Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K2Ni2(SO4)3

Ivica Živković; Virgile Favre; Catalina Salazar Mejia; Harald O. Jeschke; Arnaud Magrez; Bhupen Dabholkar; Vincent Noculak; Rafael S. Freitas; Minki Jeong; Nagabhushan G. Hegde; Luc Testa; Peter Babkevich; Yixi Su; Pascal Manuel; Hubertus Luetkens; Christopher Baines; Peter J. Baker; Jochen Wosnitza; Oksana Zaharko; Yasir Iqbal; Johannes Reuther; Henrik M. Rønnow

doi:10.1103/PhysRevLett.127.157204

Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K₂Ni₂(SO₄)₃

Ivica Živković, Virgile Favre, Catalina Salazar Mejia, Harald O. Jeschke, Arnaud Magrez, Bhupen Dabholkar, Vincent Noculak, Rafael S. Freitas, Minki Jeong, Nagabhushan G. Hegde, Luc Testa, Peter Babkevich, Yixi Su, Pascal Manuel, Hubertus Luetkens, Christopher Baines, Peter J. Baker, Jochen Wosnitza, Oksana Zaharko, Yasir IqbalJohannes Reuther, Henrik M. Rønnow

Physics and Astronomy

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Abstract

Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K₂Ni₂(SO₄)₃ forming a three-dimensional network of Ni²⁺ spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B≳4T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.

Original language	English
Article number	157204
Number of pages	7
Journal	Physical Review Letters
Volume	127
Issue number	15
Early online date	6 Oct 2021
DOIs	https://doi.org/10.1103/PhysRevLett.127.157204
Publication status	Published - 8 Oct 2021

Bibliographical note

Funding Information:

We thank Bi Wen Hua for his help with x-ray diffraction experiments. I. Ž. acknowledges financial support by the Swiss National Science Foundation (SNSF) Projects No. 200021-169699 and 206021-189644. H. M. R. acknowledges financial support by SNFS Projects No. 200020-188648 and 206021-189644. Part of this work was supported by the Deutsche Forschungsgemeinschaft (DFG) through the SFB 1143 and the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter--ct: qmat (EXC 2147, Project No. 390858490), the Innovation Pool project MaDQuanT, as well as by the HLD at HZDR, a member of the European Magnetic Field Laboratory (EMFL). R. S. F. acknowledges financial support by FAPESP (Grant No. 2015/16191-5) and CNPq (Grant No. 429511/2018-3). J. R. acknowledges financial support by the German Research Foundation within the CRC183 (project A04). Y. I. acknowledges financial support by SERB, Department of Science and Technology (DST), India through grants SRG (No. SRG/2019/000056), MATRICS (No. MTR/2019/001042), and Indo-French Center for the Promotion of Advanced Research CEFIPRA (No. 64T3-1). This research was supported in part by the National Science Foundation under Grant No. NSF PHY-1748958, the ICTP through the Simons Associateship scheme, IIT Madras through the IoE program for establishing the QuCenDiEM group (Project No. SB20210813PHMHRD002720), and ICTS, Bengaluru, India during a visit for participating in the program “Novel phases of quantum matter” (Code: ICTS/topmatter2019/12). Y. I. acknowledges the use of the computing resources at HPCE, IIT Madras. The experiments were performed at the MUSR beamline [ISIS (1710223)] and the LTF and GPS beamlines [PSI (2017119 and 2017119)]. The neutron diffraction experiment was performed at WISH beamline [ISIS (2010010)]. The spin-polarized neutron diffraction and time-of-flight experiments were performed at DNS beamline [MLZ (13656)].

Publisher Copyright:
© 2021 American Physical Society

ASJC Scopus subject areas

General Physics and Astronomy

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10.1103/PhysRevLett.127.157204

ŽivkovićI2021MagneticAccepted author manuscript, 2.27 MBLicence: None: All rights reserved

Cite this

Živković, I., Favre, V., Mejia, C. S., Jeschke, H. O., Magrez, A., Dabholkar, B., Noculak, V., Freitas, R. S., Jeong, M., Hegde, N. G., Testa, L., Babkevich, P., Su, Y., Manuel, P., Luetkens, H., Baines, C., Baker, P. J., Wosnitza, J., Zaharko, O., ... Rønnow, H. M. (2021). Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K₂Ni₂(SO₄)₃. Physical Review Letters, 127(15), Article 157204. https://doi.org/10.1103/PhysRevLett.127.157204

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title = "Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K2Ni2(SO4)3",

abstract = "Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K2Ni2(SO4)3 forming a three-dimensional network of Ni2+ spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B≳4T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.",

author = "Ivica {\v Z}ivkovi{\'c} and Virgile Favre and Mejia, {Catalina Salazar} and Jeschke, {Harald O.} and Arnaud Magrez and Bhupen Dabholkar and Vincent Noculak and Freitas, {Rafael S.} and Minki Jeong and Hegde, {Nagabhushan G.} and Luc Testa and Peter Babkevich and Yixi Su and Pascal Manuel and Hubertus Luetkens and Christopher Baines and Baker, {Peter J.} and Jochen Wosnitza and Oksana Zaharko and Yasir Iqbal and Johannes Reuther and R{\o}nnow, {Henrik M.}",

