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:

Transient photoinduced ‘hidden’ phase in a manganite

Abstract

Photoinduced phase transitions are of special interest in condensed matter physics1,2 because they can be used to change complex macroscopic material properties on the ultrafast timescale. Cooperative interactions between microscopic degrees of freedom greatly enhance the number and nature of accessible states, making it possible to switch electronic, magnetic or structural properties in new ways2,3,4,5,6,7,8,9. Photons with high energies, of the order of electron volts, in particular are able to access electronic states that may differ greatly from states produced with stimuli close to equilibrium10. In this study we report the photoinduced change in the lattice structure of a charge and orbitally ordered Nd0.5Sr0.5MnO3 thin film using picosecond time-resolved X-ray diffraction. The photoinduced state is structurally ordered, homogeneous, metastable and has crystallographic parameters different from any thermodynamically accessible state. A femtosecond time-resolved spectroscopic study shows the formation of an electronic gap in this state. In addition, the threshold-like behaviour and high efficiency in photo-generation yield of this gapped state highlight the important role of cooperative interactions in the formation process. These combined observations point towards a ‘hidden insulating phase’ distinct from that found in the hitherto known phase diagram.

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

Access options

Buy this article

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

Figure 1: X-ray diffraction patterns for M and CO–OO phases.
Figure 2: Photoinduced structural changes at 100 K triggered by irradiation with a 130-fs laser pulse.
Figure 3: Photoinduced spectroscopic change at 100 K triggered by irradiation with a 130-fs laser pulse.
Figure 4: Schematic illustration contrasting the orbital character of a photoinduced hidden phase with that of a thermally induced M phase converted from the initial CO–OO state (ground state).

Similar content being viewed by others

References

  1. Tokura, Y. Photoinduced phase transition: A tool for generating a hidden state of matter. J. Phys. Soc. Jpn 75, 011001 (2006).

    Article  Google Scholar 

  2. Nasu, K. Photoinduced Phase Transitions (World Scientific, 2004).

    Book  Google Scholar 

  3. Vahaplar, K. et al. Ultrafast path for optical magnetization reversal via a strongly nonequilibrium state. Phys. Rev. Lett. 103, 117201 (2009).

    Article  CAS  Google Scholar 

  4. Lorenc, M. et al. Successive dynamical steps of photoinduced switching of a molecular Fe(III) spin-crossover material by time-resolved X-ray diffraction. Phys. Rev. Lett. 103, 028301 (2009).

    Article  CAS  Google Scholar 

  5. Rini, M. et al. Control of the electronic phase of a manganite by mode-selective vibrational excitation. Nature 449, 72–74 (2007).

    Article  CAS  Google Scholar 

  6. Collet, E. et al. Laser-induced ferroelectric structural order in an organic charge-transfer crystal. Science 300, 612–615 (2003).

    Article  CAS  Google Scholar 

  7. Cavalleri, A., Rini, M & Schoenlein, R. W. Ultra-broadband femtosecond measurements of the photo-induced phase transition in VO2: From the mid-IR to the hard X-rays. J. Phys. Soc. Jpn 75, 011004 (2006).

    Article  Google Scholar 

  8. Kolobov, A. V. et al. Understanding the phase-change mechanism of rewritable optical media. Nature Mater. 3, 703–708 (2004).

    Article  CAS  Google Scholar 

  9. Koshihara, S. & Adachi, S. Photo-induced phase transition in an electron–lattice correlated system—future role of a time-resolved X-ray measurement for materials science. J. Phys. Soc. Jpn 75, 011005 (2006).

    Article  Google Scholar 

  10. Huai, P. & Nasu, K. Difference between photoinduced phase and thermally excited phase. J. Phys. Soc. Jpn 71, 1182–1188 (2002).

    Article  CAS  Google Scholar 

  11. Kajimoto, R. et al. Hole-concentration-induced transformation of the magnetic and orbital structures in Nd1−xSrxMnO3 . Phys. Rev. B 60, 9506–9517 (1999).

    Article  CAS  Google Scholar 

  12. Okuyama, D. et al. Lattice-form-dependent orbital shape and charge disproportionation in charge- and orbital-ordered manganites. Phys. Rev. B 80, 064402 (2009).

    Article  Google Scholar 

  13. Tobe, K., Kimura, T. & Tokura, Y. Anisotropic optical spectra of doped manganites with pseudocubic perovskite structure. Phys. Rev. B 69, 014407 (2004).

    Article  Google Scholar 

  14. Ogimoto, Y. et al. Strain-induced crossover of the metal–insulator transition in perovskite manganites. Phys. Rev. B 71, 060403(R) (2005).

    Article  Google Scholar 

  15. Nakamura, M., Ogimoto, Y., Tamaru, H., Izumi, M. & Miyano, K. Phase control through anisotropic strain in Nd0.5Sr0.5MnO3 thin films. Appl. Phys. Lett. 86, 182504 (2005).

