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Charge-state dependent spin-orbit coupling and quantum phase transitions in Ir-Ru oxides
Department of Physics, Bennett University, Greater Noida-201310, Uttar Pradesh, India.
Department of Applied Sciences, Galgotias College of Engineering and Technology, Greater Noida, India.
Department of Physics and Astronomy, Uppsala University, Box 516, SE-751 20 Uppsala, Sweden.
Department of Physics, Bennett University, Greater Noida-201310, Uttar Pradesh, India.
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2025 (engelsk)Inngår i: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 111, nr 19, artikkel-id 195148Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

The competition between kinematic, relativistic, and Coulomb interactions has spurred intense experimental and theoretical investigations in iridium-based oxides. Their electronic structure is mostly understood in terms of the spin-orbital coupled effective J state (Jeff). However, the role of the Ir charge state in shaping the strength of effective spin-orbit coupling and defining the stability of the Jeff ground state has not been thoroughly explored. We argue here that the iridium-ruthenium triple perovskites, Ba3MRuIrO9 (M=Li, Mg, and In), are of particular interest in this regard. Using ab initio theory, we show here that the nominal charge states of Ir can be tuned from +6 (5d3) to +4 (5d5) by choosing nonmagnetic M ions as Li(+1), Mg(+2), and In(+3), while the Ru ions always remain in nominal +5 (4d3) charge state. This variation modulates the influence of the spin-orbit coupling (SOC), which is found to be negligible in Ba3LiRuIrO9, moderate in Ba3MgRuIrO9, and determining in Ba3InRuIrO9. Our analysis classifies Ba3LiRuIrO9 as a correlation-driven insulator arising from Hubbard interactions and exchange-split t2g states, Ba3MgRuIrO9 as a SOC and correlation-driven insulator that does not conform to the commonly expected J=0 ground state and Ba3InRuIrO9 as Jeff=1/2 Mott-Hubbard insulator. In the data reported here, the correlational electronic structure theory results in sizable magnetic moments of both Ru and Ir atoms in these systems and atomistic spin-dynamics simulations capture the experimental Néel temperature for Ba3LiRuIrO9 and Ba3MgRuIrO9 and provide evidence for a phase transition for Ba3InRuIrO9 when T → 0 K, to a multivalley magnetic state with strong magnetic frustration. The theory identifies that strong SOC in Ba3InRuIrO9 induces bond-dependent magnetic couplings with significant Dzyaloshinskii-Moriya interaction, strong symmetric anisotropic exchange, and finite in-plane single-ion anisotropy. The realization of such strong anisotropic interactions helps to stabilize a particularly complex energy landscape of Ba3InRuIrO9, which opens up for exotic magnetic quantum phases such as quantum spin liquid. Thus, by comparing the electronic structure and magnetism of isostructural iridates with different Ir-charge states, we provided a theoretical framework to demonstrate the structural and electronic conditions that drive the deviations from conventional magnetic ordering, facilitating the emergence of exotic quantum phases.

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American Physical Society (APS) , 2025. Vol. 111, nr 19, artikkel-id 195148
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URN: urn:nbn:se:kth:diva-364152DOI: 10.1103/PhysRevB.111.195148ISI: 001501648400004Scopus ID: 2-s2.0-105005831842OAI: oai:DiVA.org:kth-364152DiVA, id: diva2:1964108
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QC 20250604

Tilgjengelig fra: 2025-06-04 Laget: 2025-06-04 Sist oppdatert: 2025-12-05bibliografisk kontrollert

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