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Title: Spin-orbit tuned metal-insulator transitions in single-crystal Sr₂Ir1–xRhxO₄ (0≤x≤1)

Sr₂IrO₄ is a magnetic insulator driven by spin-orbit interaction (SOI) whereas the isoelectronic and isostructural Sr₂RhO₄ is a paramagnetic metal. The contrasting ground states have been shown to result from the critical role of the strong SOI in the iridate. Our investigation of structural, transport, magnetic, and thermal properties reveals that substituting 4d Rh⁴⁺ (4d⁵) ions for 5d Ir⁴⁺ (5d⁵) ions in Sr₂IrO₄ directly reduces the SOI and rebalances the competing energies so profoundly that it generates a rich phase diagram for Sr₂Ir1–xRhxO₄ featuring two major effects: (1) Light Rh doping (0 ≤ x ≤ 0.16) prompts a simultaneous and precipitous drop in both the electrical resistivity and the magnetic ordering temperature TC, which is suppressed to zero at x = 0.16 from 240 K at x = 0. (2) However, with heavier Rh doping [0.24 < x < 0.85 (±0.05)] disorder scattering leads to localized states and a return to an insulating state with spin frustration and exotic magnetic behavior that only disappears near x = 1. The intricacy of Sr₂Ir1–xRhxO₄ is further highlighted by comparison with Sr₂Ir1–xRuxO₄ where Ru⁴⁺ (4d⁴) drives a direct crossover from the insulating to metallic states.
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Publication Date:
Publisher's Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 86; Journal Issue: 12; Related Information: CHORUS Timestamp: 2017-04-06 12:33:43; Journal ID: ISSN 1098-0121
American Physical Society
Sponsoring Org:
Country of Publication:
United States
OSTI Identifier: