Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

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; Duncan N. Johnstone; Sean M. Collins; Paul A. Midgley; Florian Auras; Tomi Baikie; Rahul Jayaprakash; Fabrice Mathevet; Richard Soucek; Matthew Du; Antonios M. Alvertis; Arjun Ashoka; Silvia Vignolini; David G. Lidzey; Jeremy J. Baumberg; Richard H. Friend; Thierry Barisien; Laurent Legrand; Alex W. Chin; Joel Yuen-Zhou; Semion K. Saikin; Philipp Kukura; Andrew J. Musser; Akshay Rao

doi:10.1038/s41467-021-26617-w

Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

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, Duncan N. Johnstone, Sean M. Collins, Paul A. Midgley, Florian Auras, Tomi Baikie, Rahul Jayaprakash, Fabrice Mathevet, Richard Soucek, Matthew DuAntonios M. Alvertis, Arjun Ashoka, Silvia Vignolini, David G. Lidzey, Jeremy J. Baumberg, Richard H. Friend, Thierry Barisien, Laurent Legrand, Alex W. Chin, Joel Yuen-Zhou, Semion K. Saikin, Philipp Kukura, Andrew J. Musser, Akshay Rao^*

^*Corresponding author for this work

Physics and Astronomy

Research output: Contribution to journal › Article › peer-review

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Abstract

Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 10⁶m s⁻¹), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons

Original language	English
Article number	6519
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-26617-w
Publication status	Published - 11 Nov 2021

Bibliographical note

Funding Information:
We thank the EPSRC (UK) and Winton Program for Physics of Sustainability for financial support. R.P. thanks O. Zadvorna, T. H. Thomas, A. Tanoh, A. Cheminal and W.M. Deacon (Cambridge) for assistance with experiments and useful advice. The authors also thank D. Beljonne (Mons) and S. Pannir-Sivajothi (UCSD) for fruitful discussions. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreements No 670405 and No 758826). The work of G.J, O.D.O. and S.V. was supported by the European Research Council (ERC-2014-STG H2020 639088). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research. R.C. acknowledges support from Trinity College, University of Cambridge. T.W. acknowledges a grant from the Swedish research council (VR, 2014-06948) as well as financial support from the Knut and Alice Wallenberg Foundation through the project grant 3DEM-NATUR (no. 2012.0112). SMC acknowledges the Henslow Research Fellowship at Girton College, Cambridge. P.A.M thanks the EPSRC for financial support under grant number EP/R025517/1. C.S. acknowledges financial support by the Royal Commission for the Exhibition of 1851. We acknowledge access and support in the use of the electron Physical Science Imaging Centre (EM20527) at the Diamond Light Source. A.W.C., T.B., L.L., R. S. and F. M. acknowledge the CNRS (France) for financial support. A.J.M., R.J. and D.G.L. acknowledge support from EPSRC (UK) grant EP/M025330/1. M. D. and J.Y.-Z. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program under Early Career Research Program award DE-SC0019188.

Publisher Copyright:
© 2021, The Author(s).

ASJC Scopus subject areas

General Chemistry
General Biochemistry,Genetics and Molecular Biology
General Physics and Astronomy

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Pandya, R., Chen, R. Y. S., Gu, Q., Sung, J., Schnedermann, C., Ojambati, O. S., Chikkaraddy, R., Gorman, J., Jacucci, G., Onelli, O. D., Willhammar, T., Johnstone, D. N., Collins, S. M., Midgley, P. A., Auras, F., Baikie, T., Jayaprakash, R., Mathevet, F., Soucek, R., ... Rao, A. (2021). Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors. Nature Communications, 12(1), Article 6519. https://doi.org/10.1038/s41467-021-26617-w

@article{266644bc56994e70a708556a0f6d2997,

title = "Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors",

abstract = "Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106m s−1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons",

author = "Raj Pandya and Chen, {Richard Y.S.} and Qifei Gu and Jooyoung Sung and Christoph Schnedermann and Ojambati, {Oluwafemi S.} and Rohit Chikkaraddy and Jeffrey Gorman and Gianni Jacucci and Onelli, {Olimpia D.} and Tom Willhammar and Johnstone, {Duncan N.} and Collins, {Sean M.} and Midgley, {Paul A.} and Florian Auras and Tomi Baikie and Rahul Jayaprakash and Fabrice Mathevet and Richard Soucek and Matthew Du and Alvertis, {Antonios M.} and Arjun Ashoka and Silvia Vignolini and Lidzey, {David G.} and Baumberg, {Jeremy J.} and Friend, {Richard H.} and Thierry Barisien and Laurent Legrand and Chin, {Alex W.} and Joel Yuen-Zhou and Saikin, {Semion K.} and Philipp Kukura and Musser, {Andrew J.} and Akshay Rao",

note = "Funding Information: We thank the EPSRC (UK) and Winton Program for Physics of Sustainability for financial support. R.P. thanks O. Zadvorna, T. H. Thomas, A. Tanoh, A. Cheminal and W.M. Deacon (Cambridge) for assistance with experiments and useful advice. The authors also thank D. Beljonne (Mons) and S. Pannir-Sivajothi (UCSD) for fruitful discussions. This project has received funding from the European Research Council (ERC) under the European Union{\textquoteright}s Horizon 2020 research and innovation programme (grant agreements No 670405 and No 758826). The work of G.J, O.D.O. and S.V. was supported by the European Research Council (ERC-2014-STG H2020 639088). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research. R.C. acknowledges support from Trinity College, University of Cambridge. T.W. acknowledges a grant from the Swedish research council (VR, 2014-06948) as well as financial support from the Knut and Alice Wallenberg Foundation through the project grant 3DEM-NATUR (no. 2012.0112). SMC acknowledges the Henslow Research Fellowship at Girton College, Cambridge. P.A.M thanks the EPSRC for financial support under grant number EP/R025517/1. C.S. acknowledges financial support by the Royal Commission for the Exhibition of 1851. We acknowledge access and support in the use of the electron Physical Science Imaging Centre (EM20527) at the Diamond Light Source. A.W.C., T.B., L.L., R. S. and F. M. acknowledge the CNRS (France) for financial support. A.J.M., R.J. and D.G.L. acknowledge support from EPSRC (UK) grant EP/M025330/1. M. D. and J.Y.-Z. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program under Early Career Research Program award DE-SC0019188. Publisher Copyright: {\textcopyright} 2021, The Author(s).",

year = "2021",

month = nov,

day = "11",

doi = "10.1038/s41467-021-26617-w",

language = "English",

volume = "12",

journal = "Nature Communications",

issn = "2041-1723",

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Pandya, R, Chen, RYS, Gu, Q, Sung, J, Schnedermann, C, Ojambati, OS, Chikkaraddy, R, Gorman, J, Jacucci, G, Onelli, OD, Willhammar, T, Johnstone, DN, Collins, SM, Midgley, PA, Auras, F, Baikie, T, Jayaprakash, R, Mathevet, F, Soucek, R, Du, M, Alvertis, AM, Ashoka, A, Vignolini, S, Lidzey, DG, Baumberg, JJ, Friend, RH, Barisien, T, Legrand, L, Chin, AW, Yuen-Zhou, J, Saikin, SK, Kukura, P, Musser, AJ & Rao, A 2021, 'Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors', Nature Communications, vol. 12, no. 1, 6519. https://doi.org/10.1038/s41467-021-26617-w

TY - JOUR

T1 - Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

AU - Pandya, Raj

AU - Chen, Richard Y.S.

AU - Gu, Qifei

AU - Sung, Jooyoung

AU - Schnedermann, Christoph

AU - Ojambati, Oluwafemi S.

AU - Chikkaraddy, Rohit

AU - Gorman, Jeffrey

AU - Jacucci, Gianni

AU - Onelli, Olimpia D.

AU - Willhammar, Tom

AU - Johnstone, Duncan N.

AU - Collins, Sean M.

AU - Midgley, Paul A.

AU - Auras, Florian

AU - Baikie, Tomi

AU - Jayaprakash, Rahul

AU - Mathevet, Fabrice

AU - Soucek, Richard

AU - Du, Matthew

AU - Alvertis, Antonios M.

AU - Ashoka, Arjun

AU - Vignolini, Silvia

AU - Lidzey, David G.

AU - Baumberg, Jeremy J.

AU - Friend, Richard H.

AU - Barisien, Thierry

AU - Legrand, Laurent

AU - Chin, Alex W.

AU - Yuen-Zhou, Joel

AU - Saikin, Semion K.

AU - Kukura, Philipp

AU - Musser, Andrew J.

AU - Rao, Akshay

N1 - Funding Information: We thank the EPSRC (UK) and Winton Program for Physics of Sustainability for financial support. R.P. thanks O. Zadvorna, T. H. Thomas, A. Tanoh, A. Cheminal and W.M. Deacon (Cambridge) for assistance with experiments and useful advice. The authors also thank D. Beljonne (Mons) and S. Pannir-Sivajothi (UCSD) for fruitful discussions. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreements No 670405 and No 758826). The work of G.J, O.D.O. and S.V. was supported by the European Research Council (ERC-2014-STG H2020 639088). O.S.O acknowledges the support of a Rubicon fellowship from the Netherlands Organisation for Scientific Research. R.C. acknowledges support from Trinity College, University of Cambridge. T.W. acknowledges a grant from the Swedish research council (VR, 2014-06948) as well as financial support from the Knut and Alice Wallenberg Foundation through the project grant 3DEM-NATUR (no. 2012.0112). SMC acknowledges the Henslow Research Fellowship at Girton College, Cambridge. P.A.M thanks the EPSRC for financial support under grant number EP/R025517/1. C.S. acknowledges financial support by the Royal Commission for the Exhibition of 1851. We acknowledge access and support in the use of the electron Physical Science Imaging Centre (EM20527) at the Diamond Light Source. A.W.C., T.B., L.L., R. S. and F. M. acknowledge the CNRS (France) for financial support. A.J.M., R.J. and D.G.L. acknowledge support from EPSRC (UK) grant EP/M025330/1. M. D. and J.Y.-Z. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS Program under Early Career Research Program award DE-SC0019188. Publisher Copyright: © 2021, The Author(s).

PY - 2021/11/11

Y1 - 2021/11/11

N2 - Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106m s−1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons

AB - Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106m s−1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons

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U2 - 10.1038/s41467-021-26617-w

DO - 10.1038/s41467-021-26617-w

M3 - Article

C2 - 34764252

AN - SCOPUS:85118936223

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 6519

ER -

Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

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