Hao Chu

Evidence of an odd-parity hidden order in a spin-orbit coupled correlated iridate

A rare combination of strong spin–orbit coupling and electron–electron correlations makes the iridate Mott insulator Sr_2IrO_4 a promising host for novel electronic phases of matter. The resemblance of its crystallographic, magnetic and electronic structures to La_2CuO_4, as well as the emergence on doping of a pseudogap region and a low-temperature d-wave gap, has particularly strengthened analogies to cuprate high-T_c superconductors. However, unlike the cuprate phase diagram, which features a plethora of broken symmetry phases in a pseudogap region that includes charge density wave, stripe, nematic and possibly intra-unit-cell loop-current orders, no broken symmetry phases proximate to the parent antiferromagnetic Mott insulating phase in Sr_2IrO_4 have been observed so far, making the comparison of iridate to cuprate phenomenology incomplete. Using optical second-harmonic generation, we report evidence of a hidden non-dipolar magnetic order in Sr_2IrO_4 that breaks both the spatial inversion and rotational symmetries of the underlying tetragonal lattice. Four distinct domain types corresponding to discrete 90°-rotated orientations of a pseudovector order parameter are identified using nonlinear optical microscopy, which is expected from an electronic phase that possesses the symmetries of a magneto-electric loop-current order. The onset temperature of this phase is monotonically suppressed with bulk hole doping, albeit much more weakly than the Neel temperature, revealing an extended region of the phase diagram with purely hidden order. Driving this hidden phase to its quantum critical point may be a path to realizing superconductivity in Sr_2IrO_4.

A Low Temperature Nonlinear Optical Rotational Anisotropy Spectrometer for the Determination of Crystallographic and Electronic Symmetries

Nonlinear optical generation from a crystalline material can reveal the symmetries of both its lattice structure and underlying ordered electronic phases and can therefore be exploited as a complementary technique to diffraction based scattering probes. Although this technique has been successfully used to study the lattice and magnetic structures of systems such as semiconductor surfaces, multiferroic crystals, magnetic thin films, and multilayers, challenging technical requirements have prevented its application to the plethora of complex electronic phases found in strongly correlated electron systems. These requirements include an ability to probe small bulk single crystals at the μm length scale, a need for sensitivity to the entire nonlinear optical susceptibility tensor, oblique light incidence reflection geometry, and incident light frequency tunability among others. These measurements are further complicated by the need for extreme sample environments such as ultra low temperatures, high magnetic fields, or high pressures. In this review we present a novel experimental construction using a rotating light scattering plane that meets all the aforementioned requirements. We demonstrate the efficacy of our scheme by making symmetry measurements on a μm scale facet of a small bulk single crystal of Sr2IrO4 using optical second and third harmonic generation.

A charge density wave-like instability in a doped spin-orbit-assisted weak Mott insulator

Layered perovskite iridates realize a rare class of Mott insulators that are predicted to be strongly spin-orbit coupled analogues of the parent state of cuprate high-temperature superconductors. Recent discoveries of pseudogap, magnetic multipolar ordered and possible d-wave superconducting phases in doped Sr2IrO4 have reinforced this analogy among the single layer variants. However, unlike the bilayer cuprates, no electronic instabilities have been reported in the doped bilayer iridate Sr3Ir2O7. Here we show that Sr3Ir2O7 realizes a weak Mott state with no cuprate analogue by using ultrafast time-resolved optical reflectivity to uncover an intimate connection between its insulating gap and antiferromagnetism. However, we detect a subtle charge density wave-like Fermi surface instability in metallic electron doped Sr3Ir2O7 at temperatures (TDW) close to 200 K via the coherent oscillations of its collective modes, which is reminiscent of that observed in cuprates. The absence of any signatures of a new spatial periodicity below TDW from diffraction, scanning tunnelling and photoemission based probes suggests an unconventional and possibly short-ranged nature of this density wave order.

Nonlinear and time-resolved optical study of the 112-type iron-based superconductor parent Ca 1 − x La x FeAs 2 across its structural phase transition

The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the ɑ 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.

Doping-driven structural distortion in the bilayer iridate (Sr_(1−x)La_x)_3Ir_2O_7

Neutron single-crystal diffraction and rotational anisotropy optical second harmonic generation data are presented resolving the nature of the structural distortion realized in electron-doped (Sr_(1−x)La_x)_3Ir_2O_7 with x = 0.035 and x = 0.071. Once electrons are introduced into the bilayer spin-orbit assisted Mott insulator Sr_2Ir_2O_7, previous studies have identified the appearance of a low-temperature structural distortion and have suggested the presence of a competing electronic instability in the phase diagram of this material. Our measurements resolve a lowering of the structural symmetry from monoclinic C2/c to monoclinic P2_1/c and the creation of two unique Ir sites within the chemical unit cell as the lattice distorts below a critical temperature T_S. Details regarding the modifications to oxygen octahedral rotations and tilting through the transition are discussed as well as the evolution of the low-temperature distorted lattice as a function of carrier substitution.