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Dynamically driven interacting quantum many-body systems have the potential to exhibit properties that defy the laws of equilibrium statistical mechanics. A widely studied model is the impulsively driven antiferromagnetic Mott insulator, which is predicted to realize exotic transient phenomena including dynamical phase transitions into thermally forbidden states and highly non-thermal magnon distributions. However such far-from-equilibrium regimes, where conventional time-dependent Ginzburg-Landau descriptions fail, are experimentally challenging to prepare and to probe especially in solid state systems. Here we use a combination of time-resolved second harmonic optical polarimetry and coherent magnon spectroscopy to interrogate $n$-type photo-doping induced ultrafast magnetic order parameter dynamics in the Mott insulator Sr$_2$IrO$_4$. We uncover an unusual far-from-equilibrium critical regime in which the divergences of the magnetic correlation length and relaxation time are decoupled. This violation of conventional thermal critical behavior arises from the interplay of photo-doping and non-thermal magnon population induced demagnetization effects. Our findings, embodied in a non-equilibrium "phase diagram", provide a blueprint for engineering the out-of-equilibrium properties of quantum matter, with potential applications to terahertz spintronics technologies., Comment: 7 pages main text, 4 figures, 19 pages supplementary information

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at $T_c = 200$ K in the strongly spin-orbit coupled correlated metal Cd$_2$Re$_2$O$_7$. We establish that the structural distortion at $T_c$ is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near $T_c$. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters., Comment: 5 pages main text, 5 figures, 7 pages supplementary information

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd$_2$Re$_2$O$_7$ using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of the multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd$_2$Re$_2$O$_7$ and induces a parity-breaking lattice distortion as a secondary order., Comment: 9 pages main text, 4 figures, 10 pages supplementary information

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr$_2$RuO$_4$ and its isoelectronic counterpart Ba$_2$RuO$_4$ using oxide molecular beam epitaxy (MBE), \emph{in situ} angle-resolved photoemission spectroscopy (ARPES), and transport measurements. Near the topological transition of the $\gamma$ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.

The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the $a$ and $b$ axes. This feature eliminates the need for uniaxial strain that is usually required to stabilize large single domains in the electronic nematic state that exists in the vicinity of magnetic order in the iron-based superconductors. We report detailed structural symmetry measurements of 112-type Ca$_{0.73}$La$_{0.27}$FeAs$_{2}$ using rotational anisotropy optical second harmonic generation. This technique is complementary to diffraction experiments and enables a precise determination of the point group symmetry of a crystal. By combining our measurements with density functional theory calculations, we uncover a strong optical second harmonic response of bulk electric dipole origin from the Fe and Ca $3d$-derived states that enables us to assign $C_2$ as the crystallographic point group. This makes the 112-type materials high-temperature superconductors without a center of inversion, allowing for the possible mixing of singlet and triplet Cooper pairs in the superconducting state. We also perform pump-probe transient reflectivity experiments that reveal a 4.6 THz phonon mode associated with the out-of-plane motion of As atoms in the FeAs layers. We do not observe any suppression of the optical second harmonic response or shift in the phonon frequency upon cooling through the reported monoclinic-to-triclinic transition at 58 K. This allows us to identify $C_1$ as the low-temperature crystallographic point group but suggests that structural changes induced by long-range magnetic order are subtle and do not significantly affect electronic states near the Fermi level.

We present a method of performing high-speed rotational anisotropy nonlinear optical harmonic generation experiments at rotational frequencies of several hertz by projecting the harmonic light reflected at different angles from a sample onto a stationary position sensitive detector. The high rotational speed of the technique, $10^3$ to $10^4$ times larger than existing methods, permits precise measurements of the crystallographic and electronic symmetries of samples by averaging over low frequency laser power, beam pointing, and pulse width fluctuations. We demonstrate the sensitivity of our technique by resolving the bulk four-fold rotational symmetry of GaAs about its [001] axis using second harmonic generation.

We report high-resolution angle-resolved photoemission studies of epitaxial thin films of the correlated 4d transition metal oxide ferromagnet SrRuO3. The Fermi surface in the ferromagnetic state consists of well-defined Landau quasiparticles, exhibiting strong coupling to low-energy bosonic modes which contributes to the large effective masses observed by transport and thermodynamic measurements. Upon warming the material through its Curie temperature, we observe a substantial decrease in quasiparticle coherence, but negligible changes in the ferromagnetic exchange splitting, suggesting that local moments play an important role in the ferromagnetism in SrRuO3., Comment: 5 pages, 4 figures, supplementary information (see other files)

We present angle-resolved photoemission spectroscopy of Eu(1-x)Gd(x)O through the ferromagnetic metal-insulator transition. In the ferromagnetic phase, we observe Fermi surface pockets at the Brillouin zone boundary, consistent with density functional theory, which predicts a half metal. Upon warming into the paramagnetic state, our results reveal a strong momentum-dependent evolution of the electronic structure, where the metallic states at the zone boundary are replaced by pseudogapped states at the Brillouin zone center due to the absence of magnetic long-range order of the Eu 4f moments., Comment: 5 pages, 5 figures, supplementary information (see other files)

We study a model of a d-wave superconductor with strong potential scatterers in the presence of antiferromagnetic correlations and apply it to experimental nuclear magnetic resonance (NMR) results on Zn impurities in the superconducting state of YBCO. We then focus on the contribution of impurity-induced paramagnetic moments, with Hubbard correlations in the host system accounted for in Hartree approximation. We show that local magnetism around individual impurities broadens the line, but quasiparticle interference between impurity states plays an important role in smearing out impurity satellite peaks. The model, together with estimates of vortex lattice effects, provides a semi-quantitative description of the impurity concentration dependence of the NMR line shape in the superconducting state, and gives a qualitative description of the temperature dependence of the line asymmetry. We argue that impurity-induced paramagnetism and resonant local density of states effects are both necessary to explain existing experiments., Comment: 15 pages, 23 figures, submitted to Phys. Rev. B