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

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.

doi:10.1038/NMAT4641

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

Journal Article · Mon May 09 00:00:00 EDT 2016 · Nature Materials

DOI:https://doi.org/10.1038/NMAT4641· OSTI ID:1311357

^[1];

^[1]; Liu, X. ^[2];

^[3]; Zhu, D. ^[4]; Mankowsky, R. ^[5]; Thampy, V. ^[1]; Chen, X. M. ^[1]; Vale, J. G. ^[6]; Casa, D. ^[7]; Kim, Jungho ^[7]; Said, A. H. ^[7]; Juhas, P. ^[1]; Alonso-Mori, R. ^[4]; Glownia, J. M. ^[4]; Robert, A. ^[4]; Robinson, J. ^[4]; Sikorski, M. ^[4];

^[4]; Kozina, M. ^[4] more »

Brookhaven National Lab. (BNL), Upton, NY (United States)
Chinese Academy of Sciences (CAS), Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China)
The Barcelona Institute of Science and Technology, Castelldefels (Barcelona) (Spain)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
Univ. College London, London (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
RIKEN SPring-8 Center, Hyogo (Japan)
Japan Synchrotron Radiation Institute, Hyogo (Japan)
Univ. of Tennessee, Knoxville, TN (United States)
Univ. of California, Berkeley, CA (United States)
Max Planck Institute for Solid State Research, Stuttgart (Germany)
ETH Zurich, Zurich (Switzerland)
Univ. of Groningen, Groningen (The Netherlands)

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity^{1, 2, 3, 4}. Recently, photo-excitation has been used to induce similarly exotic states transiently^{5, 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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1311357

Report Number(s):: BNL-112461-2016-JA; R&D Project: PO011; KC0201060

Journal Information:: Nature Materials, Vol. 15, Issue 6; ISSN 1476-1122

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 93 works

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References (33)

