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Photoinduced Charge Transfer in Single-Molecule p–n Junctions

  • Shenkai Wang
    Shenkai Wang
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
    More by Shenkai Wang
  • Natcha Wattanatorn
    Natcha Wattanatorn
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
  • Naihao Chiang
    Naihao Chiang
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
  • Yuxi Zhao
    Yuxi Zhao
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
    More by Yuxi Zhao
  • Moonhee Kim
    Moonhee Kim
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
    More by Moonhee Kim
  • Hong Ma
    Hong Ma
    Department of Materials Science and Engineering, University of Washington, Seattle, Washington 98185, United States
    More by Hong Ma
  • Alex K.-Y. Jen
    Alex K.-Y. Jen
    Department of Materials Science and Engineering, University of Washington, Seattle, Washington 98185, United States
  • , and 
  • Paul S. Weiss*
    Paul S. Weiss
    Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095, United States
    California NanoSystems Institute, University of California, Los Angeles, Los Angeles, California 90095, United States
    Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, California 90095, United States
    *E-mail: [email protected]
Cite this: J. Phys. Chem. Lett. 2019, 10, 9, 2175–2181
Publication Date (Web):April 16, 2019
https://doi.org/10.1021/acs.jpclett.9b00855
Copyright © 2019 American Chemical Society

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    Abstract

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    We measured photoinduced charge separation in isolated individual C60-tethered 2,5-dithienylpyrrole triad (C60 triad) molecules with submolecular resolution using a custom-built laser-assisted scanning tunneling microscope. Laser illumination was introduced evanescently into the tunneling junction through total internal reflection, and the changes in tunneling current and electronic spectra caused by photoexcitation were measured and spatially resolved. Photoinduced charge separation was not detected for all C60 triad molecules, indicating that the conformations of the molecules may affect the excitation probability, lifetime, and/or charge distribution. A photoinduced signal was not observed for dodecanethiol molecules in the surrounding matrix or for control molecules without C60 moieties, as neither absorbs incident photons at this energy. This spectroscopic imaging technique has the potential to elucidate detailed photoinduced carrier dynamics, which are inaccessible via ensemble-scale (i.e., averaging) measurements, which can be used to direct the rational design and optimization of molecular p–n junctions and assemblies for energy harvesting.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.9b00855.

    • The design of our custom-built laser-assisted scanning tunneling microscopy and methodology followed for the preparation of Au{111}/Al2O3(0001) substrates and self-assembled monolayers (PDF)

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    Cited By

    This article is cited by 9 publications.

    1. Sarah Wieghold, Lea Nienhaus. Viewing Optical Processes at the Nanoscale: Combining Scanning Tunneling Microscopy and Optical Spectroscopy. The Journal of Physical Chemistry C 2023, 127 (8) , 3913-3920. https://doi.org/10.1021/acs.jpcc.2c08912
    2. Yi Cao, Yanting Feng, Chenyu Li, Wenwen Li, Yuqing Cheng, Jindou Ru, Lingyan Meng, Mengtao Sun. Plasmonic Gradient and Plexcitonic Effects in Single-Molecule Tip-Enhanced (Resonance) Raman Spectroscopy. The Journal of Physical Chemistry C 2023, 127 (1) , 476-489. https://doi.org/10.1021/acs.jpcc.2c07971
    3. Kristopher K. Barr, Naihao Chiang, Andrea L. Bertozzi, Jérôme Gilles, Stanley J. Osher, Paul S. Weiss. Extraction of Hidden Science from Nanoscale Images. The Journal of Physical Chemistry C 2022, 126 (1) , 3-13. https://doi.org/10.1021/acs.jpcc.1c08712
    4. Shenkai Wang, Naihao Chiang, Han Guo, Natcha Wattanatorn, Kristopher K. Barr, Anastassia N. Alexandrova, Paul S. Weiss. Photoinduced Carrier Generation and Distribution in Solution-Deposited Titanyl Phthalocyanine Monolayers. Chemistry of Materials 2019, 31 (24) , 10109-10116. https://doi.org/10.1021/acs.chemmater.9b03252
    5. Wei Xu, Ruihao Li, Chenhao Wang, Jiahe Zhong, Junyang Liu, Wenjing Hong. Investigation of electronic excited states in single-molecule junctions. Nano Research 2022, 15 (6) , 5726-5745. https://doi.org/10.1007/s12274-022-4102-3
    6. Peihui Li, Zhou Li, Cong Zhao, Hongyu Ju, Qinghua Gao, Wei Si, Li Cheng, Jie Hao, Mengmeng Li, Yijian YiChen, Chuancheng Jia, Xuefeng Guo. Single-molecule nano-optoelectronics: Insights from physics. Reports on Progress in Physics 2022, https://doi.org/10.1088/1361-6633/ac7401
    7. Jeremy F Schultz, Shaowei Li, Song Jiang, Nan Jiang. Optical scanning tunneling microscopy based chemical imaging and spectroscopy. Journal of Physics: Condensed Matter 2020, 32 (46) , 463001. https://doi.org/10.1088/1361-648X/aba8c7
    8. Alison Wallum, Huy A. Nguyen, Martin Gruebele. Excited-State Imaging of Single Particles on the Subnanometer Scale. Annual Review of Physical Chemistry 2020, 71 (1) , 415-433. https://doi.org/10.1146/annurev-physchem-071119-040108
    9. Sarah Wieghold, Lea Nienhaus. Probing Semiconductor Properties with Optical Scanning Tunneling Microscopy. Joule 2020, 4 (3) , 524-538. https://doi.org/10.1016/j.joule.2020.02.003

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