Spatiotemporal migration of antiferromagnetic domain walls in Sr2IrO4
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75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Engineering topics
Zhao, Hengdi
Publications and source records attributed to Zhao, Hengdi.
Transition between Heavy-Fermion-Strange-Metal and Quantum Spin Liquid in a $4d$-Electron Trimer Lattice
We present experimental evidence that a heavy Fermi surface consisting of itinerant, charge-neutral spinons underpins both heavy-fermion-strange-metal (without f electrons) and quantum-spin-liquid states in the 4d-electron trimer lattice, Ba 4 Nb 1-x Ru 3+x O 12 (|x| < 0.20). These two exotic states both exhibit an extraordinarily large entropy, a linear heat capacity extending into the milli-Kelvin regime, a linear thermal conductivity at low temperatures, and separation of charges and spins. Furthermore, the insulating spin liquid is a much better thermal conductor than the heavy-fermion-strange-metal that separately is observed to strongly violate the Wiedemann- Franz law. Here, we propose that at the heart of this 4d system is a universal, heavy spinon Fermi surface that provides a unified framework for explaining the exotic phenomena observed throughout the entire series. The control of such exotic ground states provided by variable Nb concentration offers a new paradigm for studies of correlated quantum matter.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Anisotropy of antiferromagnetic domains in a spin-orbit Mott insulator
The temperature-dependent behavior of magnetic domains plays an essential role in the magnetic properties of materials, leading to widespread applications. However, experimental methods to access the three-dimensional (3D) magnetic domain structures are very limited, especially for antiferromagnets. Over the past decades, the spin-orbit Mott insulator iridate Sr 2 IrO 4 has attracted particular attention because of its interesting magnetic structure and analogy to superconducting cuprates. Here, in this work, we apply resonant x-ray magnetic Bragg coherent diffraction imaging to track the real-space 3D evolution of antiferromagnetic ordering inside a Sr 2 IrO 4 single crystal as a function of temperature, finding that the antiferromagnetic domain shows anisotropic changes. The anisotropy of the domain shape reveals the underlying anisotropy of the antiferromagnetic coupling strength within Sr 2 IrO 4 . These results demonstrate the high potential significance of 3D domain imaging in magnetism research.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Evidence for Bootstrap Percolation Dynamics in a Photoinduced Phase Transition
Upon intense femtosecond photo-excitation, a many-body system can undergo a phase transition through a non-equilibrium route, but understanding these pathways remains an outstanding challenge. Here, we use time-resolved second harmonic generation to investigate a photo-induced phase transition in Ca 3 Ru 2 O 7 and show that mesoscale inhomogeneity profoundly influences the transition dynamics. We observe a marked slowing down of the characteristic time τ that quantifies the transition between two structures. τ evolves non-monotonically as a function of photo-excitation fluence, rising from below 200 fs to ~1.4 ps, then falling again to below 200 fs. To account for the observed behavior, we perform a bootstrap percolation simulation that demonstrates how local structural interactions govern the transition kinetics. Finally, our work highlights the importance of percolating mesoscale inhomogeneity in the dynamics of photo-induced phase transitions and provides a model that may be useful for understanding such transitions more broadly.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Magnetic Structure and Spin Fluctuation in Colossal Magnetoresistance Ferrimagnet Mn 3 Si 2 Te 6
The ferrimagnetic insulator Mn 3 Si 2 Te 6 , which features a Curie temperature T c at 78 K and a delicate yet consequential magnetic frustration, exhibits colossal magnetoresistance (CMR) when the magnetic field is applied along the magnetic hard axis, surprisingly inconsistent with existing precedents [Y. Ni, H. Zhao, Y. Zhang, B. Hu, I. Kimchi, and G. Cao, Phys. Rev. B 103, L161105 (2021)]. This discovery motivates a thorough single-crystal neutron diffraction study in order to gain insights into the magnetic structure and its hidden correlation with the new type of CMR. Here we report a noncollinear magnetic structure below the T c where the moments lie predominantly within the basal plane but tilt toward the c axis by ≈10° at ambient conditions. A substantial magnetic diffuse scattering decays slowly and persists well above the T c . The evolution of the spin correlation lengths agrees well with the electrical resistivity, underscoring the role of spin fluctuation contributing to the magnetoresistivity near the transition. Further, application of magnetic field along the c axis renders a swift occurrence of CMR but only a slow tilting of the magnetic moments toward the c axis. The unparalleled changes indicate a nonconsequential role of magnetic polarization.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Control of chiral orbital currents in a colossal magnetoresistance material
Colossal magnetoresistance (CMR) is an extraordinary enhancement of the electrical conductivity in the presence of a magnetic field. It is conventionally associated with a field-induced spin polarization that drastically reduces spin scattering and electric resistance. Ferrimagnetic Mn 3 Si 2 Te 6 is an intriguing exception to this rule: it exhibits a seven-order-of-magnitude reduction in ab plane resistivity that occurs only when a magnetic polarization is avoided 1,2 . Here, we report an exotic quantum state that is driven by ab plane chiral orbital currents (COC) flowing along edges of MnTe 6 octahedra. The c axis orbital moments of ab plane COC couple to the ferrimagnetic Mn spins to drastically increase the ab plane conductivity (CMR) when an external magnetic field is aligned along the magnetic hard c axis. Consequently, COC-driven CMR is highly susceptible to small direct currents exceeding a critical threshold, and can induce a time-dependent, bistable switching that mimics a first-order ‘melting transition’ that is a hallmark of the COC state. Further, the demonstrated current-control of COC-enabled CMR offers a new paradigm for quantum technologies.
