Journal of the American Chemical Society 2023, 145 (38) , 20883-20896. https://doi.org/10.1021/jacs.3c06075
    4. Max Attwood, Xiaotian Xu, Michael Newns, Zhu Meng, Rebecca A. Ingle, Hao Wu, Xi Chen, Weidong Xu, Wern Ng, Temitope T. Abiola, Vasilios G. Stavros, Mark Oxborrow. N-Heteroacenes as an Organic Gain Medium for Room-Temperature Masers. Chemistry of Materials 2023, 35 (11) , 4498-4509. https://doi.org/10.1021/acs.chemmater.3c00640
    5. Yusuke Wakikawa, Tadaaki Ikoma. Radio-wave Effect on Singlet Fission in Polycrystalline Tetracene near Zero Magnetic Field. The Journal of Physical Chemistry Letters 2023, 14 (16) , 3907-3911. https://doi.org/10.1021/acs.jpclett.3c00341
    6. Chenjian Lin, Yue Qi, Paige J. Brown, Malik L. Williams, Jonathan R. Palmer, Michele Myong, Xingang Zhao, Ryan M. Young, Michael R. Wasielewski. Singlet Fission in Perylene Monoimide Single Crystals and Polycrystalline Films. The Journal of Physical Chemistry Letters 2023, 14 (10) , 2573-2579. https://doi.org/10.1021/acs.jpclett.2c03621
    7. Youn Jue Bae, Xingang Zhao, Matthew D. Kryzaniak, Hiroki Nagashima, Joseph Strzalka, Qingteng Zhang, Michael R. Wasielewski. Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films. The Journal of Physical Chemistry C 2020, 124 (18) , 9822-9833. https://doi.org/10.1021/acs.jpcc.0c03189
    8. Alexandr S. Bogomolov, Vladislav M. Rogoveshko, Alexey V. Baklanov. Fast intersystem crossing in the tetracene dimers as a source of “dark” state. AIP Advances 2023, 13 (1) https://doi.org/10.1063/5.0121337
    9. Wenjun Ni, Tianjiao Li, Christian Kloc, Licheng Sun, Gagik G. Gurzadyan. Singlet Fission, Polaron Generation and Intersystem Crossing in Hexaphenyl Film. Molecules 2022, 27 (16) , 5067. https://doi.org/10.3390/molecules27165067
    10. Brandon K. Rugg, Kori E. Smyser, Brian Fluegel, Christopher H. Chang, Karl J. Thorley, Sean Parkin, John E. Anthony, Joel D. Eaves, Justin C. Johnson. Triplet-pair spin signatures from macroscopically aligned heteroacenes in an oriented single crystal. Proceedings of the National Academy of Sciences 2022, 119 (29) https://doi.org/10.1073/pnas.2201879119
    11. Victor Gray, Leah Weiss, Akshay Rao. Singlet Fission: Mechanisms and Molecular Design. 2022, 291-311. https://doi.org/10.1007/978-3-030-70358-5_14
    12. Hélène Seiler, Marcin Krynski, Daniela Zahn, Sebastian Hammer, Yoav William Windsor, Thomas Vasileiadis, Jens Pflaum, Ralph Ernstorfer, Mariana Rossi, Heinrich Schwoerer. Nuclear dynamics of singlet exciton fission in pentacene single crystals. Science Advances 2021, 7 (26) https://doi.org/10.1126/sciadv.abg0869
    13. Muhammad Imran, Xue Zhang, Zhijia Wang, Xi Chen, Jianzhang Zhao, Antonio Barbon, Violeta K. Voronkova. Electron spin dynamics in excited state photochemistry: recent development in the study of intersystem crossing and charge transfer in organic compounds. Physical Chemistry Chemical Physics 2021, 78 https://doi.org/10.1039/D1CP01937F
    14. Chad D. Cruz, Eric L. Chronister, Christopher J. Bardeen. Using temperature dependent fluorescence to evaluate singlet fission pathways in tetracene single crystals. The Journal of Chemical Physics 2020, 153 (23) https://doi.org/10.1063/5.0031458
    15. Saki Matsuda, Shinya Oyama, Yasuhiro Kobori. Electron spin polarization generated by transport of singlet and quintet multiexcitons to spin-correlated triplet pairs during singlet fissions. Chemical Science 2020, 11 (11) , 2934-2942. https://doi.org/10.1039/C9SC04949E

    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