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.

Possible light-induced superconductivity in K3C60 at high temperature

Nature volume 530, pages 461–464 (2016)Cite this article

Subjects

This article has been updated

Abstract

The non-equilibrium control of emergent phenomena in solids is an important research frontier, encompassing effects such as the optical enhancement of superconductivity1. Nonlinear excitation2,3 of certain phonons in bilayer copper oxides was recently shown to induce superconducting-like optical properties at temperatures far greater than the superconducting transition temperature, Tc (refs 4, 5, 6). This effect was accompanied by the disruption of competing charge-density-wave correlations7,8, which explained some but not all of the experimental results. Here we report a similar phenomenon in a very different compound, K3C60. By exciting metallic K3C60 with mid-infrared optical pulses, we induce a large increase in carrier mobility, accompanied by the opening of a gap in the optical conductivity. These same signatures are observed at equilibrium when cooling metallic K3C60 below Tc (20 kelvin). Although optical techniques alone cannot unequivocally identify non-equilibrium high-temperature superconductivity, we propose this as a possible explanation of our results.

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

Relevant articles

Open Access articles citing this article.

Access options

Rent or buy this article

Prices vary by article type

from$1.95

to$39.95

Learn more

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

Figure 1: Structure and equilibrium optical properties of K3C60.
Figure 2: Transient optical response of photo-excited K3C60 at T = 25 K and T = 100 K.
Figure 3: Transient optical response of photo-excited K3C60 at T = 200 K and T = 300 K.
Figure 4: Scaling of the σ1(ω) gap with experimental parameters.

Change history

  • 24 February 2016

    The final sentence of the Fig. 4 legend was inadvertently truncated in the PDF of the AOP version, but has now been corrected.

References

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

    Article  CAS  ADS  Google Scholar 

  2. Mankowsky, R. et al. Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5 . Nature 516, 71–73 (2014)

    Article  CAS  ADS  Google Scholar 

  3. Mankowsky, R. et al. Coherent modulation of the YBa2Cu3O6+x atomic structure by displacive stimulated ionic Raman scattering. Phys. Rev. B 91, 094308 (2015)

    Article  ADS  Google Scholar 

  4. Kaiser, S. et al. Optically-induced coherent transport far above T c in underdoped YBa2Cu3O6+δ . Phys. Rev. B 89, 184516 (2014)

    Article  ADS  Google Scholar 

  5. Hu, W. et al. Optically enhanced coherent transport in YBa2Cu3O6.5 by ultrafast redistribution of interlayer coupling. Nature Mater . 13, 705–711 (2014)

    Article  CAS  ADS  Google Scholar 

  6. Hunt, C. R. et al. Two distinct kinetic regimes in the relaxation of light induced superconductivity in La1.675Eu0.2Sr0.125CuO4 . Phys. Rev. B 91, 020505 (2015)

    Article  ADS  Google Scholar 

  7. Först, M. et al. Melting of charge stripes in vibrationally driven La1.875Ba0.125CuO4: assessing the respective roles of electronic and lattice order in frustrated superconductors. Phys. Rev. Lett. 112, 157002 (2014)

    Article  ADS  Google Scholar 

  8. Först, M. et al. Femtosecond X-rays link melting of charge density wave correlations and light enhanced coherent transport in YBa2Cu3O6.6 . Phys. Rev. B 90, 184514 (2014)

    Article  ADS  Google Scholar 

  9. Gunnarsson, O. Alkali-doped Fullerides: Narrow-band Solids with Unusual Properties (World Scientific, 2004)

  10. Hebard, A. F. et al. Superconductivity at 18 K in potassium-doped C60 . Nature 350, 600–601 (1991)

    Article  CAS  ADS  Google Scholar 

  11. Xiang, X.-D. et al. Synthesis and electronic transport of single crystal K3C60 . Science 256, 1190–1191 (1992)

    Article  CAS  ADS  Google Scholar 

  12. Chakravarty, S., Gelfand, M. P. & Kivelson, S. Electronic correlation effects and superconductivity in doped fullerenes. Science 254, 970–974 (1991)