note = "Funding Information: We thank Bi Wen Hua for his help with x-ray diffraction experiments. I. {\v Z}. acknowledges financial support by the Swiss National Science Foundation (SNSF) Projects No. 200021-169699 and 206021-189644. H. M. R. acknowledges financial support by SNFS Projects No. 200020-188648 and 206021-189644. Part of this work was supported by the Deutsche Forschungsgemeinschaft (DFG) through the SFB 1143 and the W{\"u}rzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter--ct: qmat (EXC 2147, Project No. 390858490), the Innovation Pool project MaDQuanT, as well as by the HLD at HZDR, a member of the European Magnetic Field Laboratory (EMFL). R. S. F. acknowledges financial support by FAPESP (Grant No. 2015/16191-5) and CNPq (Grant No. 429511/2018-3). J. R. acknowledges financial support by the German Research Foundation within the CRC183 (project A04). Y. I. acknowledges financial support by SERB, Department of Science and Technology (DST), India through grants SRG (No. SRG/2019/000056), MATRICS (No. MTR/2019/001042), and Indo-French Center for the Promotion of Advanced Research CEFIPRA (No. 64T3-1). This research was supported in part by the National Science Foundation under Grant No. NSF PHY-1748958, the ICTP through the Simons Associateship scheme, IIT Madras through the IoE program for establishing the QuCenDiEM group (Project No. SB20210813PHMHRD002720), and ICTS, Bengaluru, India during a visit for participating in the program “Novel phases of quantum matter” (Code: ICTS/topmatter2019/12). Y. I. acknowledges the use of the computing resources at HPCE, IIT Madras. The experiments were performed at the MUSR beamline [ISIS (1710223)] and the LTF and GPS beamlines [PSI (2017119 and 2017119)]. The neutron diffraction experiment was performed at WISH beamline [ISIS (2010010)]. The spin-polarized neutron diffraction and time-of-flight experiments were performed at DNS beamline [MLZ (13656)]. Publisher Copyright: {\textcopyright} 2021 American Physical Society",

year = "2021",

month = oct,

day = "8",

doi = "10.1103/PhysRevLett.127.157204",

language = "English",

volume = "127",

journal = "Physical Review Letters",

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Živković, I, Favre, V, Mejia, CS, Jeschke, HO, Magrez, A, Dabholkar, B, Noculak, V, Freitas, RS, Jeong, M, Hegde, NG, Testa, L, Babkevich, P, Su, Y, Manuel, P, Luetkens, H, Baines, C, Baker, PJ, Wosnitza, J, Zaharko, O, Iqbal, Y, Reuther, J & Rønnow, HM 2021, 'Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K₂Ni₂(SO₄)₃', Physical Review Letters, vol. 127, no. 15, 157204. https://doi.org/10.1103/PhysRevLett.127.157204

TY - JOUR

T1 - Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K2Ni2(SO4)3

AU - Živković, Ivica

AU - Favre, Virgile

AU - Mejia, Catalina Salazar

AU - Jeschke, Harald O.

AU - Magrez, Arnaud

AU - Dabholkar, Bhupen

AU - Noculak, Vincent

AU - Freitas, Rafael S.

AU - Jeong, Minki

AU - Hegde, Nagabhushan G.

AU - Testa, Luc

AU - Babkevich, Peter

AU - Su, Yixi

AU - Manuel, Pascal

AU - Luetkens, Hubertus

AU - Baines, Christopher

AU - Baker, Peter J.

AU - Wosnitza, Jochen

AU - Zaharko, Oksana

AU - Iqbal, Yasir

AU - Reuther, Johannes

AU - Rønnow, Henrik M.

N1 - Funding Information: We thank Bi Wen Hua for his help with x-ray diffraction experiments. I. Ž. acknowledges financial support by the Swiss National Science Foundation (SNSF) Projects No. 200021-169699 and 206021-189644. H. M. R. acknowledges financial support by SNFS Projects No. 200020-188648 and 206021-189644. Part of this work was supported by the Deutsche Forschungsgemeinschaft (DFG) through the SFB 1143 and the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter--ct: qmat (EXC 2147, Project No. 390858490), the Innovation Pool project MaDQuanT, as well as by the HLD at HZDR, a member of the European Magnetic Field Laboratory (EMFL). R. S. F. acknowledges financial support by FAPESP (Grant No. 2015/16191-5) and CNPq (Grant No. 429511/2018-3). J. R. acknowledges financial support by the German Research Foundation within the CRC183 (project A04). Y. I. acknowledges financial support by SERB, Department of Science and Technology (DST), India through grants SRG (No. SRG/2019/000056), MATRICS (No. MTR/2019/001042), and Indo-French Center for the Promotion of Advanced Research CEFIPRA (No. 64T3-1). This research was supported in part by the National Science Foundation under Grant No. NSF PHY-1748958, the ICTP through the Simons Associateship scheme, IIT Madras through the IoE program for establishing the QuCenDiEM group (Project No. SB20210813PHMHRD002720), and ICTS, Bengaluru, India during a visit for participating in the program “Novel phases of quantum matter” (Code: ICTS/topmatter2019/12). Y. I. acknowledges the use of the computing resources at HPCE, IIT Madras. The experiments were performed at the MUSR beamline [ISIS (1710223)] and the LTF and GPS beamlines [PSI (2017119 and 2017119)]. The neutron diffraction experiment was performed at WISH beamline [ISIS (2010010)]. The spin-polarized neutron diffraction and time-of-flight experiments were performed at DNS beamline [MLZ (13656)]. Publisher Copyright: © 2021 American Physical Society

PY - 2021/10/8

Y1 - 2021/10/8

N2 - Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K2Ni2(SO4)3 forming a three-dimensional network of Ni2+ spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B≳4T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.

AB - Quantum spin liquids are exotic states of matter that form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K2Ni2(SO4)3 forming a three-dimensional network of Ni2+ spins. Using density functional theory calculations, we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering, and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B≳4T diminishes the ordered component and drives the system into a pure quantum spin liquid state. This shows that a system of interconnected S=1 trillium lattices exhibits a significantly elevated level of geometrical frustration.

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DO - 10.1103/PhysRevLett.127.157204

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JO - Physical Review Letters

JF - Physical Review Letters

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