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

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 Ca${}_2$RuO${}_4$ 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.

arXiv comment9 pages main text, 4 figures, 21 pages supplementary information

References in corpus (36)

• Strong electronic correlations from Hund's coupling
• An optically stimulated superconducting-like phase in K3C60 far above equilibrium Tc
• Ultrafast switching to a stable hidden topologically protected quantum state in an electronic crystal
• Terahertz-Field-Induced Ferroelectricity in Quantum Paraelectric SrTiO${}_3$
• Metastable ferroelectricity in optically strained $SrTi{O}_3$
• Light-Induced Charge Density Wave in LaTe${}_3$
• Excitonic Magnetism in Van Vleck-type d^4 Mott Insulators
• Light-driven ultrafast phonomagnetism
• Pseudospin-selective Floquet band engineering in black phosphorus
• Ultrafast energy and momentum resolved dynamics of magnetic correlations in photo-doped Mott insulator Sr${}_2$IrO${}_4$
• Phase-ordering of charge density waves traced by ultrafast low-energy electron diffraction
• Cooperative photoinduced metastable phase control in strained manganite films
• Higgs mode and its decay in a two dimensional antiferromagnet
• Magnetic Phase Diagram of Ca2-xSrxRuO4 Governed by Structural Distortions
• From Mott insulator to ferromagnetic metal: a pressure study of Ca${}_2$RuO${}_4$
• Controlling the anisotropy of a van der Waals antiferromagnet with light
• Giant modulation of optical nonlinearity by Floquet engineering
• Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO${}_3$
• Novel magnetic state in $d^4$ Mott insulators
• In-situ strain-tuning of the metal-insulator-transition of Ca${}_2$RuO${}_4$ in angle-resolved photoemission experiments
• Orbital ordering transition in Ca${}_2$RuO${}_4$ observed with resonant x-ray diffraction
• Optical manipulation of electronic dimensionality in a quantum material
• Raman scattering from Higgs mode oscillations in the two-dimensional antiferromagnet Ca${}_2$RuO${}_4$
• High pressure diffraction studies on Ca2RuO4
• Magnetic and Orbital Orders Coupled to Negative Thermal Expansion in Mott Insulators, Ca2Ru1-xMxO4 (M = Mn and Fe)
• Anomalous mirror symmetry breaking in a model insulating cuprate Sr${}_2$CuO${}_2$Cl${}_2$
• High-speed measurement of rotational anisotropy nonlinear optical harmonic generation using position sensitive detection
• Nonequilibrium Orbital Transitions via Applied Electrical Current in Calcium Ruthenate
• Keldysh space control of charge dynamics in a strongly driven Mott insulator
• Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr${}_2$IrO${}_4$
• A light-induced Weyl semiconductor-to-metal transition mediated by Peierls instability
• Picosecond volume expansion drives a later-time insulator-metal transition in a nano-textured Mott Insulator
• Persistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca${}_2$RuO${}_4$
• Decoupling of static and dynamic criticality in a driven Mott insulator
• Magnetic reorientation transition in a three orbital model for $\mathrm{C}{\mathrm{a}}_2\mathrm{Ru}{\mathrm{O}}_4$ -- Interplay of spin-orbit coupling, tetragonal distortion, and Coulomb interactions
• A coherent phonon-induced hidden quadrupolar ordered state in Ca${}_2$RuO${}_4$