36 MATERIALS SCIENCE↗
Resolution of zigzag magnetic correlations in Na-deficient Na x IrO 3 without long-range ordering
The materials search for Kitaev quantum spin liquids led to the discovery of many honeycomb lattice materials. Much attention has been paid to materials without magnetic order down to the lowest temperatures. The newly synthesized Na-deficient Na x IrO 3 has been found to bear no sign of long-range magnetic order above 1 K from physical property measurements. In this paper, we report momentum-and energy-resolved excitation spectra in Na-deficient Na x IrO 3 measured using a resonant inelastic x-ray scattering spectrometer. Orbital excitation spectra show that the octahedral and trigonal crystal field splittings are larger in Na x IrO 3 than in Na 2 IrO 3 . On the other hand, the low-energy spectrum at low temperature shows a wave-vector dispersion and a spectral weight distribution that are similar to those of Na 2 IrO 3 , revealing that the two-dimensional zigzag magnetic correlations in Na x IrO 3 are similar to those in Na 2 IrO 3 in terms of the ordered magnetic moment direction and three dynamically fluctuating zigzag orders. The azimuth angle dependence of the low-energy spectrum corroborates these results. The two-dimensional zigzag magnetic correlations rapidly weaken until 50 K. At high temperatures, the spectral weight distribution of the low-energy excitation resembles that of the pure Kitaev model, indicating that the Kitaev interaction dominates the dynamic magnetic response at high temperature. Here we suggest that the larger crystal field and distortion and the weakened longer-range Heisenberg exchange interactions due to the Na deficiency in Na x IrO 3 contribute to bring Na x IrO 3 away from the zigzag long-range magnetic order phase.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Spinons and damped phonons in the spin- 1 2 quantum liquid Ba 4 Ir 3 O 10 observed by Raman scattering
In spin-1/2 Mott insulators, nonmagnetic quantum liquid phases are often argued to arise when the system shows no magnetic ordering, but identifying positive signatures of these phases or related spinon quasiparticles can be elusive. Here, we use Raman scattering to provide three signatures for spinons in a possible spin-orbit quantum liquid material Ba 4 Ir 3 O 10 : (1) a broad hump, which we show can arise from Luttinger liquid spinons in Raman with parallel photon polarizations normal to one-dimensional chains; (2) strong phonon damping from phonon-spin coupling via the spin-orbit interaction; and (3) the absence of (1) and (2) in the magnetically ordered phase that is produced when 2% of Ba is substituted by Sr [(Ba 0.98 Sr 0.02 ) 4 Ir 3 O 10 ]. Furthermore, the phonon damping via itinerant spinons seen in this quantum liquid insulator suggests a mechanism for enhancing thermoelectricity in strongly correlated conductors, through a neutral quantum liquid that need not affect electronic transport.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Lattice flexibility in Ca 3 Ru 2 O 7 : Control of electrical transport via anisotropic magnetostriction
We report that Ca 3 Ru 2 O 7 is a correlated and spin-orbit coupled system with an extraordinary anisotropy. It is both interesting and unique largely because this material exhibits conflicting phenomena that are often utterly inconsistent with traditional precedents, particularly, the quantum oscillations in the nonmetallic state and colossal magnetoresistivity achieved by avoiding a fully spin-polarized state. This work focuses on the relationship between the lattice and transport properties along each crystalline axis and reveals that application of magnetic field, H, along different crystalline axes readily stretches or shrinks the lattice in a uniaxial manner, resulting in distinct electronic states. Furthermore, application of modest pressure drastically amplifies the anisotropic magnetoelastic effect, leading to either an occurrence of a robust metallic state at H $∥$ hard axis or a reentrance of the nonmetallic state at H $∥$ easy axis. Ca3Ru2O7 presents a rare lattice-dependent magnetotransport mechanism, in which the extraordinary lattice flexibility enables an exquisite control of the electronic state via magnetically stretching or shrinking the crystalline axes, and the spin polarization plays an unconventional role unfavorable for maximizing conductivity. At the heart of the intriguing physics is the anisotropic magnetostriction that leads to exotic states.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Ground state in proximity to a possible Kitaev spin liquid: The undistorted honeycomb iridate Na x IrO 3 (0.60 ≤ x ≤ 0.80)
Here, we report the results of our study of a recently synthesized honeycomb iridate Na x IrO 3 (0.60 ≤ x ≤ 0.80). Single-crystal Na x IrO 3 adopts a honeycomb lattice noticeably without distortions and stacking disorder inherently existent in its sister compound Na 2 IrO 3 . The oxidation state of the Ir ion is a mixed valence state resulting from a majority Ir 5+ (5d 4 ) ion and a minority Ir 6+ (5d 3 ) ion. Na x IrO 3 is a Mott insulator likely with a predominant pseudospin =1 state. It exhibits an effective moment of 1.1 μB/Ir and a Curie-Weiss temperature of –19 K but with no discernible long-range order above 1 K. The physical behavior below 1 K features two prominent anomalies at T h = 0.9 K and T l = 0.12 K in both the heat capacity and AC magnetic susceptibility. Intermediate between T h and T l lies a pronounced temperature linearity of the heat capacity with a large slope of 77 mJ /mole K 2 , a feature expected for highly correlated metals but not at all for insulators. These results along with a comparison drawn with the honeycomb lattices Na 2 IrO 3 and (Na 0.2 Li 0.8 ) 2 IrO 3 point to an exotic ground state in proximity to a possible Kitaev spin liquid.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr 2 Ir O 4 : A study of Sr 2 Ir 1 – x M x O 4 ( M = Fe or Co)
Sr 2 IrO 4 is an archetypal spin-orbit-coupled Mott insulator with an antiferromagnetic state below 240 K. Here we report results of our study on single crystals of Sr 2 Ir 1–x Fe x O 4 (0 ≤ x < 0.32) and Sr 2 Ir 1–x Co x O 4 (0 ≤ x < 0.22). Fe doping retains the antiferromagnetic state but simultaneously precipitates an emergent metallic state whereas Co doping causes a rapid collapse of both the antiferromagnetic and Mott states, giving rise to a confined metallic state featuring a pronounced linearity of the basal-plane resistivity up to 700 K. The results indicate tetravalent Fe 4+ (3d 4 ) ions in the intermediate spin state with S = 1 and Co 4+ (3d 5 ) ions in the high spin state with S = 5/2 substituting for Ir 4+ (5d 5 ) ions in Sr 2 IrO 4 , respectively. The effective magnetic moment closely tracks the Néel temperature as doping increases, suggesting that the spin state of the dopant predominately determines the magnetic properties in doped Sr 2 IrO 4 . Furthermore, all relevant properties including charge-carrier density (e.g., 10 28 /m 3 ), Sommerfeld coefficient (e.g., 19 mJ / mole K 2 ), and Wilson ratio (e.g., 2.6) consistently demonstrate an emergent metallic state that is both robust and highly correlated in the two systems, arising from the percolation of bound states and the weakening of structural distortions. Furthermore, this study strongly indicates that the antiferromagnetic and Mott states are correlated in an unconventional manner in Sr 2 IrO 4 .
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Pseudospin-lattice coupling and electric control of the square-lattice iridate Sr2IrO4
Sr 2 IrO 4 is an archetypal spin-orbit-coupled Mott insulator and has been extensively studied in part because of a wide range of predicted states. Limited experimental characterization of these states thus far brings to light the extraordinary susceptibility of the physical properties to the lattice, particularly, the Ir-O-Ir bond angle. Here, we report a microscopic rotation of the IrO 6 octahedra below 50 K measured by single crystal neutron diffraction. Overall, this sharp lattice anomaly provides keys to understanding the anomalous low-temperature physics and a direct confirmation of a crucial role that the Ir-O-Ir bond angle plays in determining the ground state. Indeed, as also demonstrated in this study, applied electric current readily weakens the antiferromagnetic order via the straightening of the Ir-O-Ir bond angle, highlighting that even slight change in the local structure can disproportionately affect the physical properties in the spin-orbit-coupled system.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Quantum liquid from strange frustration in the trimer magnet Ba4Ir3O10
Abstract Quantum spin systems such as magnetic insulators usually show magnetic order, but such classical states can give way to quantum liquids with exotic entanglement through two known mechanisms of frustration: geometric frustration in lattices with triangle motifs, and spin-orbit-coupling frustration in the exactly solvable quantum liquid of Kitaev’s honeycomb lattice. Here we present the experimental observation of a new kind of frustrated quantum liquid arising in an unlikely place: the magnetic insulator Ba 4 Ir 3 O 10 where Ir 3 O 12 trimers form an unfrustrated square lattice. The crystal structure shows no apparent spin chains. Experimentally we find a quantum liquid state persisting down to 0.2 K that is stabilized by strong antiferromagnetic interaction with Curie–Weiss temperature ranging from −766 to −169 K due to magnetic anisotropy. The anisotropy-averaged frustration parameter is 2000, seldom seen in iridates. Heat capacity and thermal conductivity are both linear at low temperatures, a familiar feature in metals but here in an insulator pointing to an exotic quantum liquid state; a mere 2% Sr substitution for Ba produces long-range order at 130 K and destroys the linear-T features. Although the Ir 4+ (5d 5 ) ions in Ba 4 Ir 3 O 10 appear to form Ir 3 O 12 trimers of face-sharing IrO 6 octahedra, we propose that intra-trimer exchange is reduced and the lattice recombines into an array of coupled 1D chains with additional spins. An extreme limit of decoupled 1D chains can explain most but not all of the striking experimental observations, indicating that the inter-chain coupling plays an important role in the frustration mechanism leading to this quantum liquid.
36 MATERIALS SCIENCE↗