Pressure-driven collapse of the relativistic electronic ground state in a honeycomb

J. Patrick Clancy; Hlynur Gretarsson; Jennifer A. Sears; Yogesh Singh; Serge Desgreniers; Kavita Mehlawat; Samar Layek; Gregory Kh Rozenberg; Yang Ding; Mary H. Upton; Diego Casa; Ning Chen; Junhyuck Im; Yongjae Lee; Ravi Yadav; Liviu Hozoi; Dmitri Efremov; Jeroen Van Den Brink; Young June Kim

doi:10.1038/s41535-018-0109-0

Pressure-driven collapse of the relativistic electronic ground state in a honeycomb

J. Patrick Clancy, Hlynur Gretarsson, Jennifer A. Sears, Yogesh Singh, Serge Desgreniers, Kavita Mehlawat, Samar Layek, Gregory Kh Rozenberg, Yang Ding, Mary H. Upton, Diego Casa, Ning Chen, Junhyuck Im, Yongjae Lee, Ravi Yadav, Liviu Hozoi, Dmitri Efremov, Jeroen Van Den Brink, Young June Kim

Research output: Contribution to journal › Article › peer-review

33 Citations (Scopus)

Abstract

Honeycomb-lattice quantum magnets with strong spin-orbit coupling are promising candidates for realizing a Kitaev quantum spin liquid. Although iridate materials such as Li₂IrO₃ and Na₂IrO₃ have been extensively investigated in this context, there is still considerable debate as to whether a localized relativistic wavefunction (J _eff = 1/2) provides a suitable description for the electronic ground state of these materials. To address this question, we have studied the evolution of the structural and electronic properties of α-Li₂IrO₃ as a function of applied hydrostatic pressure using a combination of X-ray diffraction and X-ray spectroscopy techniques. We observe striking changes even under the application of only small hydrostatic pressure (P ≤ 0.1 GPa): A distortion of the Ir honeycomb lattice (via X-ray diffraction), a dramatic decrease in the strength of spin-orbit coupling effects (via X-ray absorption spectroscopy), and a significant increase in non-cubic crystal electric field splitting (via resonant inelastic X-ray scattering). Our data indicate that α-Li₂IrO₃ is best described by a J _eff = 1/2 state at ambient pressure, but demonstrate that this state is extremely fragile and collapses under the influence of applied pressure.

Original language	English
Article number	35
Journal	npj Quantum Materials
Volume	3
Issue number	1
DOIs	https://doi.org/10.1038/s41535-018-0109-0
Publication status	Published - 2018 Dec 1

Bibliographical note

Funding Information:
Work at the University of Toronto was supported by the Natural Science and Engineering Research Council (NSERC) of Canada through the Collaborative Research and Training Experience (CREATE) program (432242-2013) and a Discovery Grant (RGPIN-2014-06071). Y.S. acknowledges DST, India for support through DST Grant No. SB/S2/CMP-001/2013. S. D. acknowledges support from NSERC. K.M. acknowledges UGC-CSIR India for a fellowship. G. R. acknowledges Israeli Science Foundation Grant #1189/14. Y.D is supported by NSFC Grant No. U1530402, National Key R & D Program of China 2018YFA0305703 and the Science Challenge Project, No. TZ2016001. Y.L. thanks the support by the National Research Foundation of Korea (NRF) grant (No. 2018R1A3B1052042) funded by the Korea government (MSIP). Research described in this paper was performed at the Canadian Light Source, which is supported by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. In addition, this research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Publisher Copyright:
© 2018 The Author(s).

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
Condensed Matter Physics

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10.1038/s41535-018-0109-0

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Clancy, J. P., Gretarsson, H., Sears, J. A., Singh, Y., Desgreniers, S., Mehlawat, K., Layek, S., Rozenberg, G. K., Ding, Y., Upton, M. H., Casa, D., Chen, N., Im, J., Lee, Y., Yadav, R., Hozoi, L., Efremov, D., Van Den Brink, J., & Kim, Y. J. (2018). Pressure-driven collapse of the relativistic electronic ground state in a honeycomb. npj Quantum Materials, 3(1), Article 35. https://doi.org/10.1038/s41535-018-0109-0

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title = "Pressure-driven collapse of the relativistic electronic ground state in a honeycomb",

abstract = "Honeycomb-lattice quantum magnets with strong spin-orbit coupling are promising candidates for realizing a Kitaev quantum spin liquid. Although iridate materials such as Li2IrO3 and Na2IrO3 have been extensively investigated in this context, there is still considerable debate as to whether a localized relativistic wavefunction (J eff = 1/2) provides a suitable description for the electronic ground state of these materials. To address this question, we have studied the evolution of the structural and electronic properties of α-Li2IrO3 as a function of applied hydrostatic pressure using a combination of X-ray diffraction and X-ray spectroscopy techniques. We observe striking changes even under the application of only small hydrostatic pressure (P ≤ 0.1 GPa): A distortion of the Ir honeycomb lattice (via X-ray diffraction), a dramatic decrease in the strength of spin-orbit coupling effects (via X-ray absorption spectroscopy), and a significant increase in non-cubic crystal electric field splitting (via resonant inelastic X-ray scattering). Our data indicate that α-Li2IrO3 is best described by a J eff = 1/2 state at ambient pressure, but demonstrate that this state is extremely fragile and collapses under the influence of applied pressure.",

author = "Clancy, {J. Patrick} and Hlynur Gretarsson and Sears, {Jennifer A.} and Yogesh Singh and Serge Desgreniers and Kavita Mehlawat and Samar Layek and Rozenberg, {Gregory Kh} and Yang Ding and Upton, {Mary H.} and Diego Casa and Ning Chen and Junhyuck Im and Yongjae Lee and Ravi Yadav and Liviu Hozoi and Dmitri Efremov and {Van Den Brink}, Jeroen and Kim, {Young June}",

