Spin-orbit coupling controlled ground states in the double perovskite iridates $$\textit{A}_2\textit{B}$$IrO$$_6$$ ($$\textit{A}$$ = Ba, Sr; $$\textit{B}$$ = Lu, Sc)
Abstract
Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $$\textit{J}$$ = 0 electronic ground state for each Ir5+ ion. The major focus of prior research has been on the double perovskite iridates Ba2YIrO6 and Sr2YIrO6, where the nature of the ground states (i.e., ordered vs nonmagnetic) is still controversial. Here, we present neutron powder diffraction, high-energy-resolution fluorescence-detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba2LuIrO6, Sr2LuIrO6, Ba2ScIrO6, and Sr2ScIrO6 that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. In this work, our HERFD-XAS and RIXS measurements establish $$\textit{J}$$ = 0 electronic ground states for the Ir5+ ions in all cases, with similar values for Hund's coupling $$J_H$$ and the spin-orbit coupling constant $$λ_{\text{SOC}}$$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do exhibit weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $$λ_{\text{SOC}}$$ is the key driving force behind the electronic and magnetic ground states realized in the $5d^4$ double perovskite iridates, which agrees well with conventional wisdom.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- McMaster Univ., Hamilton, ON (Canada)
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- Cornell Univ., Ithaca, NY (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
- Villanova Univ., PA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC)
- OSTI Identifier:
- 1892414
- Grant/Contract Number:
- AC05-00OR22725; DMR-1829070; AC02-06CH11357; DMR-1455264; DMR-2003117
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Aczel, Adam A., Chen, Q., Clancy, J. P., dela Cruz, Clarina R., Reig-i-Plessis, D., MacDougall, G. J., Pollock, C. J., Upton, M. H., Williams, Travis J., LaManna, N., Carlo, J. P., Beare, J., Luke, G. M., and Zhou, H. D. Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc). United States: N. p., 2022.
Web. doi:10.1103/physrevmaterials.6.094409.
Aczel, Adam A., Chen, Q., Clancy, J. P., dela Cruz, Clarina R., Reig-i-Plessis, D., MacDougall, G. J., Pollock, C. J., Upton, M. H., Williams, Travis J., LaManna, N., Carlo, J. P., Beare, J., Luke, G. M., & Zhou, H. D. Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc). United States. https://doi.org/10.1103/physrevmaterials.6.094409
Aczel, Adam A., Chen, Q., Clancy, J. P., dela Cruz, Clarina R., Reig-i-Plessis, D., MacDougall, G. J., Pollock, C. J., Upton, M. H., Williams, Travis J., LaManna, N., Carlo, J. P., Beare, J., Luke, G. M., and Zhou, H. D. Mon .
"Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc)". United States. https://doi.org/10.1103/physrevmaterials.6.094409. https://www.osti.gov/servlets/purl/1892414.
@article{osti_1892414,
title = {Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc)},
author = {Aczel, Adam A. and Chen, Q. and Clancy, J. P. and dela Cruz, Clarina R. and Reig-i-Plessis, D. and MacDougall, G. J. and Pollock, C. J. and Upton, M. H. and Williams, Travis J. and LaManna, N. and Carlo, J. P. and Beare, J. and Luke, G. M. and Zhou, H. D.},
abstractNote = {Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $\textit{J}$ = 0 electronic ground state for each Ir5+ ion. The major focus of prior research has been on the double perovskite iridates Ba2YIrO6 and Sr2YIrO6, where the nature of the ground states (i.e., ordered vs nonmagnetic) is still controversial. Here, we present neutron powder diffraction, high-energy-resolution fluorescence-detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba2LuIrO6, Sr2LuIrO6, Ba2ScIrO6, and Sr2ScIrO6 that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. In this work, our HERFD-XAS and RIXS measurements establish $\textit{J}$ = 0 electronic ground states for the Ir5+ ions in all cases, with similar values for Hund's coupling $J_H$ and the spin-orbit coupling constant $λ_{\text{SOC}}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do exhibit weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\text{SOC}}$ is the key driving force behind the electronic and magnetic ground states realized in the $5d^4$ double perovskite iridates, which agrees well with conventional wisdom.},
doi = {10.1103/physrevmaterials.6.094409},
journal = {Physical Review Materials},
number = 9,
volume = 6,
place = {United States},
year = {Mon Sep 19 00:00:00 EDT 2022},
month = {Mon Sep 19 00:00:00 EDT 2022}
}
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