A common thread: The pairing interaction for unconventional superconductors Scalapino, D. J. Reviews of Modern Physics, Vol. 84, Issue 4 https://doi.org/10.1103/RevModPhys.84.1383	journal	October 2012
Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet Kim, Y. K.; Krupin, O.; Denlinger, J. D. Science, Vol. 345, Issue 6193 https://doi.org/10.1126/science.1251151	journal	June 2014
Hallmarks of the Mott-metal crossover in the hole-doped pseudospin-1/2 Mott insulator Sr2IrO4 Cao, Yue; Wang, Qiang; Waugh, Justin A. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11367	journal	April 2016
Collapse of the Mott Gap and Emergence of a Nodal Liquid in Lightly Doped ${Sr}_{2} {IrO}_{4}$ de la Torre, A.; McKeown Walker, S.; Bruno, F. Y. Physical Review Letters, Vol. 115, Issue 17 https://doi.org/10.1103/PhysRevLett.115.176402	journal	October 2015
Light-Induced Superconductivity in a Stripe-Ordered Cuprate Fausti, D.; Tobey, R. I.; Dean, N. Science, Vol. 331, Issue 6014 https://doi.org/10.1126/science.1197294	journal	January 2011
Dynamics and Control in Complex Transition Metal Oxides Zhang, J.; Averitt, R. D. Annual Review of Materials Research, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-matsci-070813-113258	journal	July 2014
Nonequilibrium dynamical mean-field theory and its applications Aoki, Hideo; Tsuji, Naoto; Eckstein, Martin Reviews of Modern Physics, Vol. 86, Issue 2 https://doi.org/10.1103/RevModPhys.86.779	journal	June 2014
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 Kim, B. J.; Ohsumi, H.; Komesu, T. Science, Vol. 323, Issue 5919 https://doi.org/10.1126/science.1167106	journal	March 2009
Magnetic Excitation Spectra of ${Sr}_{2} {IrO}_{4}$ Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors Kim, Jungho; Casa, D.; Upton, M. H. Physical Review Letters, Vol. 108, Issue 17 https://doi.org/10.1103/PhysRevLett.108.177003	journal	April 2012
Doping a Mott insulator: Physics of high-temperature superconductivity Lee, Patrick A.; Nagaosa, Naoto; Wen, Xiao-Gang Reviews of Modern Physics, Vol. 78, Issue 1 https://doi.org/10.1103/RevModPhys.78.17	journal	January 2006
Twisted Hubbard Model for ${Sr}_{2} {IrO}_{4}$ : Magnetism and Possible High Temperature Superconductivity Wang, Fa; Senthil, T. Physical Review Letters, Vol. 106, Issue 13 https://doi.org/10.1103/PhysRevLett.106.136402	journal	March 2011
Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal ${Sr}_{2} {IrO}_{4}$ Cao, G.; Bolivar, J.; McCall, S. Physical Review B, Vol. 57, Issue 18 https://doi.org/10.1103/PhysRevB.57.R11039	journal	May 1998
Electronic structures of layered perovskite ${Sr}_{2} M O_{4}$ ( $M = Ru$ , Rh, and Ir) Moon, S. J.; Kim, M. W.; Kim, K. W. Physical Review B, Vol. 74, Issue 11 https://doi.org/10.1103/PhysRevB.74.113104	journal	September 2006
Photoinduced Melting of Antiferromagnetic Order in ${La}_{0.5} {Sr}_{1.5} {MnO}_{4}$ Measured Using Ultrafast Resonant Soft X-Ray Diffraction Ehrke, H.; Tobey, R. I.; Wall, S. Physical Review Letters, Vol. 106, Issue 21 https://doi.org/10.1103/PhysRevLett.106.217401	journal	May 2011
Glass-like recovery of antiferromagnetic spin ordering in a photo-excited manganite Pr0.7Ca0.3MnO3 Zhou, S. Y.; Langner, M. C.; Zhu, Y. Scientific Reports, Vol. 4, Issue 1 https://doi.org/10.1038/srep04050	journal	February 2014
Real-Time Manifestation of Strongly Coupled Spin and Charge Order Parameters in Stripe-Ordered ${La}_{1.75} {Sr}_{0.25} {NiO}_{4}$ Nickelate Crystals Using Time-Resolved Resonant X-Ray Diffraction Chuang, Y. D.; Lee, W. S.; Kung, Y. F. Physical Review Letters, Vol. 110, Issue 12 https://doi.org/10.1103/PhysRevLett.110.127404	journal	March 2013
Photoinduced melting of magnetic order in the correlated electron insulator NdNiO $_{3}$ Caviglia, A. D.; Först, M.; Scherwitzl, R. Physical Review B, Vol. 88, Issue 22 https://doi.org/10.1103/PhysRevB.88.220401	journal	December 2013
Phase fluctuations and the absence of topological defects in a photo-excited charge-ordered nickelate Lee, W. S.; Chuang, Y. D.; Moore, R. G. Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1837	journal	January 2012
Distinguishing the ultrafast dynamics of spin and orbital moments in solids Boeglin, C.; Beaurepaire, E.; Halté, V. Nature, Vol. 465, Issue 7297 https://doi.org/10.1038/nature09070	journal	May 2010
Coherent terahertz control of antiferromagnetic spin waves Kampfrath, Tobias; Sell, Alexander; Klatt, Gregor Nature Photonics, Vol. 5, Issue 1 https://doi.org/10.1038/nphoton.2010.259	journal	November 2010
Control of speed and efficiency of ultrafast demagnetization by direct transfer of spin angular momentum Malinowski, G.; Dalla Longa, F.; Rietjens, J. H. H. Nature Physics, Vol. 4, Issue 11 https://doi.org/10.1038/nphys1092	journal	September 2008
Resonant inelastic x-ray scattering studies of elementary excitations Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P. Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.705	journal	June 2011
Insights into the high temperature superconducting cuprates from resonant inelastic X-ray scattering Dean, M. P. M. Journal of Magnetism and Magnetic Materials, Vol. 376 https://doi.org/10.1016/j.jmmm.2014.03.057	journal	February 2015
Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet Batignani, G.; Bossini, D.; Di Palo, N. Nature Photonics, Vol. 9, Issue 8 https://doi.org/10.1038/nphoton.2015.121	journal	July 2015
Momentum-resolved electronic excitations in the Mott insulator ${Sr}_{2} {IrO}_{4}$ studied by resonant inelastic x-ray scattering Ishii, K.; Jarrige, I.; Yoshida, M. Physical Review B, Vol. 83, Issue 11 https://doi.org/10.1103/PhysRevB.83.115121	journal	March 2011
Excitonic quasiparticles in a spin–orbit Mott insulator Kim, Jungho; Daghofer, M.; Said, A. H. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5453	journal	July 2014
Ultrafast charge dynamics in photoexcited ${Nd}_{2} {CuO}_{4}$ and ${La}_{2} {CuO}_{4}$ cuprate compounds investigated by femtosecond absorption spectroscopy Okamoto, H.; Miyagoe, T.; Kobayashi, K. Physical Review B, Vol. 82, Issue 6 https://doi.org/10.1103/PhysRevB.82.060513	journal	August 2010
The spin-½ Heisenberg antiferromagnet on a square lattice and its application to the cuprous oxides Manousakis, Efstratios Reviews of Modern Physics, Vol. 63, Issue 1 https://doi.org/10.1103/RevModPhys.63.1	journal	January 1991
Spin Dynamics of the 2D Spin $\frac{1}{2}$ Quantum Antiferromagnet Copper Deuteroformate Tetradeuterate (CFTD) Rønnow, H. M.; McMorrow, D. F.; Coldea, R. Physical Review Letters, Vol. 87, Issue 3 https://doi.org/10.1103/PhysRevLett.87.037202	journal	June 2001
Two-Dimensional Heisenberg Behavior of $J_{eff} = 1 / 2$ Isospins in the Paramagnetic State of the Spin-Orbital Mott Insulator ${Sr}_{2} {IrO}_{4}$ Fujiyama, S.; Ohsumi, H.; Komesu, T. Physical Review Letters, Vol. 108, Issue 24 https://doi.org/10.1103/PhysRevLett.108.247212	journal	June 2012
Importance of $X Y$ anisotropy in ${Sr}_{2} {IrO}_{4}$ revealed by magnetic critical scattering experiments Vale, J. G.; Boseggia, S.; Walker, H. C. Physical Review B, Vol. 92, Issue 2 https://doi.org/10.1103/PhysRevB.92.020406	journal	July 2015
Epitaxy-distorted spin-orbit Mott insulator in Sr $_{2}$ IrO $_{4}$ thin films Rayan Serrao, C.; Liu, Jian; Heron, J. T. Physical Review B, Vol. 87, Issue 8 https://doi.org/10.1103/PhysRevB.87.085121	journal	February 2013
The X-ray Pump–Probe instrument at the Linac Coherent Light Source Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco Journal of Synchrotron Radiation, Vol. 22, Issue 3 https://doi.org/10.1107/S1600577515005135	journal	April 2015

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Perspective: Opportunities for ultrafast science at SwissFEL Abela, Rafael; Beaud, Paul; Van Bokhoven, Jeroen A. AIP Publishing https://doi.org/10.7892/boris.114739	text	January 2017
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