note = "Funding Information: Work at the University of Toronto was supported by the Natural Science and Engineering Research Council (NSERC) of Canada through the Collaborative Research and Training Experience (CREATE) program (432242-2013) and a Discovery Grant (RGPIN-2014-06071). Y.S. acknowledges DST, India for support through DST Grant No. SB/S2/CMP-001/2013. S. D. acknowledges support from NSERC. K.M. acknowledges UGC-CSIR India for a fellowship. G. R. acknowledges Israeli Science Foundation Grant #1189/14. Y.D is supported by NSFC Grant No. U1530402, National Key R & D Program of China 2018YFA0305703 and the Science Challenge Project, No. TZ2016001. Y.L. thanks the support by the National Research Foundation of Korea (NRF) grant (No. 2018R1A3B1052042) funded by the Korea government (MSIP). Research described in this paper was performed at the Canadian Light Source, which is supported by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. In addition, this research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2018 The Author(s).",

year = "2018",

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doi = "10.1038/s41535-018-0109-0",

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Clancy, JP, Gretarsson, H, Sears, JA, Singh, Y, Desgreniers, S, Mehlawat, K, Layek, S, Rozenberg, GK, Ding, Y, Upton, MH, Casa, D, Chen, N, Im, J, Lee, Y, Yadav, R, Hozoi, L, Efremov, D, Van Den Brink, J & Kim, YJ 2018, 'Pressure-driven collapse of the relativistic electronic ground state in a honeycomb', npj Quantum Materials, vol. 3, no. 1, 35. https://doi.org/10.1038/s41535-018-0109-0

TY - JOUR

T1 - Pressure-driven collapse of the relativistic electronic ground state in a honeycomb

AU - Clancy, J. Patrick

AU - Gretarsson, Hlynur

AU - Sears, Jennifer A.

AU - Singh, Yogesh

AU - Desgreniers, Serge

AU - Mehlawat, Kavita

AU - Layek, Samar

AU - Rozenberg, Gregory Kh

AU - Ding, Yang

AU - Upton, Mary H.

AU - Casa, Diego

AU - Chen, Ning

AU - Im, Junhyuck

AU - Lee, Yongjae

AU - Yadav, Ravi

AU - Hozoi, Liviu

AU - Efremov, Dmitri

AU - Van Den Brink, Jeroen

AU - Kim, Young June

N1 - Funding Information: Work at the University of Toronto was supported by the Natural Science and Engineering Research Council (NSERC) of Canada through the Collaborative Research and Training Experience (CREATE) program (432242-2013) and a Discovery Grant (RGPIN-2014-06071). Y.S. acknowledges DST, India for support through DST Grant No. SB/S2/CMP-001/2013. S. D. acknowledges support from NSERC. K.M. acknowledges UGC-CSIR India for a fellowship. G. R. acknowledges Israeli Science Foundation Grant #1189/14. Y.D is supported by NSFC Grant No. U1530402, National Key R & D Program of China 2018YFA0305703 and the Science Challenge Project, No. TZ2016001. Y.L. thanks the support by the National Research Foundation of Korea (NRF) grant (No. 2018R1A3B1052042) funded by the Korea government (MSIP). Research described in this paper was performed at the Canadian Light Source, which is supported by the Canada Foundation for Innovation, the Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. In addition, this research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2018 The Author(s).

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Honeycomb-lattice quantum magnets with strong spin-orbit coupling are promising candidates for realizing a Kitaev quantum spin liquid. Although iridate materials such as Li2IrO3 and Na2IrO3 have been extensively investigated in this context, there is still considerable debate as to whether a localized relativistic wavefunction (J eff = 1/2) provides a suitable description for the electronic ground state of these materials. To address this question, we have studied the evolution of the structural and electronic properties of α-Li2IrO3 as a function of applied hydrostatic pressure using a combination of X-ray diffraction and X-ray spectroscopy techniques. We observe striking changes even under the application of only small hydrostatic pressure (P ≤ 0.1 GPa): A distortion of the Ir honeycomb lattice (via X-ray diffraction), a dramatic decrease in the strength of spin-orbit coupling effects (via X-ray absorption spectroscopy), and a significant increase in non-cubic crystal electric field splitting (via resonant inelastic X-ray scattering). Our data indicate that α-Li2IrO3 is best described by a J eff = 1/2 state at ambient pressure, but demonstrate that this state is extremely fragile and collapses under the influence of applied pressure.

AB - Honeycomb-lattice quantum magnets with strong spin-orbit coupling are promising candidates for realizing a Kitaev quantum spin liquid. Although iridate materials such as Li2IrO3 and Na2IrO3 have been extensively investigated in this context, there is still considerable debate as to whether a localized relativistic wavefunction (J eff = 1/2) provides a suitable description for the electronic ground state of these materials. To address this question, we have studied the evolution of the structural and electronic properties of α-Li2IrO3 as a function of applied hydrostatic pressure using a combination of X-ray diffraction and X-ray spectroscopy techniques. We observe striking changes even under the application of only small hydrostatic pressure (P ≤ 0.1 GPa): A distortion of the Ir honeycomb lattice (via X-ray diffraction), a dramatic decrease in the strength of spin-orbit coupling effects (via X-ray absorption spectroscopy), and a significant increase in non-cubic crystal electric field splitting (via resonant inelastic X-ray scattering). Our data indicate that α-Li2IrO3 is best described by a J eff = 1/2 state at ambient pressure, but demonstrate that this state is extremely fragile and collapses under the influence of applied pressure.

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Pressure-driven collapse of the relativistic electronic ground state in a honeycomb

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