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Register a new userUltrafast energy and momentum resolved dynamics of magnetic correlations in photo-doped Mott insulator Sr$_2$IrO$_4$
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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 $T_C$ 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 Sr$_2$IrO$_4$. 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 Neel 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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Despite many efforts to rationalize the strongly correlated electronic ground states in doped Mott insulators, the nature of the doping induced insulator to metal transition is still a subject under intensive investigation. Here we probe the nanoscale electronic structure of the Mott insulator Sr$_2$IrO$_{4-delta}$ with low-temperature scanning tunneling microscopy and find enhanced local density of states (LDOS) inside the Mott gap at the location of individual apical oxygen site defects. We visualize paths of enhanced conductance arising from the overlapping of defect states which induces finite LDOS at the Fermi level. By combining these findings with the typical spatial extension of isolated defects of about 2~nm, we show that the insulator to metal transition in Sr$_2$IrO$_{4-delta}$ is of percolative nature.
We report a high-field electron spin resonance study in the sub-THz frequency domain of a single crystal of Sr$_2$IrO$_4$ that has been recently proposed as a prototypical spin-orbital Mott insulator. In the antiferromagnetically (AFM) ordered state with noncollinear spin structure that occurs in this material at $T_{rm N} approx 240$ K we observe both the low frequency mode due to the precession of weak ferromagnetic moments arising from a spin canting, and the high frequency modes due to the precession of the AFM sublattices. Surprisingly, the energy gap for the AFM excitations appears to be very small, amounting to 0.83 meV only. This suggests a rather isotropic Heisenberg dynamics of interacting Ir$^{4+}$ effective spins despite the spin-orbital entanglement in the ground state.
High temperature superconductivity in cuprates arises from doping a parent Mott insulator by electrons or holes. A central issue is how the Mott gap evolves and the low-energy states emerge with doping. Here we report angle-resolved photoemission spectroscopy measurements on a cuprate parent compound by sequential in situ electron doping. The chemical potential jumps to the bottom of the upper Hubbard band upon a slight electron doping, making it possible to directly visualize the charge transfer band and the full Mott gap region. With increasing doping, the Mott gap rapidly collapses due to the spectral weight transfer from the charge transfer band to the gapped region and the induced low-energy states emerge in a wide energy range inside the Mott gap. These results provide key information on the electronic evolution in doping a Mott insulator and establish a basis for developing microscopic theories for cuprate superconductivity.
We investigate the temporal evolution of electronic states in strontium iridate Sr$_2$IrO$_4$. The time resolved photoemission spectra of intrinsic, electron doped and the hole doped samples are monitored in identical experimental conditions. Our data on intrinsic and electron doped samples, show that primary doublon-holon pairs relax near to the chemical potential on a timescale shorter than $70$ fs. The subsequent cooling of low energy excitations takes place in two step: a rapid dynamics of $cong120$ fs is followed by a slower decay of $cong 1$ ps. The reported timescales endorse the analogies between Sr$_2$IrO$_4$ and copper oxides.
We report the existence of Griffiths phase (GP) and its influence on critical phenomena in layered Sr$_2$IrO$_4$ ferromagnet (T$_C$ = 221.5 K). The power law behavior of inverse magentic susceptibility, 1/$chi$(T) with exponent $lambda = 0.18(2)$ confirm the GP in the regime T$_C$ $<$ T $leq$ T$_G$ = 279.0(5) K. Moreover, the detailed critical analysis via modified Arrott plot method exhibits unrealistic critical exponents $beta$ = 0.77(1), $gamma$ = 1.59(2) and $delta = 3.06(4)$, in corroboration with magneto-caloric study. The abnormal exponent values have been viewed in context of ferromagnetic-Griffiths phase transition. The GP has been further analyzed using Bray model, which yields a reliable value of $beta$ = 0.19(2), belonging to the two-dimensional (2D) XYh$_4$ universality class with strong anisotropy present in Sr$_2$IrO$_4$. The present study proposes Bray model as a possible tool to investigate the critical behavior for Griffiths ferromagnets in place of conventional Arrott plot analysis. The possible origins of GP and its correlation with insulating nature of Sr$_2$IrO$_4$ have been discussed.
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