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Title: Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4

Abstract

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity1, 2, 3, 4. Recently, photo-excitation has been used to induce similarly exotic states transiently5, 6, 7. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. In conclusion, the marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [5];  [1];  [1];  [6];  [7];  [7];  [7];  [1];  [4];  [4];  [4];  [4];  [4]; ORCiD logo [4];  [4] more »;  [4];  [8];  [9];  [10]; ORCiD logo [9];  [9];  [10];  [11]; ORCiD logo [12];  [13];  [14];  [15];  [6];  [5];  [1] « less
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Chinese Academy of Sciences (CAS), Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China)
  3. The Barcelona Institute of Science and Technology, Castelldefels (Barcelona) (Spain)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  6. Univ. College London, London (United Kingdom)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
  8. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  9. RIKEN SPring-8 Center, Hyogo (Japan)
  10. Japan Synchrotron Radiation Institute, Hyogo (Japan)
  11. Univ. of Tennessee, Knoxville, TN (United States)
  12. Univ. of California, Berkeley, CA (United States)
  13. Max Planck Institute for Solid State Research, Stuttgart (Germany)
  14. ETH Zurich, Zurich (Switzerland)
  15. Univ. of Groningen, Groningen (The Netherlands)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1311357
Report Number(s):
BNL-112461-2016-JA
Journal ID: ISSN 1476-1122; R&D Project: PO011; KC0201060
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 15; Journal Issue: 6; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Dean, M. P. M., Cao, Y., Liu, X., Wall, S., Zhu, D., Mankowsky, R., Thampy, V., Chen, X. M., Vale, J. G., Casa, D., Kim, Jungho, Said, A. H., Juhas, P., Alonso-Mori, R., Glownia, J. M., Robert, A., Robinson, J., Sikorski, M., Song, S., Kozina, M., Lemke, H., Patthey, L., Owada, S., Katayama, T., Yabashi, M., Tanaka, Yoshikazu, Togashi, T., Liu, J., Rayan Serrao, C., Kim, B. J., Huber, L., Chang, C. -L., McMorrow, D. F., Forst, M., and Hill, J. P. Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4. United States: N. p., 2016. Web. https://doi.org/10.1038/NMAT4641.
Dean, M. P. M., Cao, Y., Liu, X., Wall, S., Zhu, D., Mankowsky, R., Thampy, V., Chen, X. M., Vale, J. G., Casa, D., Kim, Jungho, Said, A. H., Juhas, P., Alonso-Mori, R., Glownia, J. M., Robert, A., Robinson, J., Sikorski, M., Song, S., Kozina, M., Lemke, H., Patthey, L., Owada, S., Katayama, T., Yabashi, M., Tanaka, Yoshikazu, Togashi, T., Liu, J., Rayan Serrao, C., Kim, B. J., Huber, L., Chang, C. -L., McMorrow, D. F., Forst, M., & Hill, J. P. Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4. United States. https://doi.org/10.1038/NMAT4641
Dean, M. P. M., Cao, Y., Liu, X., Wall, S., Zhu, D., Mankowsky, R., Thampy, V., Chen, X. M., Vale, J. G., Casa, D., Kim, Jungho, Said, A. H., Juhas, P., Alonso-Mori, R., Glownia, J. M., Robert, A., Robinson, J., Sikorski, M., Song, S., Kozina, M., Lemke, H., Patthey, L., Owada, S., Katayama, T., Yabashi, M., Tanaka, Yoshikazu, Togashi, T., Liu, J., Rayan Serrao, C., Kim, B. J., Huber, L., Chang, C. -L., McMorrow, D. F., Forst, M., and Hill, J. P. Mon . "Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4". United States. https://doi.org/10.1038/NMAT4641. https://www.osti.gov/servlets/purl/1311357.
@article{osti_1311357,
title = {Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4},
author = {Dean, M. P. M. and Cao, Y. and Liu, X. and Wall, S. and Zhu, D. and Mankowsky, R. and Thampy, V. and Chen, X. M. and Vale, J. G. and Casa, D. and Kim, Jungho and Said, A. H. and Juhas, P. and Alonso-Mori, R. and Glownia, J. M. and Robert, A. and Robinson, J. and Sikorski, M. and Song, S. and Kozina, M. and Lemke, H. and Patthey, L. and Owada, S. and Katayama, T. and Yabashi, M. and Tanaka, Yoshikazu and Togashi, T. and Liu, J. and Rayan Serrao, C. and Kim, B. J. and Huber, L. and Chang, C. -L. and McMorrow, D. F. and Forst, M. and Hill, J. P.},
abstractNote = {Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity1, 2, 3, 4. Recently, photo-excitation has been used to induce similarly exotic states transiently5, 6, 7. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. In conclusion, the marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.},
doi = {10.1038/NMAT4641},
journal = {Nature Materials},
number = 6,
volume = 15,
place = {United States},
year = {2016},
month = {5}
}

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