IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v13y2022i1d10.1038_s41467-022-35046-2.html
   My bibliography  Save this article

Energy cascades in donor-acceptor exciton-polaritons observed by ultrafast two-dimensional white-light spectroscopy

Author

Listed:
  • Minjung Son

    (University of Wisconsin-Madison)

  • Zachary T. Armstrong

    (University of Wisconsin-Madison)

  • Ryan T. Allen

    (University of Wisconsin-Madison)

  • Abitha Dhavamani

    (University of Wisconsin-Madison)

  • Michael S. Arnold

    (University of Wisconsin-Madison)

  • Martin T. Zanni

    (University of Wisconsin-Madison)

Abstract

Exciton-polaritons are hybrid states formed when molecular excitons are strongly coupled to photons trapped in an optical cavity. These systems exhibit many interesting, but not fully understood, phenomena. Here, we utilize ultrafast two-dimensional white-light spectroscopy to study donor-acceptor microcavities made from two different layers of semiconducting carbon nanotubes. We observe the delayed growth of a cross peak between the upper- and lower-polariton bands that is oftentimes obscured by Rabi contraction. We simulate the spectra and use Redfield theory to learn that energy cascades down a manifold of new electronic states created by intermolecular coupling and the two distinct bandgaps of the donor and acceptor. Energy most effectively enters the manifold when light-matter coupling is commensurate with the energy distribution of the manifold, contributing to long-range energy transfer. Our results broaden the understanding of energy transfer dynamics in exciton-polariton systems and provide evidence that long-range energy transfer benefits from moderately-coupled cavities.