    Article  CAS  ADS  Google Scholar 

  13. Capone, M. et al. Strongly correlated superconductivity. Science 296, 2364–2366 (2002)

    Article  CAS  ADS  Google Scholar 

  14. Varma, C. M., Zaanen, J. & Raghavachari, K. Superconductivity in the fullerenes. Science 254, 989–992 (1991)

    Article  CAS  ADS  Google Scholar 

  15. Schluter, M. et al. Electron-phonon coupling and superconductivity in alkali-intercalated C60 solid. Phys. Rev. Lett. 68, 526–529 (1992)

    Article  CAS  ADS  Google Scholar 

  16. Han, J. E., Gunnarson, O. & Crespi, V. H. Strong superconductivity with local Jahn Teller phonons in C60 solids. Phys. Rev. Lett. 90, 167006 (2003)

    Article  CAS  ADS  Google Scholar 

  17. Degiorgi, L. et al. Optical properties of the alkali-metal-doped superconducting fullerenes: K3C60 and Rb3C60 . Phys. Rev. B 49, 7012–7025 (1994)

    Article  CAS  ADS  Google Scholar 

  18. Degiorgi, L. et al. Optical measurements of the superconducting gap in single-crystal K3C60 and Rb3C60 . Nature 369, 541–543 (1994)

    Article  CAS  ADS  Google Scholar 

  19. Degiorgi, L. The complete excitation spectrum of the alkali-metal-doped superconducting fullerenes. Mod. Phys. Lett. B 9, 445–468 (1995)

    Article  CAS  ADS  Google Scholar 

  20. Rice, M. G. & Choi, H.-Y. Charged-phonon absorption in doped C60 . Phys. Rev. B 45, 10173–10176 (1992)

    Article  CAS  ADS  Google Scholar 

  21. Zimmermann, W. et al. Optical conductivity of BCS superconductors with arbitrary purity. Physica C 183, 99–104 (1991)

    Article  ADS  Google Scholar 

  22. Först, M. et al. Nonlinear phononics as a new ultrafast route to lattice control. Nature Phys . 7, 854–856 (2011)

    Article  ADS  Google Scholar 

  23. Subedi, A., Cavalleri, A. & Georges A. Theory of nonlinear phononics for coherent light control of solids. Phys. Rev. B 89, 220301(R) (2014)

    Article  ADS  Google Scholar 

  24. Kaiser, S. et al. Optical properties of a vibrationally modulated solid state Mott insulator. Sci. Rep. 4, 3823 (2014)

    Article  CAS  Google Scholar 

  25. Singla, R. et al. THz-frequency modulation of the Hubbard U in an organic Mott insulator. Phys. Rev. Lett. 115, 187401 (2015)

    Article  CAS  ADS  Google Scholar 

  26. Stephens, P. W. et al. Structure of single-phase superconducting K3C60 . Nature 351, 632–634 (1991)

    Article  CAS  ADS  Google Scholar 

  27. Lupi, S. et al. Performance of SISSI, the infrared beamline of the ELETTRA storage ring. J. Opt. Soc. Am. B 24, 959–964 (2007)

    Article  CAS  ADS  Google Scholar 

  28. Plaskett, J. S. & Schatz, P. N. On the Robinson and Price (Kramers-Kronig) method of interpreting reflection data taken through a transparent window. J. Chem. Phys. 38, 612–617 (1963)

    Article  CAS  ADS  Google Scholar 

  29. Brito Cruz, C. H. et al. Dynamics of spectral hole burning. IEEE J. Quantum Electron. 24, 261–269 (1988)

    Article  ADS  Google Scholar 

  30. Orenstein, J. & Dodge, J. S. Terahertz time-domain spectroscopy of transient metallic and superconducting states. Phys. Rev. B 92, 134507 (2015)

