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

Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high TC superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant inelastic X-ray scattering at a free electron laser, and directly determine the magnetization dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state 2~ps after the excitation has strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. The magnetism recovers its two-dimensional (2D) in-plane N\'eel correlations on a timescale of a few ps, while the three-dimensional (3D) long-range magnetic order restores over a far longer, fluence-dependent timescale of a few hundred ps. The dramatic difference in these two timescales, implies that characterizing the dimensionality of magnetic correlations will be vital in our efforts to understand ultrafast magnetic dynamics.
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Publication Date:
OSTI Identifier:
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature Materials; Journal Volume: 15; Journal Issue: 6
Nature Publishing Group
Research Org:
Argonne National Laboratory (ANL)
Sponsoring Org:
USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division; USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; Chinese Academy of Sciences (CAS); Spanish Ministerio de Economia y Competitividad (MINECO); Engineering and Physical Sciences Research Council (EPSRC)
Country of Publication:
United States