IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v13y2022i1d10.1038_s41467-022-29003-2.html
   My bibliography  Save this article

Molecular orbital theory in cavity QED environments

Author

Listed:
  • Rosario R. Riso

    (Norwegian University of Science and Technology)

  • Tor S. Haugland

    (Norwegian University of Science and Technology)

  • Enrico Ronca

    (Istituto per i Processi Chimico Fisici del CNR (IPCF-CNR))

  • Henrik Koch

    (Norwegian University of Science and Technology
    Scuola Normale Superiore)

Abstract

Coupling between molecules and vacuum photon fields inside an optical cavity has proven to be an effective way to engineer molecular properties, in particular reactivity. To ease the rationalization of cavity induced effects we introduce an ab initio method leading to the first fully consistent molecular orbital theory for quantum electrodynamics environments. Our framework is non-perturbative and explains modifications of the electronic structure due to the interaction with the photon field. In this work, we show that the newly developed orbital theory can be used to predict cavity induced modifications of molecular reactivity and pinpoint classes of systems with significant cavity effects. We also investigate electronic cavity-induced modifications of reaction mechanisms in vibrational strong coupling regimes.

Suggested Citation

  • Rosario R. Riso & Tor S. Haugland & Enrico Ronca & Henrik Koch, 2022. "Molecular orbital theory in cavity QED environments," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29003-2
    DOI: 10.1038/s41467-022-29003-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-022-29003-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-022-29003-2?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. J. Fregoni & G. Granucci & E. Coccia & M. Persico & S. Corni, 2018. "Manipulating azobenzene photoisomerization through strong light–molecule coupling," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    2. Rohit Chikkaraddy & Bart de Nijs & Felix Benz & Steven J. Barrow & Oren A. Scherman & Edina Rosta & Angela Demetriadou & Peter Fox & Ortwin Hess & Jeremy J. Baumberg, 2016. "Single-molecule strong coupling at room temperature in plasmonic nanocavities," Nature, Nature, vol. 535(7610), pages 127-130, July.
    3. A. Shalabney & J. George & J. Hutchison & G. Pupillo & C. Genet & T. W. Ebbesen, 2015. "Coherent coupling of molecular resonators with a microcavity mode," Nature Communications, Nature, vol. 6(1), pages 1-6, May.
    Full references (including those not matched with items on IDEAS)

    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. Kaihong Sun & Raphael F. Ribeiro, 2024. "Theoretical formulation of chemical equilibrium under vibrational strong coupling," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Tingting Wu & Chongwu Wang & Guangwei Hu & Zhixun Wang & Jiaxin Zhao & Zhe Wang & Ksenia Chaykun & Lin Liu & Mengxiao Chen & Dong Li & Song Zhu & Qihua Xiong & Zexiang Shen & Huajian Gao & Francisco J, 2024. "Ultrastrong exciton-plasmon couplings in WS2 multilayers synthesized with a random multi-singular metasurface at room temperature," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Fuhuan Shen & Zhenghe Zhang & Yaoqiang Zhou & Jingwen Ma & Kun Chen & Huanjun Chen & Shaojun Wang & Jianbin Xu & Zefeng Chen, 2022. "Transition metal dichalcogenide metaphotonic and self-coupled polaritonic platform grown by chemical vapor deposition," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Nicholas A. Güsken & Ming Fu & Maximilian Zapf & Michael P. Nielsen & Paul Dichtl & Robert Röder & Alex S. Clark & Stefan A. Maier & Carsten Ronning & Rupert F. Oulton, 2023. "Emission enhancement of erbium in a reverse nanofocusing waveguide," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Xiang-Dong Chen & En-Hui Wang & Long-Kun Shan & Ce Feng & Yu Zheng & Yang Dong & Guang-Can Guo & Fang-Wen Sun, 2021. "Focusing the electromagnetic field to 10−6λ for ultra-high enhancement of field-matter interaction," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    6. 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.
    7. Longlong Yang & Yu Yuan & Bowen Fu & Jingnan Yang & Danjie Dai & Shushu Shi & Sai Yan & Rui Zhu & Xu Han & Hancong Li & Zhanchun Zuo & Can Wang & Yuan Huang & Kuijuan Jin & Qihuang Gong & Xiulai Xu, 2023. "Revealing broken valley symmetry of quantum emitters in WSe2 with chiral nanocavities," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    8. Joel Kuttruff & Marco Romanelli & Esteban Pedrueza-Villalmanzo & Jonas Allerbeck & Jacopo Fregoni & Valeria Saavedra-Becerril & Joakim Andréasson & Daniele Brida & Alexandre Dmitriev & Stefano Corni &, 2023. "Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    9. Chi Zhang & Huatian Hu & Chunmiao Ma & Yawen Li & Xujie Wang & Dongyao Li & Artur Movsesyan & Zhiming Wang & Alexander Govorov & Quan Gan & Tao Ding, 2024. "Quantum plasmonics pushes chiral sensing limit to single molecules: a paradigm for chiral biodetections," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    10. Connor K. Terry Weatherly & Justin Provazza & Emily A. Weiss & Roel Tempelaar, 2023. "Theory predicts UV/vis-to-IR photonic down conversion mediated by excited state vibrational polaritons," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    11. 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.
    12. Renming Liu & Ming Geng & Jindong Ai & Xinyi Fan & Zhixiang Liu & Yu-Wei Lu & Yanmin Kuang & Jing-Feng Liu & Lijun Guo & Lin Wu, 2024. "Deterministic positioning and alignment of a single-molecule exciton in plasmonic nanodimer for strong coupling," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    13. Guang-Can Li & Dangyuan Lei & Meng Qiu & Wei Jin & Sheng Lan & Anatoly V. Zayats, 2021. "Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    14. Shu Hu & Junyang Huang & Rakesh Arul & Ana Sánchez-Iglesias & Yuling Xiong & Luis M. Liz-Marzán & Jeremy J. Baumberg, 2024. "Robust consistent single quantum dot strong coupling in plasmonic nanocavities," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    15. Ferry Anggoro Ardy Nugroho & Ping Bai & Iwan Darmadi & Gabriel W. Castellanos & Joachim Fritzsche & Christoph Langhammer & Jaime Gómez Rivas & Andrea Baldi, 2022. "Inverse designed plasmonic metasurface with parts per billion optical hydrogen detection," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    16. Shima Rajabali & Sergej Markmann & Elsa Jöchl & Mattias Beck & Christian A. Lehner & Werner Wegscheider & Jérôme Faist & Giacomo Scalari, 2022. "An ultrastrongly coupled single terahertz meta-atom," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    17. Irene Dolado & Carlos Maciel-Escudero & Elizaveta Nikulina & Evgenii Modin & Francesco Calavalle & Shu Chen & Andrei Bylinkin & Francisco Javier Alfaro-Mozaz & Jiahan Li & James H. Edgar & Fèlix Casan, 2022. "Remote near-field spectroscopy of vibrational strong coupling between organic molecules and phononic nanoresonators," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    18. 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.
    19. 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.
    20. 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.

    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_s41467-022-29003-2. 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.