    Article  ADS  Google Scholar 

  31. Beard, M. C., Turner, G. M. & Schmuttenmaer, C. A. Subpicosecond carrier dynamics in low-temperature grown GaAs as measured by time-resolved terahertz spectroscopy. J. Appl. Phys. 90, 5915–5923 (2001)

    Article  CAS  ADS  Google Scholar 

  32. Nicoletti, D., Mitrano, M., Cantaluppi, A. & Cavalleri, A. Comment on “Terahertz time-domain spectroscopy of transient metallic and superconducting states” (arXiv:1506.06758). Preprint at http://arXiv.org/abs/1506.07846 (2015)

  33. Iwasa, Y. & Kaneyasu, T. Optical study of electronic structures and phonons in alkali-metal-doped C60 . Phys. Rev. B 51, 3678–3685 (1995)

    Article  CAS  ADS  Google Scholar 

  34. Kuzmenko, A. et al. Gate tunable infrared phonon anomalies in bilayer graphene. Phys. Rev. Lett. 103, 116804 (2009)

    Article  CAS  ADS  Google Scholar 

  35. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996)

    Article  CAS  ADS  Google Scholar 

  36. Togo, A., Oba, F. & Tanaka, I. First-principles calculations of the ferroelastic transition between rutile-type and CaCl2-type SiO2 at high pressures. Phys. Rev. B 78, 134106 (2008)

    Article  ADS  Google Scholar 

  37. Giannozzi, P. et al. QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials. J. Phys. Condens. Matter 21, 395502 (2009)

    Article  Google Scholar 

  38. Laouini, N., Andersen, O. K. & Gunnarsson, O. Analytical molecular orbitals and band structures of solid C60 . Phys. Rev. B 51, 17446–17478 (1995)

    Article  Google Scholar 

  39. Hands, I. D., Dunn, J. L. & Bates, C. A. A complete nearest-neighbor force field model for C60 . J. Chem. Phys. 120, 6912–6921 (2004)

    Article  CAS  ADS  Google Scholar 

  40. Antropov, V. P., Gunnarsson, O. & Jespen, O. Coulomb integrals and model Hamiltonians for C60 . Phys. Rev. B 46, 13647–13650 (1992)

    Article  CAS  ADS  Google Scholar 

Download references

Acknowledgements

We acknowledge S. Kivelson and A. Georges for discussion. We are also grateful to A. Subedi for sharing microscopic calculations of anharmonic mode coupling. We thank L. Degiorgi for sharing optical data measured on single crystals. Technical support during sample handling was provided by H.-P. Liermann and M. Wendt. We additionally acknowledge support from M. Gaboardi (for SQUID magnetometry) and from J. Harms (for graphics). The research leading to these results received funding from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007-2013)/ERC Grant Agreement no. 319286 (QMAC). We acknowledge support from the Deutsche Forschungsgemeinschaft via the excellence cluster ‘The Hamburg Centre for Ultrafast Imaging — Structure, Dynamics and Control of Matter at the Atomic Scale’ and the priority program SFB925. This work was also supported by the Swiss National Supercomputing Center (CSCS) under the project ID s497.

Author information

Authors and Affiliations

  1. Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761, Hamburg, Germany

    M. Mitrano, A. Cantaluppi, D. Nicoletti, S. Kaiser, S. R. Clark & A. Cavalleri

  2. The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, Hamburg, 22761, Germany

    A. Cantaluppi, D. Nicoletti & A. Cavalleri

  3. INSTM UdR Trieste-ST and Elettra–Sincrotrone Trieste S.C.p.A., Area Science Park, Basovizza, 34012, Trieste, Italy

    A. Perucchi & P. Di Pietro

  4. CNR-IOM and Dipartimento di Fisica, Università di Roma “Sapienza”, Piazzale A. Moro 2, Roma, 00185, Italy

    S. Lupi

  5. Dipartimento di Fisica e Scienze della Terra, Università degli Studi di Parma, Parco Area delle Scienze, 7/a, Parma, 43124, Italy

    D. Pontiroli & M. Riccò

  6. Department of Physics, University of Bath, Claverton Down, Bath, BA2 7AY, UK

    S. R. Clark

  7. Department of Physics, Oxford University, Clarendon Laboratory, Parks Road, Oxford, OX1 3PU, UK

    S. R. Clark, D. Jaksch & A. Cavalleri

  8. Centre for Quantum Technologies, National University of Singapore, 3 Science Drive 2, Singapore, 117543, Singapore

    D. Jaksch

Authors
  1. M. Mitrano
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. A. Cantaluppi
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. D. Nicoletti
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. S. Kaiser
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. A. Perucchi
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. S. Lupi
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. P. Di Pietro
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. D. Pontiroli
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. M. Riccò
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. S. R. Clark
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. D. Jaksch
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. A. Cavalleri
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

A. Cavalleri conceived the project and the experiments together with M.M. and S.K. The time-resolved THz set-up was built by M.M. and A. Cantaluppi, who performed the pump–probe measurements and analysed the data with support from D.N. and S.K. Equilibrium optical properties were measured and analysed by M.M. and A. Cantaluppi, with support from A.P., S.L. and P.D.P. Samples were grown and characterized by D.P. and M.R. S.R.C. and D.J. provided calculations of time-dependent on-site correlation energies. The manuscript was written by A. Cavalleri, D.N. and M.M., with input from all authors.

Corresponding author

Correspondence to A. Cavalleri.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Extended data figures and tables

Extended Data Figure 1 K3C60 sample characterization.

a, Powder X-ray diffraction of K3C60 (black circles) fitted with a single f.c.c. phase Rietveld refinement (red). Positions of reflections are shown in green, fit residuals are in grey. b, Temperature dependent magnetic susceptibility, χm (FCC, field-cooled cooling; ZFC, zero-field cooling). The extracted superconducting transition temperature is Tc = 19.8 K.

Extended Data Figure 2 ‘Raw’ electric field transients below and above Tc.

a–d, Stationary electric field (a, c; grey) reflected at the sample–diamond interface, ER(t), and pump-induced changes in the same quantity, ΔER(t, τ), measured at τ = 3 ps (b) and at τ = 1 ps (d). Data are shown both below (blue) and above Tc (red). e, f, Corresponding frequency-dependent differential changes in reflectivity, ΔER/ER(ω, τ), calculated as Fourier transform magnitude ratios of the quantities in a–d.

Extended Data Figure 3 Models for penetration depth mismatch.

a, Schematics of pump–probe penetration depth mismatch. b, c, Also shown are the single-layer model (b) and the multi-layer model with exponential decay (c) (see Methods) used to calculate the pump-induced changes in the complex refractive index, . d–f, Reflectivity, R(ω), and complex optical conductivity, σ(ω), of K3C60 at τ = 1 ps pump–probe delay and T = 25 K, extracted using the single-layer model (light blue) and the multi-layer model with exponential decay (dark blue).

Extended Data Figure 4 Equilibrium optical properties.

a, Reflectivity (left column), and real and imaginary parts (respectively middle and right columns) of the optical conductivity of K3C60 displayed at different temperatures above Tc. Dashed lines are fits to the 25 K data performed with a Drude–Lorentz model. b, Same quantities displayed at different T < Tc. In the inset, the temperature dependent optical gap (filled circles) is compared with previously published data on K3C60 single crystals (open circles18). c, Optical properties of compressed powders of K3C60 from a and b shown at representative temperatures below and above Tc. The R(ω) has been recalculated at the sample–vacuum interface. d, Same quantities as in c, measured on single crystals18.