    Article  Google Scholar 

  16. Miyasaka, K., Nakamura, M., Ogimoto, Y., Tamaru, H. & Miyano, K. Ultrafast photoinduced magnetic moment in a charge–orbital-ordered antiferromagnetic Nd0.5Sr0.5MnO3 thin film. Phys. Rev. B 74, 012401 (2006).

    Article  Google Scholar 

  17. Wakabayashi, Y. et al. Size of orbital-ordering domain controlled by the itinerancy of the 3d electrons in a manganite thin film. Phys. Rev. B 79, 220403(R) (2009).

    Article  Google Scholar 

  18. Wakabayashi, Y. et al. Orbital ordering structures in (Nd,Pr)0.5Sr0.5MnO3 manganite thin films on perovskite (011) substrates. J. Phys. Soc. Jpn 77, 014712 (2008).

    Article  Google Scholar 

  19. Anisimov, V. I., Elfimov, I. S., Korotin, M. A. & Terakura, K. Orbital and charge ordering in Pr1−xCaxMnO3 (x=0 and 0.5) from the ab initio calculations. Phys. Rev. B 55, 15494–15499 (1997).

    Article  CAS  Google Scholar 

  20. Maezono, R., Ishihara, S. & Nagaosa, N. Phase diagram of manganese oxides. Phys. Rev. B 58, 11583–11596 (1998).

    Article  CAS  Google Scholar 

  21. Yunoki, S., Hotta, T. & Dagotto, E. Ferromagnetic, A-type, and charge-ordered CE-type states in doped manganites using Jahn–Teller phonons. Phys. Rev. Lett. 84, 3714–3717 (2000).

    Article  CAS  Google Scholar 

  22. Ebata, K., Mizokawa, T. & Fujimori, A. Orbital ordering in La0.5Sr1.5MnO4 studied by model Hartree–Fock calculation. Phys. Rev. B 72, 233104 (2005).

    Article  Google Scholar 

  23. Miyano, K., Tanaka, T., Tomioka, Y. & Tokura, Y. Photoinduced insulator-to-metal transition in a perovskite manganite. Phys. Rev. Lett. 78, 4257–4260 (1997).

    Article  CAS  Google Scholar 

  24. Dagotto, E. Springer Series in Solid-State Sciences 136 (Springer, 2003).

    Google Scholar 

  25. Matsubara, M. et al. Key for photoinduced insulator–metal transitions in manganites; lattice constant matching between charge/orbital ordered insulator and ferromagnetic metal. J. Phys. Soc. Jpn 78, 023707 (2009).

    Article  Google Scholar 

  26. Tamaru, H., Ishida, K, Ogawa, N., Kubo, Y. & Miyano, K. Pump-and-probe study in LaMnO3 thin films. Phys. Rev. B 78, 075119 (2008).

    Article  Google Scholar 

  27. Polli, D. et al. Coherent orbital waves in the photo-induced insulator–metal dynamics of a magnetoresistive manganite. Nature Mater. 6, 643–647 (2007).

    Article  CAS  Google Scholar 

  28. Satoh, K. & Ishihara, S. Photo-induced phase transition in charge ordered perovskite manganites. J. Magn. Magn. Mater. 310, 798–800 (2007).

    Article  CAS  Google Scholar 

  29. Kanamori, Y., Matsueda, H. & Ishihara, S. Dynamical coupling and separation of multiple degrees of freedom in a photoexcited double-exchange system. Phys. Rev. Lett. 103, 267401 (2009).

    Article  CAS  Google Scholar 

  30. Beaud, P. et al. Ultrafast structural phase transition driven by photoinduced melting of charge and orbital order. Phys. Rev. Lett. 103, 155702 (2009).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was partially supported by Grant-in-Aids for Scientific Research from the MEXT, Japan, and the G-COE programme for chemistry in Tokyo Institute of Technology. This work was carried out with the approval of the Photon Factory Program Advisory Committee (Proposal No. 2004S1-001). The authors thank Y. Okimoto (Tokyo Institute of Technology) for fruitful discussions.

Author information

Authors and Affiliations

Authors

Contributions

Sample preparation and optical measurements were carried out by Y.O., M.N., R.T. and K.M. H.I. planned the X-ray measurements and carried out the experiment and analysis. S.N., S-i.A., T-h.A. and H.S. planned, conducted and analysed the X-ray measurements; in addition, T.S., A.T., K.I., M.C. and L.G. assisted with the X-ray measurements. N.D. also assisted with the X-ray experiment under the supervision of A.C., as part of the G-COE student exchange program. All authors discussed the results and contributed to the manuscript. S-y.K. and K.M. initiated and oversaw the work.

Corresponding author

Correspondence to Shin-ya Koshihara.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 1314 kb)

Supplementary Video

Supplementary Video (MPG 5689 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Ichikawa, H., Nozawa, S., Sato, T. et al. Transient photoinduced ‘hidden’ phase in a manganite. Nature Mater 10, 101–105 (2011). https://doi.org/10.1038/nmat2929

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nmat2929

This article is cited by

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