close
Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Macroscopic coherence of a single exciton state in an organic quantum wire

Abstract

Macroscopic quantum coherence has been observed in some many-body systems including superconductors, quantum liquids1 and cold atom condensates2, but never for a single quasi-particle state. In an ideal semiconductor, excitons (electron–hole pairs bound by the Coulomb interaction) can, in principle, exist as delocalized plane waves extending over the entire volume. However, any kind of disorder prevents long-range spatial coherence from emerging. There has been evidence for the formation of macroscopic coherent states only in condensate phases such as in the case of microcavity polaritons condensation3,4 or in a dense quasi-two-dimensional exciton gas5. It is unclear however, whether in this latter case the observations are really related to macroscopic coherence6. Here, we show that a single exciton state in an individual ordered conjugated polymer chain7,8, shows macroscopic quantum spatial coherence reaching tens of micrometres, limited by the chain length. The spatial coherence of the k=0 exciton state is demonstrated by selecting two spatially separated emitting regions of the chain and observing their interference.

This is a preview of subscription content, access via your institution

Access options

Buy this article

USD 39.95

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Microscopic imaging spectroscopy of a single chain.
Figure 2: Interference pattern of a single-chain emission.

Similar content being viewed by others

References

  1. Yarmuck, E. J., Gordon, M. J. V. & Packard, R. E. Observation of stationary vortex arrays in rotating superfluid helium. Phys. Rev. Lett. 43, 214–217 (1979).

    Article  ADS  Google Scholar 

  2. Simsarian, J. E. et al. Imaging the phase of an evolving Bose-Einstein condensate wave function. Phys. Rev. Lett. 85, 2040–2043 (2000).

    Article  ADS  Google Scholar 

  3. Savvidis, P. G. & Lagoudakis, P. G. Teaching polaritons new tricks. Semicond. Sci. Technol. 18, S311–S318 (2003).

    Article  ADS  Google Scholar 

  4. Bloch, J. et al. Monitoring the dynamics of a coherent cavity polariton population. Phys. Rev. B 71, 155311 (2005).

    Article  ADS  Google Scholar 

  5. Butov, L. V., Gossard, A. C. & Chemla, D. S. Macroscopically ordered state in an exciton system. Nature 418, 751–754 (2002).

    Article  ADS  Google Scholar 

  6. Snoke, D., Denev, S., Liu, Y., Pfeiffer, L. & West, K. Long-range transport in excitonic dark states in coupled quantum wells. Nature 418, 754–757 (2002).

    Article  ADS  Google Scholar 

  7. Dubin, F. et al. Optical evidence of a purely one-dimensional exciton density of states in a single conjugated polymer chain. Phys. Rev. B 66, 113202 (2002).

    Article  ADS  Google Scholar 

  8. Lécuiller, R. et al. Fluorescence yield and lifetime of isolated polydiacetylene chains: evidence of a one-dimensional exciton band in a conjugated polymer. Phys. Rev. B 66, 125205 (2002).

    Article  ADS  Google Scholar 

  9. Schott, M. in Photophysics of Molecular Materials. From Single Molecules to Single Crystals (ed. Lanzani, G.) (Wiley–VCH, Berlin, in the press).

  10. Sariciftci, N. S. (ed.) Primary Photoexcitations in Conjugated Polymers: Molecular Excitons Versus Semiconductor Band Model (World Scientific, Singapore, 1997).

  11. Lécuiller, R., Berréhar, J., Lapersonne-Meyer, C. & Schott, M. Dual resonance fluorescence of polydiacetylene chains isolated in their crystalline monomer matrix. Phys. Rev. Lett. 80, 4068–4071 (1998).

    Article  ADS  Google Scholar 

  12. Guillet, T. et al. Emission of a single conjugated polymer chain isolated in its single crystal monomer matrix. Phys. Rev. Lett. 87, 087401 (2001).

    Article  ADS  Google Scholar 

  13. Haacke, S., Berréhar, J., Lapersonne-Meyer, C. & Schott, M. Dynamics of singlet excitons in one-dimensional conjugated polydiacetylene chains: a femtosecond fluorescence study. Chem. Phys. Lett. 308, 363–368 (1999).

    Article  ADS  Google Scholar 

  14. Dubin, F., Berréhar, J., Grousson, R., Schott, M. & Voliotis, V. Evidence of polariton induced transparency in a single organic quantum wire. Preprint at < http://arxiv.org/abs/cond-mat/0508602> 2005.

  15. Pulizzi, F., Thijssen, W. H. A., Christianen, P. C. M. & Maan, J. C. Diffusion of two-dimensional magnetoexcitons. Physica B 298, 441–445 (2001).

    Article  ADS  Google Scholar 

  16. Hopfield, J. J. Theory of the contribution of excitons to the complex dielectric constant of crystals. Phys. Rev. 112, 1555–1567 (1958).

    Article  ADS  Google Scholar 

  17. Citrin, D. S. Long intrinsic radiative lifetimes of excitons in quantum wires. Phys. Rev. Lett. 69, 3393–3396 (1992) ibid Phys. Rev. Lett. 70, 1186 (1993).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

This work has been supported by the Region Ile de France (SESAME NE. 1751).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Valia Voliotis.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Dubin, F., Melet, R., Barisien, T. et al. Macroscopic coherence of a single exciton state in an organic quantum wire. Nature Phys 2, 32–35 (2006). https://doi.org/10.1038/nphys196

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue date:

  • DOI: https://doi.org/10.1038/nphys196

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing