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In the quasi-one-dimensional cuprate PrBa$_2$Cu$_4$O$_8$, the Pr cations order antiferromagnetically at 17 K in zero field. Through a combination of magnetic susceptibility, torque magnetometry, specific heat and interchain transport measurements, the anisotropic temperature-magnetic field phase diagram associated with this ordering has been mapped out. A low-temperature spin-flop transition in the Pr sub-lattice is found to occur at the same magnetic field strength and orientation as a dimensional crossover in the ground state of the metallic CuO chains. This coincidence suggests that the spin reorientation is driven by a change in the anisotropic Rudermann-Kittel-Kasuya-Yosida (RKKY) interaction induced by a corresponding change in effective dimensionality of the conduction electrons.
Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr$_3$Ir$_2$O$_7$, a significant contrast to the single layer Sr$_2$IrO$_4$ with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO$_2$ layers is due to strong competition among intra- and inter-layer bond-directional pseudo-dipolar interactions of the spin-orbit entangled $J_{eff}$=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5$d$ transition metal oxides.
Upon reduction of the film thickness we observe a metal-insulator transition in epitaxially stabilized, spin-orbit coupled SrIrO$_3$ ultrathin films. By comparison of the experimental electronic dispersions with density functional theory at various levels of complexity we identify the leading microscopic mechanisms, i.e., a dimensionality-induced re-adjustment of octahedral rotations, magnetism, and electronic correlations. The astonishing resemblance of the band structure in the two-dimensional limit to that of bulk Sr$_2$IrO$_4$ opens new avenues to unconventional superconductivity by clean electron doping through electric field gating.
Calcium vanadate CaV$_2$O$_4$ has a crystal structure of quasi-one-dimensional zigzag chains composed of orbital-active V$^{3+}$ ions and undergoes successive structural and antiferromagnetic phase transitions at $T_ssim 140$ K and $T_N sim 70$ K, respectively. We perform ultrasound velocity measurements on a single crystal of CaV$_2$O$_4$. The temperature dependence of its shear elastic moduli exhibits huge Curie-type softening upon cooling that emerges above and below $T_s$ depending on the elastic mode. The softening above $T_s$ suggests the presence of either onsite Jahn-Teller-type or intersite ferro-type orbital fluctuations in the two inequivalent V$^{3+}$ zigzag chains. The softening below $T_s$ suggests the occurrence of a dimensional spin-state crossover, from quasi-one to three, that is driven by the spin-lattice coupling along the inter-zigzag-chain orthogonal direction. The successive emergence of the orbital- and spin-driven lattice instabilities above and below $T_s$, respectively, is unique to the orbital-spin zigzag chain system of CaV$_2$O$_4$.
By means of nuclear spin-lattice relaxation rate 1/T1, we follow the spin dynamics as a function of the applied magnetic field in two gapped one-dimensional quantum antiferromagnets: the anisotropic spin-chain system NiCl2-4SC(NH2)2 and the spin-ladder system (C5H12N)2CuBr4. In both systems, spin excitations are confirmed to evolve from magnons in the gapped state to spinons in the gapples Tomonaga-Luttinger-liquid state. In between, 1/T1 exhibits a pronounced, continuous variation, which is shown to scale in accordance with quantum criticality. We extract the critical exponent for 1/T1, compare it to the theory, and show that this behavior is identical in both studied systems, thus demonstrating the universality of quantum critical behavior.
The microscopic mechanism of the metal-insulator transition is studied by orbital-resolved 51V NMR spectroscopy in a prototype of the quasi-one-dimensional system V6O13. We uncover that the transition involves a site-selective d orbital order lifting twofold orbital degeneracy in one of the two VO6 chains. The other chain leaves paramagnetic moments on the singly occupied dxy orbital across the transition. The two chains respectively stabilize an orbital-assisted spin-Peierls state and an antiferromagnetic long-range order in the ground state. The site-selective Mott transition may be a source of the anomalous metal and the Mott-Peierls duality.