Published March 2025 | Version Published
Journal Article Open

Time-hidden magnetic order in a multi-orbital Mott insulator

  • 1. ROR icon California Institute of Technology
  • 2. ROR icon National University of Singapore
  • 3. ROR icon University of Colorado Boulder
  • 4. ROR icon Wellesley College

Abstract

Photo-excited quantum materials can be driven into thermally inaccessible metastable states that exhibit structural, charge, spin, topological and superconducting orders. Metastable states typically emerge on timescales set by the intrinsic electronic and phononic energy scales, ranging from femtoseconds to picoseconds, and can persist for weeks. Therefore, studies have primarily focused on ultrafast or quasi-static limits, leaving the intermediate time window less explored. Here we reveal a metastable state with broken glide-plane symmetry in photo-doped Ca2RuO4 using time-resolved optical second-harmonic generation and birefringence measurements. We find that the metastable state appears long after intralayer antiferromagnetic order has melted and photo-carriers have recombined. Its properties are distinct from all known states in the equilibrium phase diagram and are consistent with intralayer ferromagnetic order. Furthermore, model Hamiltonian calculations reveal that a non-thermal trajectory to this state can be accessed via photo-doping. Our results expand the search space for out-of-equilibrium electronic matter to metastable states emerging at intermediate timescales.

Copyright and License

© 2025, The Author(s), under exclusive licence to Springer Nature Limited.

Acknowledgement

We thank E. Demler, A. Millis, G. Khaliullin and W. Liu for useful discussions. D.H. acknowledges support for instrumentation and theory from the Institute for Quantum Information and Matter (IQIM), an NSF Physics Frontiers Center (grant number PHY-2317110). Optical spectroscopy measurements were funded in part by the Gordon and Betty Moore Foundation through grant number GBMF11564 to Caltech to support the work of D.H. G.R. acknowledges the support of the Simons Foundation, ARO MURI grant number W911NF-16-1- 0361 and the Institute of Quantum Information and Matter (grant number PHY-2317110). X.L. acknowledges support from the Caltech Postdoctoral Prize Fellowship and the Singapore National Research Foundation under award number NRF-NRFF16-2024-0008. G.C. acknowledges support from the National Science Foundation via grant number DMR 2204811. I.E. acknowledges support from the Simons Foundation and the IQIM.

Supplemental Material

Supplementary Figs. 1–17, Table 1, Sections 1–12 and References: Supplementary Information

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Additional details

Related works

Describes
Journal Article: https://rdcu.be/el4LT (ReadCube)

Funding

National Science Foundation
Physics Frontiers Center PHY-2317110
Simons Foundation
Gordon and Betty Moore Foundation
GBMF11564
National Science Foundation
PHY-2317110
National Science Foundation
DMR 2204811
National Science Foundation
PHY-2317110
California Institute of Technology
Postdoctoral Prize Fellowship -
United States Army Research Office
MURI W911NF-16-1-0361
National Research Foundation
NRF-NRFF16-2024-0008

Dates

Available
2025-01-23
Published online

Caltech Custom Metadata

Caltech groups
Institute for Quantum Information and Matter, Division of Physics, Mathematics and Astronomy (PMA)
Publication Status
Published