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Title: Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S = 1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S = 1 quantum antiferromagnet]

Abstract

The magnetic ground state of the quasi-one-dimensional spin-1 antiferromagnetic chain is sensitive to the relative sizes of the single-ion anisotropy (D) and the intrachain (J) and interchain (J') exchange interactions. The ratios D/J and J' /J dictate the material's placement in one of three competing phases: a Haldane gapped phase, a quantum paramagnet, and an XY-ordered state, with a quantum critical point at their junction. We have identified [Ni(HF 2)(pyz) 2] SbF 6, where pyz = pyrazine, as a rare candidate in which this behavior can be explored in detail. Combining neutron scattering (elastic and inelastic) in applied magnetic fields of up to 10 tesla and magnetization measurements in fields of up to 60 tesla with numerical modeling of experimental observables, we are able to obtain accurate values of all of the parameters of the Hamiltonian [D = 13.3(1) K, J = 10.4(3) K, and J' = 1.4(2) K], despite the polycrystalline nature of the sample. Density-functional theory calculations result in similar couplings (J = 9.2 K, J' = 1.8 K) and predict that the majority of the total spin population resides on the Ni(II) ion, while the remaining spin density is delocalized over both ligand types. Finally, the generalmore » procedures outlined in this paper permit phase boundaries and quantum-critical points to be explored in anisotropic systems for which single crystals are as yet unavailable.« less

Authors:
 [1];  [2];  [1];  [3];  [4];  [5];  [6];  [7];  [8];  [8];  [8];  [9];  [10];  [10];  [9];  [9];  [11]
  1. Univ. of Warwick, Coventry (United Kingdom)
  2. Eastern Washington Univ., Cheney, WA (United States); National Institute of Standards and Technology, Gaithersburg, MD (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Oxford, Oxford (United Kingdom); STFC Rutherford Appleton Lab., Oxfordshire (United Kingdom)
  5. STFC Rutherford Appleton Lab., Oxfordshire (United Kingdom)
  6. Eastern Washington Univ., Cheney, WA (United States)
  7. National Institute of Standards and Technology, Gaithersburg, MD (United States)
  8. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  9. Argonne National Lab. (ANL), Argonne, IL (United States)
  10. Univ. of Bern, Bern (Switzerland)
  11. Univ. of Oxford, Oxford (United Kingdom); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1373946
Alternate Identifier(s):
OSTI ID: 1352461; OSTI ID: 1407877; OSTI ID: 1471948
Report Number(s):
LA-UR-16-28827
Journal ID: ISSN 2469-9950; PRBMDO; 131765; TRN: US1702673
Grant/Contract Number:  
AC02-06CH11357; AC52-06NA25396; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 13; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; High Magnetic Field Science

Citation Formats

Brambleby, Jamie, Manson, Jamie L., Goddard, Paul A., Stone, Matthew B., Johnson, Roger D., Manuel, Pascal, Villa, Jacqueline A., Brown, Craig M., Lu, Helen, Chikara, Shalinee, Zapf, Vivien, Lapidus, Saul H., Scatena, Rebecca, Macchi, Piero, Chen, Yu-sheng, Wu, Lai -Chin, and Singleton, John. Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S=1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S=1 quantum antiferromagnet]. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.95.134435.
Brambleby, Jamie, Manson, Jamie L., Goddard, Paul A., Stone, Matthew B., Johnson, Roger D., Manuel, Pascal, Villa, Jacqueline A., Brown, Craig M., Lu, Helen, Chikara, Shalinee, Zapf, Vivien, Lapidus, Saul H., Scatena, Rebecca, Macchi, Piero, Chen, Yu-sheng, Wu, Lai -Chin, & Singleton, John. Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S=1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S=1 quantum antiferromagnet]. United States. doi:10.1103/PhysRevB.95.134435.
Brambleby, Jamie, Manson, Jamie L., Goddard, Paul A., Stone, Matthew B., Johnson, Roger D., Manuel, Pascal, Villa, Jacqueline A., Brown, Craig M., Lu, Helen, Chikara, Shalinee, Zapf, Vivien, Lapidus, Saul H., Scatena, Rebecca, Macchi, Piero, Chen, Yu-sheng, Wu, Lai -Chin, and Singleton, John. Thu . "Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S=1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S=1 quantum antiferromagnet]". United States. doi:10.1103/PhysRevB.95.134435. https://www.osti.gov/servlets/purl/1373946.
@article{osti_1373946,
title = {Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S=1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S=1 quantum antiferromagnet]},
author = {Brambleby, Jamie and Manson, Jamie L. and Goddard, Paul A. and Stone, Matthew B. and Johnson, Roger D. and Manuel, Pascal and Villa, Jacqueline A. and Brown, Craig M. and Lu, Helen and Chikara, Shalinee and Zapf, Vivien and Lapidus, Saul H. and Scatena, Rebecca and Macchi, Piero and Chen, Yu-sheng and Wu, Lai -Chin and Singleton, John},
abstractNote = {The magnetic ground state of the quasi-one-dimensional spin-1 antiferromagnetic chain is sensitive to the relative sizes of the single-ion anisotropy (D) and the intrachain (J) and interchain (J') exchange interactions. The ratios D/J and J' /J dictate the material's placement in one of three competing phases: a Haldane gapped phase, a quantum paramagnet, and an XY-ordered state, with a quantum critical point at their junction. We have identified [Ni(HF2)(pyz)2] SbF6, where pyz = pyrazine, as a rare candidate in which this behavior can be explored in detail. Combining neutron scattering (elastic and inelastic) in applied magnetic fields of up to 10 tesla and magnetization measurements in fields of up to 60 tesla with numerical modeling of experimental observables, we are able to obtain accurate values of all of the parameters of the Hamiltonian [D = 13.3(1) K, J = 10.4(3) K, and J' = 1.4(2) K], despite the polycrystalline nature of the sample. Density-functional theory calculations result in similar couplings (J = 9.2 K, J' = 1.8 K) and predict that the majority of the total spin population resides on the Ni(II) ion, while the remaining spin density is delocalized over both ligand types. Finally, the general procedures outlined in this paper permit phase boundaries and quantum-critical points to be explored in anisotropic systems for which single crystals are as yet unavailable.},
doi = {10.1103/PhysRevB.95.134435},
journal = {Physical Review B},
number = 13,
volume = 95,
place = {United States},
year = {2017},
month = {4}
}

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    Works referencing / citing this record:

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    Giant Pressure Dependence and Dimensionality Switching in a Metal-Organic Quantum Antiferromagnet
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    Giant Pressure Dependence and Dimensionality Switching in a Metal-Organic Quantum Antiferromagnet
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