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:

Nonlinear charge oscillation driven by a single-cycle light field in an organic superconductor

Nature Photonics volume 12, pages 474–478 (2018)Cite this article

Subjects

Abstract

Application of an intense light field to solids produces enormous and ultrafast nonlinear phenomena such as high-harmonic generation1,2 and attosecond charge dynamics3,4. These are distinct from conventional photonics. However, the main targets for investigation have been limited to insulators and semiconductors, although theoretical approaches have also been developed for correlated metals and superconductors5. Here, in a layered organic superconductor, a nonlinear charge oscillation driven by a nearly single-cycle strong electric field of >10 MV cm−1 is observed as a stimulated emission. The charge oscillation is different from a linear response and ascribed to a polar charge oscillation with a period of ∼6 fs. This nonlinear polar charge oscillation is enhanced by critical fluctuations near a superconducting transition temperature and a critical end-point of first-order Mott transitions. Its observation on an ultrafast timescale of ∼10 fs clarifies that Coulomb repulsion plays an essential role in the superconductivity of organic superconductors.

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

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

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

Fig. 1: Temperature–t/Udimer phase diagram and nonlinear charge oscillation.
Fig. 2: Transient reflectivity(ΔR/R) and transmittance (ΔT/T) spectra.
Fig. 3: Nonlinearity of transient reflectivity.
Fig. 4: Anomalous enhancement of ΔR/R near TSC and TEND.
Fig. 5: Origin of nonlinear charge oscillation in a 2D extended Hubbard model.

Similar content being viewed by others

References

  1. Schubert, O. et al. Sub-cycle control of terahertz high-harmonic generation by dynamical Bloch oscillations. Nat. Photon. 8, 119–123 (2014).

    Article  ADS  Google Scholar 

  2. Luu, T. T. et al. Extreme ultraviolet high-harmonic spectroscopy of solids. Nature 521, 498–502 (2015).

    Article  ADS  Google Scholar 

  3. Schultze, M. et al. Attosecond band-gap dynamics in silicon. Science 346, 1348–1352 (2014).

    Article  ADS  Google Scholar 

  4. Lucchini, M. et al. Attosecond dynamical Franz–Keldysh effect in polycrystalline diamond. Science 353, 916–919 (2016).

    Article  ADS  Google Scholar 

  5. Aoki, H. et al. Nonequilibrium dynamical mean-field theory and its applications. Rev. Mod. Phys. 86, 779–837 (2014).

    Article  ADS  Google Scholar 

  6. Huber, R. et al. How many-particle interactions develop after ultrafast excitation of an electron–hole plasma. Nature 414, 286–289 (2001).

    Article  ADS  Google Scholar 

  7. Hase, M., Kitajima, M., Constantinescu, A. M. & Petek, H. The birth of a quasiparticle in silicon observed in time–frequency space. Nature 426, 51–54 (2003).

    Article  ADS  Google Scholar 

  8. Basov, D. N. et al. Electrodynamics of correlated electron materials. Rev. Mod. Phys. 83, 471–541 (2011).

    Article  ADS  Google Scholar 

  9. Schoenlein, R. W., Lin, W. Z., Fujimoto, J. G. & Eesley, G. L. Femtosecond studies of nonequilibrium electronic processes in metals. Phys. Rev. Lett. 58, 1680–1683 (1987).

    Article  ADS  Google Scholar 

  10. Han, S. G. et al. Femtosecond optical detection of quasiparticle dynamics in high-T c YBa2Cu3O7−δ superconducting thin films. Phys. Rev. Lett. 65, 2708–2711 (1990).

    Article  ADS  Google Scholar 

  11. Demsar, J. et al. Superconducting gap Δ c, the pseudogap Δ p, and pair fluctuations above T c in overdoped Y1 − xCaxBa2Cu3O7 − δ from femtosecond time-domain spectroscopy. Phys. Rev. Lett. 82, 4918–4921 (1999).

    Article  ADS  Google Scholar 

  12. Kaindl, R. A. et al. Ultrafast mid-infrared response of YBa2Cu3O7 − δ. Science 287, 470–473 (2000).

    Article  ADS  Google Scholar 

  13. Toda, Y., Mertelj, T., Naito, T. & Mihailovic, D. Femtosecond carrier relaxation dynamics and photoinduced phase separation in κ-(BEDT-TTF)2Cu[N(CN)2]X (X = Br, Cl). Phys. Rev. Lett. 107, 227002 (2011).

    Article  ADS  Google Scholar 

  14. Giannetti, C. et al. Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach. Adv. Phys. 65, 58–238 (2016).

    Article  ADS  Google Scholar 

  15. Ishikawa, T. et al. Optical freezing of charge motion in an organic conductor. Nat. Commun. 5, 5528 (2014).

    Article  Google Scholar 

  16. Fukaya, R. et al. Ultrafast electronic state conversion at room temperature utilizing hidden state in cuprate ladder system. Nat. Commun. 6, 8519 (2015).

    Article  Google Scholar 

  17. Matsunaga, R. et al. Light-induced collective pseudospin precession resonating with Higgs mode in a superconductor. Science 345, 1145–1149 (2014).

