Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Generating Phase Singularities Using Surface Exciton Polaritons in an Organic Natural Hyperbolic Material

Philip A. Thomas*, William P. Wardley, and William L. Barnes

  • *Contact author: p.thomas2@exeter.ac.uk

Phys. Rev. Lett. 135, 146906 – Published 2 October, 2025

DOI: https://doi.org/10.1103/sj4r-cb56

Abstract

Surface polaritons (SPs) are electromagnetic waves bound to a surface through their interaction with charge carriers in the surface material. Hyperbolic SPs can be supported by optically anisotropic materials where the in-plane and out-of-plane permittivities have opposite signs. Here we report what we believe to be the first experimental study of hyperbolic surface exciton polaritons (HSEPs). We study the intensity and phase response of HSEPs in the J-aggregate TDBC (a type-II natural hyperbolic material). HSEPs can be used to generate phase singularities; the behavior of these phase singularities is a consequence of the hyperbolic nature of TDBC. The combined intensity and phase response of nonhyperbolic and hyperbolic SPs suggests that they are topologically distinct. We predict analogous effects for hyperbolic surface phonon polaritons in hexagonal boron nitride. Our Letter suggests that organic materials can provide a new platform for the exploration of hyperbolic surface polaritonics at visible frequencies.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (50)

  1. L. Novotny and B. Hecht, Principles of Nano-Optics (Cambridge University Press, Cambridge, England, 2012), 10.1017/CBO9780511794193.
  2. D. N. Basov, M. M. Fogler, and F. J. García de Abajo, Polaritons in van der Waals materials, Science 354, aag1992 (2016).
  3. S. A. Maier, Plasmonics: Fundamentals and Applications (Springer, New York, 2007), 10.1007/0-387-37825-1.
  4. P. Berini, Long-range surface plasmon polaritons, Adv. Opt. Photonics 1, 484 (2009).
  5. A. N. Grigorenko, M. Polini, and K. S. Novoselov, Graphene plasmonics, Nat. Photonics 6, 749 (2012).
  6. C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, and J. Feldmann, Drastic reduction of plasmon damping in gold nanorods, Phys. Rev. Lett. 88, 077402 (2002).
  7. M. W. Knight, N. S. King, L. Liu, H. O. Everitt, P. Nordlander, and N. J. Halas, Aluminum for plasmonics, ACS Nano 8, 834 (2014).
  8. W. P. Wardley, F. J. Rodríguez-Fortuño, A. V. Zayats, and W. Dickson, Improving propagation lengths of ultraviolet surface plasmon polaritons on thin aluminium films by ion milling, J. Phys. D 52, 074004 (2019).
  9. D. N. Basov, A. Asenjo-Garcia, P. J. Schuck, X. Zhu, and A. Rubio, Polariton panorama, Nanophotonics 10, 549 (2020).
  10. J. D. Caldwell et al., Sub-diffractional volume-confined polaritons in the natural hyperbolic material hexagonal boron nitride, Nat. Commun. 5, 5221 (2014).
  11. J. D. Caldwell, L. Lindsay, V. Giannini, I. Vurgaftman, T. L. Reinecke, S. A. Maier, and O. J. Glembocki, Low-loss, infrared and terahertz nanophotonics using surface phonon polaritons, Nanophotonics 4, 44 (2015).
  12. M. R. Philpott and J. D. Swalen, Exciton surface polaritons on organic crystals, J. Chem. Phys. 69, 2912 (1978).
  13. M. R. Philpott, A. Brillante, I. R. Pockrand, and J. R. Swalen, A new optical phenomenon: Exciton surface polaritons at room temperature, Mol. Cryst. Liq. Cryst. 50, 139 (1979).
  14. S. Chen and M. P. Jonsson, Dynamic conducting polymer plasmonics and metasurfaces, ACS Photonics 10, 571 (2023).
  15. M. G. Gentile, S. Núñez-Sánchez, and W. L. Barnes, Optical field-enhancement and subwavelength field-confinement using excitonic nanostructures, Nano Lett. 14, 2339 (2014).
  16. L. Gu, J. Livenere, G. Zhu, E. E. Narimanov, and M. A. Noginov, Quest for organic plasmonics, Appl. Phys. Lett. 103, 021104 (2013).
  17. S. Núñez-Sánchez, M. Lopez-Garcia, M. M. Murshidy, A. G. Abdel-Hady, M. Serry, A. M. Adawi, J. G. Rarity, R. Oulton, and W. L. Barnes, Excitonic optical Tamm states: A step toward a full molecular–dielectric photonic integration, ACS Photonics 3, 743 (2016).
  18. K. Takatori, T. Okamoto, K. Ishibashi, and R. Micheletto, Surface exciton polaritons supported by a J-aggregate-dye/air interface at room temperature, Opt. Lett. 42, 3876 (2017).
  19. M. J. Gentile, S. A. R. Horsley, and W. L. Barnes, Localized exciton–polariton modes in dye-doped nanospheres: A quantum approach, J. Opt. 18, 015001 (2016).
  20. A. D. Humphrey, M. J. Gentile, and W. L. Barnes, Excitonic surface lattice resonances, J. Opt. 18, 085004 (2016).
  21. M. J. Gentile and W. L. Barnes, Hybridised exciton–polariton resonances in core–shell nanoparticles, J. Opt. 19, 035003 (2017).
  22. A. Dutta and J. J. Toppari, Effect of molecular concentration on excitonic nanostructure based refractive index sensing and near-field enhanced spectroscopy, Opt. Mater. Express 13, 2426 (2023).
  23. A. Dutta and J. J. Toppari, Weak and strong coupling properties of surface excitons, Phys. Rev. B 109, 165117 (2024).
  24. E. S. H. Kang et al., Organic anisotropic excitonic optical nanoantennas, Adv. Sci. 9, 2201907 (2022).
  25. A. Poddubny, I. Iorsh, P. Belov, and Y. Kivshar, Hyperbolic metamaterials, Nat. Photonics 7, 948 (2013).
  26. Z. Liu, H. Lee, Y. Xiong, C. Sun, and X. Zhang, Far-field optical hyperlens magnifying sub-diffraction-limited objects, Science 315, 1686 (2007).
  27. A. J. Hoffman, L. Alekseyev, S. S. Howard, K. J. Franz, D. Wasserman, V. A. Podolskiy, E. E. Narimanov, D. L. Sivco, and C. Gmachl, Negative refraction in semiconductor metamaterials, Nat. Mater. 6, 946 (2007).
  28. K. Korzeb, M. Gajc, and D. A. Pawlak, Compendium of natural hyperbolic materials, Opt. Express 23, 25406 (2015).
  29. G. Carini, R. Niemann, N. S. Mueller, M. Wolf, and A. Paarmann, Surface phonon polariton ellipsometry, ACS Photonics 12, 792 (2025).
  30. J. Dintinger, S. Klein, F. Bustos, W. L. Barnes, and T. W. Ebbesen, Strong coupling between surface plasmon-polaritons and organic molecules in subwavelength hole arrays, Phys. Rev. B 71, 035424 (2005).
  31. P. Törmä and W. L. Barnes, Strong coupling between surface plasmon polaritons and emitters: A review, Rep. Prog. Phys. 78, 013901 (2014).
  32. S. T. Holder, C. Estévez-Varela, I. Pastoriza-Santos, M. Lopez-Garcia, R. Oulton, and S. Núñez-Sánchez, Bio-inspired building blocks for all-organic metamaterials from visible to near-infrared, Nanophotonics 12, 307 (2023).
  33. F. Würthner, T. E. Kaiser, and C. R. Saha-Möller, J-Aggregates: From serendipitous discovery to supramolecular engineering of functional dye materials, Angew. Chem. 50, 3376 (2011).
  34. O. Takamaya and A. V. Lavrinenko, Optics with hyperbolic materials, J. Opt. Soc. Am. B 36, F38 (2019).
  35. See Supplemental Material at http://link.aps.org/supplemental/10.1103/sj4r-cb56 for experimental and numerical methods, a review of other candidate materials, and further characterization of prism coupling experiments.
  36. K. Roodenko, H. M. Nguyen, L. Caillard, A. Radja, P. Thissen, J. M. Gordon, Y. N. Gartstein, A. V. Malko, and Y. J. Chabal, Anisotropic optical properties of thin-film thiacarbocyanine dye aggregates, J. Phys. Chem. C 117, 20186 (2013).
  37. S. Hayashi, Y. Ishigaki, and M. Fujii, Plasmonic effects on strong exciton-photon coupling in metal-insulator-metal microcavities, Phys. Rev. B 86, 045408 (2012).
  38. E. Kretschmann and H. Raether, Radiative decay of non radiative surface plasmons excited by light, Z. Naturforsch. A 23, 2135 (1968).
  39. H. Tompkins and E. A. Irene, Handbook of Ellipsometry (William Andrew Publishing, Norwich, NY, USA, 2005).
  40. E. D. Palik, Handbook of Optical Constants of Solids (Academic, New York, 1985).
  41. M. Berry, Making waves in physics, Nature (London) 403, 21 (2000).
  42. J. F. Nye and M. V. Berry, Dislocations in wave trains, Proc. R. Soc. A 336, 165 (1974).
  43. J. Ni, C. Huang, L.-M. Zhou, M. Gu, Q. Song, Y. Kivshar, and C.-W. Qiu, Multidimensional phase singularities in nanophotonics, Science 374, eabj0039 (2021).
  44. A. V. Kabashin, V. G. Kravets, and A. N. Grigorenko, Label-free optical biosensing: Going beyond the limits, Chem. Soc. Rev. 52, 6554 (2023).
  45. J. R. Tischler, M. S. Bradley, and V. Bulović, Critically coupled resonators in vertical geometry using a planar mirror and a 5 nm thick absorbing film, Opt. Lett. 31, 2045 (2006).
  46. E. Cusworth, V. G. Kravets, and A. N. Grigorenko, Topological darkness in optical heterostructures: Prediction and confirmation, ACS Photonics 10, 3715 (2023).
  47. P. A. Thomas, K. S. Menghrajani, and W. L. Barnes, All-optical control of phase singularities using strong light-matter coupling, Nat. Commun. 13, 1809 (2022).
  48. P. A. Thomas, W. J. Tan, H. A. Fernandez, and W. L. Barnes, A new signature for strong light–matter coupling using spectroscopic ellipsometry, Nano Lett. 20, 6412 (2020).
  49. N. Meinzer, W. L. Barnes, and I. R. Hooper, Plasmonic meta-atoms and metasurfaces, Nat. Photonics 8, 889 (2014).
  50. P. A. Thomas, W. P. Wardley, and W. L. Barnes, Generating phase singularities using surface exciton polaritons in an organic natural hyperbolic material (dataset), Zenodo, 2025, 10.5281/zenodo.17091986.

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation