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1. Inhomogeneous Kondo-lattice in geometrically frustrated Pr2Ir2O7

   https://doi.org/s41467-021-21698-z  

   Kavai, Mariam; Friedman, Joel; Sherman, Kyle; Gong, Mingda; Giannakis, Ioannis; Hajinazar, Samad; Hu, Haoyu; Grefe, Sarah E; Leshen, Justin; Yang, Qiu; et al (March 2021, Nature communications)

   null (Ed.)

   Magnetic fluctuations induced by geometric frustration of local Ir-spins disturb the formation of long-range magnetic order in the family of pyrochlore iridates. As a consequence, Pr2Ir2O7 lies at a tuning-free antiferromagnetic-to-paramagnetic quantum critical point and exhibits an array of complex phenomena including the Kondo effect, biquadratic band structure, and metallic spin liquid. Using spectroscopic imaging with the scanning tunneling microscope, complemented with machine learning, density functional theory and theoretical modeling, we probe the local electronic states in Pr2Ir2O7 and find an electronic phase separation. Nanoscale regions with a well-defined Kondo resonance are interweaved with a non-magnetic metallic phase with Kondo-destruction. These spatial nanoscale patterns display a fractal geometry with power-law behavior extended over two decades, consistent with being in proximity to a critical point. Our discovery reveals a nanoscale tuning route, viz. using a spatial variation of the electronic potential as a means of adjusting the balance between Kondo entanglement and geometric frustration. 

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2. Searching for a route to synthesize in situ epitaxial Pr2Ir2O7 thin films with thermodynamic methods

   https://doi.org/10.1038/s41524-021-00610-9  

   Guo, Lu; Shang, Shun-Li; Campbell, Neil; Evans, Paul G.; Rzchowski, Mark; Liu, Zi-Kui; Eom, Chang-Beom (September 2021, npj Computational Materials)

   Abstract In situ growth of pyrochlore iridate thin films has been a long-standing challenge due to the low reactivity of Ir at low temperatures and the vaporization of volatile gas species such as IrO₃(g) and IrO₂(g) at high temperatures and highP_O2. To address this challenge, we combine thermodynamic analysis of the Pr-Ir-O₂system with experimental results from the conventional physical vapor deposition (PVD) technique of co-sputtering. Our results indicate that only high growth temperatures yield films with crystallinity sufficient for utilizing and tailoring the desired topological electronic properties and the in situ synthesis of Pr₂Ir₂O₇thin films is fettered by the inability to grow withP_O2on the order of 10 Torr at high temperatures, a limitation inherent to the PVD process. Thus, we suggest techniques capable of supplying high partial pressure of key species during deposition, in particular chemical vapor deposition (CVD), as a route to synthesis of Pr₂Ir₂O₇. 

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3. Quantum liquid from strange frustration in the trimer magnet Ba4Ir3O10

   https://doi.org/10.1038/s41535-020-0232-6  

   Cao, Gang; Zheng, Hao; Zhao, Hengdi; Ni, Yifei; Pocs, Christopher A.; Zhang, Yu; Ye, Feng; Hoffmann, Christina; Wang, Xiaoping; Lee, Minhyea; et al (May 2020, npj Quantum Materials)

   Abstract Quantum spin systems such as magnetic insulators usually show magnetic order, but such classical states can give way toquantum liquids with exotic entanglementthrough 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 Ba₄Ir₃O₁₀where Ir₃O₁₂trimers 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 Ir⁴⁺(5d⁵) ions in Ba₄Ir₃O₁₀appear to form Ir₃O₁₂trimers of face-sharing IrO₆octahedra, 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. 

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4. Antiferromagnetic excitonic insulator state in Sr3Ir2O7

   https://doi.org/10.1038/s41467-022-28207-w  

   Mazzone, D. G.; Shen, Y.; Suwa, H.; Fabbris, G.; Yang, J.; Zhang, S. -S.; Miao, H.; Sears, J.; Jia, Ke; Shi, Y. G.; et al (February 2022, Nature Communications)

   Abstract Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr₃Ir₂O₇. By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material’s resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr₃Ir₂O₇indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase. 

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5. Stabilization of three-dimensional charge order through interplanar orbital hybridization in PrxY1−xBa2Cu3O6+δ

   https://doi.org/10.1038/s41467-022-33607-z  

   Ruiz, Alejandro; Gunn, Brandon; Lu, Yi; Sasmal, Kalyan; Moir, Camilla M.; Basak, Rourav; Huang, Hai; Lee, Jun-Sik; Rodolakis, Fanny; Boyle, Timothy J.; et al (October 2022, Nature Communications)

   Abstract The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the$${d}_{{x}^{2}-{y}^{2}}$$ $d_{x^2-y^2}$orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using CuL₃and PrM₅resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa₂Cu₃O₇, where the Prf-electrons create a direct orbital bridge between CuO₂planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials. 

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