    Article  ADS  MathSciNet  MATH  Google Scholar 

  18. Fausti, D. et al. Light-induced superconductivity in a stripe-ordered cuprate. Science 331, 189–191 (2011).

    Article  ADS  Google Scholar 

  19. Imada, M., Fujimori, A. & Tokura, Y. Metal–insulator transitions. Rev. Mod. Phys. 70, 1039–1263 (1998).

    Article  ADS  Google Scholar 

  20. Kanoda, K. Recent progress in NMR studies on organic conductors. Hyperfine Interact. 104, 235–249 (1997).

    Article  ADS  Google Scholar 

  21. Kagawa, F., Miyagawa, K. & Kanoda, K. Unconventional critical behavior in a quasi-two-dimensional organic conductor. Nature 436, 534–537 (2005).

    Article  ADS  Google Scholar 

  22. Powell, B. J. & McKenzie, R. H. Strong electronic correlations in superconducting organic charge transfer salts. J. Phys. Condens. Matter 18, R827–R866 (2006).

    Article  ADS  Google Scholar 

  23. Terletska, H., Vučičević, J., Tanasković, D. & Dobrosavljević, V. Quantum critical transport near the Mott transition. Phys. Rev. Lett. 107, 026401 (2011).

    Article  ADS  Google Scholar 

  24. Sasaki, T. et al. Electronic correlation in the infrared optical properties of the quasi-two-dimensional κ-type BEDT-TTF dimer system. Phys. Rev. B 69, 064508 (2004).

    Article  ADS  Google Scholar 

  25. Faltermeier, D. et al. Bandwidth-controlled Mott transition in κ-(BEDT-TTF)2Cu[N(CN)2]BrxCl1−x: optical studies of localized charge excitations. Phys. Rev. B 76, 165113 (2007).

    Article  ADS  Google Scholar 

  26. Dressel, M. & Drichiko, N. Optical properties of two-dimensional organic conductors: signatures of charge ordering and correlation effects. Chem. Rev. 104, 5689–5715 (2004).

    Article  Google Scholar 

  27. Yamamoto, H. M. et al. A strained organic field-effect transistor with a gate-tunable superconducting channel. Nat. Commun. 4, 2379 (2013).

    Article  Google Scholar 

  28. Sekine, A., Nasu, J. & Ishihara, S. Polar charge fluctuation and superconductivity in organic conductors. Phys. Rev. B 87, 085133 (2013).

    Article  ADS  Google Scholar 

  29. Watanabe, H., Seo, H. & Yunoki, S. Phase competition and superconductivity in κ-(BEDT-TTF)2X: importance of intermolecular Coulomb interactions. J. Phys. Soc. Jpn 86, 033703 (2017).

    Article  ADS  Google Scholar 

  30. Kawakami, Y. et al. Polarization selectivity of charge localization induced by a 7-fs nearly single-cycle lightfield in an organic metal. Phys. Rev. B 95, 201105(R) (2017).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

This work was supported by the Japan Science and Technology Agency (Core Research for Evolutional Science and Technology (CREST: Elucidation of elementary dynamics of photoinduced phase transition by using advanced ultrashort light pulses) and Exploratory Research for Advanced Technology (ERATO: JPMJER1301)) and the Japan Society for the Promotion of Science (grant numbers JP15H02100, JP23244062, JP16K13814, JP17K14317, JP26887003, JP16K05459, JP25287080, JP26287070, JP17H02916 and JP16H04140). Part of the work was conducted in the Equipment Development Center (Institute for Molecular Science), supported by the Nanotechnology Platform Program (Molecule and Material Synthesis) of the Ministry of Education, Culture, Sports, Science and Technology, Japan.

Author information

Authors and Affiliations

  1. Department of Physics, Tohoku University, Sendai, Japan

    Y. Kawakami, T. Amano, Y. Yoneyama, Y. Akamine, H. Itoh, S. Ishihara & S. Iwai

  2. Institute for Molecular Science, Okazaki, Japan

    G. Kawaguchi & H. M. Yamamoto

  3. Department of Applied Physics, Nagoya University, Nagoya, Japan

    H. Kishida

  4. Institute for Materials Research, Tohoku University, Sendai, Japan

    K. Itoh & T. Sasaki

  5. Department of Physics, Chuo University, Tokyo, Japan

    Y. Tanaka & K. Yonemitsu

Authors
  1. Y. Kawakami
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. T. Amano
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Y. Yoneyama
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Y. Akamine
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. H. Itoh
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. G. Kawaguchi
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. H. M. Yamamoto
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. H. Kishida
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. K. Itoh
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. T. Sasaki
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. S. Ishihara
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Y. Tanaka
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. K. Yonemitsu
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. S. Iwai
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Y.K., T.A., Y.Y., Y.A., H.I. and S.Iw. developed the 6 fs light source, carried out the transient reflectivity/transmittance measurements using the 6 fs pulse and, with contributions from H.K., analysed the data. G.K. and H.M.Y. performed the synthesis and characterization of the thin film. K.I., H.K. and T.S. performed the synthesis and characterization of the single crystal. S.Is., Y.T. and K.Y. made theoretical considerations and calculations. S.Iw. devised all of the experiments. Y.K., K.Y. and S.Iw. wrote the paper after discussions with all co-authors.

Corresponding author

Correspondence to S. Iwai.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary notes and figures.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Kawakami, Y., Amano, T., Yoneyama, Y. et al. Nonlinear charge oscillation driven by a single-cycle light field in an organic superconductor. Nature Photon 12, 474–478 (2018). https://doi.org/10.1038/s41566-018-0194-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41566-018-0194-4

This article is cited by

Search

Advanced 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