Extended Data Figure 5 Uncertainties in determining the transient optical properties.

Columns as Extended Data Fig. 4; shown are values for K3C60 at equilibrium (red) and 1 ps after photo-excitation (blue) at T = 25 K. Error bars, displayed as coloured bands, have been propagated as follows: a, ±1% and ±2.5% uncertainty in the equilibrium R(ω); b, ±10% uncertainty in the equilibrium Fresnel phase coefficient β (see Methods); c, ±25% change in the pump penetration depth d = 220 nm. In d we analyse the effect of different functional forms for modelling the pump–probe penetration depth mismatch (see Methods): a single-layer model, or a multi-layer model with exponential decay or with Gaussian-like decay, all with the same pump penetration depth d = 220 nm.

Extended Data Figure 6 Relaxation dynamics at T > Tc.

Reflectivity (left column) and complex optical conductivity (middle and right columns) of K3C60 at equilibrium (grey) and after photo-excitation (red) at T = 25 K. Data have been measured with a pump fluence of ~1 mJ cm−2 and are shown at selected pump–probe time delays: 1.5 ps, 5.5 ps and 21 ps (top, middle and bottom rows, respectively). Hatched areas highlight pump-induced changes.

Extended Data Figure 7 Mode coupling and electronic structure calculations.

a, Calculated total energy curves as a function of Hg(1) mode amplitude () when the amplitude of the T1u(4) mode is 0.0 (blue) and 2.0 Å √amu (red). b, Calculated band structure and electronic density of states N(E) of K3C60. c, Calculated electron–phonon coupling function, α2F(ω). In b and c, blue lines are for the equilibrium structure and red lines are for the structure displaced along the Hg(1) coordinate with an amplitude of 1.5 Å √amu. d, Differential changes in the electron–phonon coupling function, evaluated from the curves in c.

Extended Data Figure 8 Changes in time of single particle energy and Coulomb repulsion.

a, Depiction of the x, y, z t1u orbital wavefunctions of C60 according to the Hückel model (left, middle and right column respectively, see Methods). Sphere sizes denote the magnitude of the wavefunction and colours indicate the sign. b, Snapshots of the calculated t1u(z) orbital at various points in the T1u(4) vibration polarized along the x axis. Colours and sizes follow those of a. c, Changes in the single-particle energies, εi, of the t1u orbitals over one period of the T1u(4) vibration with an amplitude A = 5 pm. d, Relative changes in the intra-orbital Coulomb repulsions, Ui/Ui(0). e, Maximum relative changes in the single-particle energies of the t1u orbitals, εi/εi(0), as a function the driving amplitude, A. f, Relative changes in the intra-orbital Coulomb repulsions, Ui/Ui(0), under the same driving conditions.

Extended Data Figure 9 Response at early time delays below and above Tc.

Reflectivity, R(ω), and complex optical conductivity, σ(ω), of K3C60 at equilibrium (red, dark blue) and 1 ps after photo-excitation (light blue), measured at T > Tc (a–c) and T < Tc (d–f). Data were taken using pump fluences of ~1 mJ cm−2 in a–c and ~0.5 mJ cm−2 in d–f. Hatched areas highlight pump-induced changes.

Extended Data Figure 10 Relaxation dynamics at T < Tc.

Columns as Extended Data Fig. 9; data were measured at equilibrium (grey) and after photo-excitation (red) at T = 10 K, with a pump fluence of ~0.5 mJ cm−2. Data are shown at selected pump–probe time delays: 3 ps (top row), 11 ps (middle row) and 21 ps (bottom row). Hatched areas highlight pump-induced changes.

PowerPoint slides

Rights and permissions

Reprints and Permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Mitrano, M., Cantaluppi, A., Nicoletti, D. et al. Possible light-induced superconductivity in K3C60 at high temperature. Nature 530, 461–464 (2016). https://doi.org/10.1038/nature16522

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature16522

This article is cited by

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

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