Suggested Citation

  • Minjung Son & Zachary T. Armstrong & Ryan T. Allen & Abitha Dhavamani & Michael S. Arnold & Martin T. Zanni, 2022. "Energy cascades in donor-acceptor exciton-polaritons observed by ultrafast two-dimensional white-light spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35046-2
    DOI: 10.1038/s41467-022-35046-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-022-35046-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-022-35046-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. D. G. Lidzey & D. D. C. Bradley & M. S. Skolnick & T. Virgili & S. Walker & D. M. Whittaker, 1998. "Strong exciton–photon coupling in an organic semiconductor microcavity," Nature, Nature, vol. 395(6697), pages 53-55, September.
    2. Andrea B. Grafton & Adam D. Dunkelberger & Blake S. Simpkins & Johan F. Triana & Federico J. Hernández & Felipe Herrera & Jeffrey C. Owrutsky, 2021. "Excited-state vibration-polariton transitions and dynamics in nitroprusside," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    3. Randy D. Mehlenbacher & Thomas J. McDonough & Maksim Grechko & Meng-Yin Wu & Michael S. Arnold & Martin T. Zanni, 2015. "Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy," Nature Communications, Nature, vol. 6(1), pages 1-7, November.
    4. Raj Pandya & Richard Y. S. Chen & Qifei Gu & Jooyoung Sung & Christoph Schnedermann & Oluwafemi S. Ojambati & Rohit Chikkaraddy & Jeffrey Gorman & Gianni Jacucci & Olimpia D. Onelli & Tom Willhammar &, 2021. "Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    5. Kati Stranius & Manuel Hertzog & Karl Börjesson, 2018. "Selective manipulation of electronically excited states through strong light–matter interactions," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Daniel Timmer & Moritz Gittinger & Thomas Quenzel & Sven Stephan & Yu Zhang & Marvin F. Schumacher & Arne Lützen & Martin Silies & Sergei Tretiak & Jin-Hui Zhong & Antonietta De Sio & Christoph Lienau, 2023. "Plasmon mediated coherent population oscillations in molecular aggregates," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Siddhartha Sohoni & Indranil Ghosh & Geoffrey T. Nash & Claire A. Jones & Lawson T. Lloyd & Beiye C. Li & Karen L. Ji & Zitong Wang & Wenbin Lin & Gregory S. Engel, 2024. "Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Ilia Sokolovskii & Ruth H. Tichauer & Dmitry Morozov & Johannes Feist & Gerrit Groenhof, 2023. "Multi-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Fan Wu & Daniel Finkelstein-Shapiro & Mao Wang & Ilmari Rosenkampff & Arkady Yartsev & Torbjörn Pascher & Tu C. Nguyen- Phan & Richard Cogdell & Karl Börjesson & Tönu Pullerits, 2022. "Optical cavity-mediated exciton dynamics in photosynthetic light harvesting 2 complexes," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    2. Arpan Dutta & Ville Tiainen & Ilia Sokolovskii & Luís Duarte & Nemanja Markešević & Dmitry Morozov & Hassan A. Qureshi & Siim Pikker & Gerrit Groenhof & J. Jussi Toppari, 2024. "Thermal disorder prevents the suppression of ultra-fast photochemistry in the strong light-matter coupling regime," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Qi Yu & Joel M. Bowman, 2023. "Manipulating hydrogen bond dissociation rates and mechanisms in water dimer through vibrational strong coupling," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Arjun Ashoka & Nicolas Gauriot & Aswathy V. Girija & Nipun Sawhney & Alexander J. Sneyd & Kenji Watanabe & Takashi Taniguchi & Jooyoung Sung & Christoph Schnedermann & Akshay Rao, 2022. "Direct observation of ultrafast singlet exciton fission in three dimensions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    5. Ahmed Jaber & Michael Reitz & Avinash Singh & Ali Maleki & Yongbao Xin & Brian T. Sullivan & Ksenia Dolgaleva & Robert W. Boyd & Claudiu Genes & Jean-Michel Ménard, 2024. "Hybrid architectures for terahertz molecular polaritonics," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    6. Tao E. Li & Abraham Nitzan & Joseph E. Subotnik, 2022. "Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    7. María Barra-Burillo & Unai Muniain & Sara Catalano & Marta Autore & Fèlix Casanova & Luis E. Hueso & Javier Aizpurua & Ruben Esteban & Rainer Hillenbrand, 2021. "Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    8. Sindhana Pannir-Sivajothi & Jorge A. Campos-Gonzalez-Angulo & Luis A. Martínez-Martínez & Shubham Sinha & Joel Yuen-Zhou, 2022. "Driving chemical reactions with polariton condensates," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    9. Ilia Sokolovskii & Ruth H. Tichauer & Dmitry Morozov & Johannes Feist & Gerrit Groenhof, 2023. "Multi-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    10. Raj Pandya & Richard Y. S. Chen & Qifei Gu & Jooyoung Sung & Christoph Schnedermann & Oluwafemi S. Ojambati & Rohit Chikkaraddy & Jeffrey Gorman & Gianni Jacucci & Olimpia D. Onelli & Tom Willhammar &, 2021. "Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    11. Daniel Timmer & Moritz Gittinger & Thomas Quenzel & Sven Stephan & Yu Zhang & Marvin F. Schumacher & Arne Lützen & Martin Silies & Sergei Tretiak & Jin-Hui Zhong & Antonietta De Sio & Christoph Lienau, 2023. "Plasmon mediated coherent population oscillations in molecular aggregates," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    12. Clara Schäfer & Rasmus Ringström & Jörg Hanrieder & Martin Rahm & Bo Albinsson & Karl Börjesson, 2024. "Lowering of the singlet-triplet energy gap via intramolecular exciton-exciton coupling," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    13. Ruixiang Chen & Ningning Liang & Tianrui Zhai, 2024. "Dual-color emissive OLED with orthogonal polarization modes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    14. Philip A. Thomas & Kishan S. Menghrajani & William L. Barnes, 2022. "All-optical control of phase singularities using strong light-matter coupling," Nature Communications, Nature, vol. 13(1), pages 1-6, December.
    15. Konrad Birkmeier & Tobias Hertel & Achim Hartschuh, 2022. "Probing the ultrafast dynamics of excitons in single semiconducting carbon nanotubes," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    16. David Allemeier & Benjamin Isenhart & Ekraj Dahal & Yuki Tsuda & Tsukasa Yoshida & Matthew S. White, 2021. "Emergence and control of photonic band structure in stacked OLED microcavities," Nature Communications, Nature, vol. 12(1), pages 1-7, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35046-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.