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Title: Pressure-Induced Collapse of Magnetic Order in Jarosite

Abstract

We report a pressure-induced phase transition in the frustrated kagomé material jarosite at ~45 GPa , which leads to the disappearance of magnetic order. Using a suite of experimental techniques, we characterize the structural, electronic, and magnetic changes in jarosite through this phase transition. Synchrotron powder x-ray diffraction and Fourier transform infrared spectroscopy experiments, analyzed in aggregate with the results from density functional theory calculations, indicate that the material changes from a R 3 ¯ m structure to a structure with a R 3 ¯ c space group. The resulting phase features a rare twisted kagomé lattice in which the integrity of the equilateral Fe 3 + triangles persists. Based on symmetry arguments we hypothesize that the resulting structural changes alter the magnetic interactions to favor a possible quantum paramagnetic phase at high pressure.

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [4];  [5];  [6];  [1];  [6];  [6];  [4];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]
  1. Northwestern University, Evanston, IL (United States)
  2. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
  3. University of Illinois, Chicago, IL (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. University of Alabama, Birmingham, AL (United States)
  6. Argonne National Laboratory (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
University of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1650655
Alternate Identifier(s):
OSTI ID: 1660736; OSTI ID: 1662035
Report Number(s):
LLNL-JRNL-807945
Journal ID: ISSN 0031-9007; TRN: US2203040
Grant/Contract Number:  
NA0003975; AC52-07NA27344; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 125; Journal Issue: 7; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Density of states; Exotic phases of matter; Frustrated magnetism; Magnetic anisotropy; Magnetic coupling; Magnetic interactions; Magnetic order; Magnetic phase transitions; Magnetic susceptibility; Magnetism; Phase transitions; Quantum phase transitions; Spin liquid

Citation Formats

Klein, Ryan  A., Walsh, James P. S., Clarke, Samantha  M., Liu, Zhenxian, Alp, E. Ercan, Bi, Wenli, Meng, Yue, Altman, Alison  B., Chow, Paul, Xiao, Yuming, Norman, M. R., Rondinelli, James  M., Jacobsen, Steven  D., Puggioni, Danilo, and Freedman, Danna E. Pressure-Induced Collapse of Magnetic Order in Jarosite. United States: N. p., 2020. Web. doi:10.1103/physrevlett.125.077202.
Klein, Ryan  A., Walsh, James P. S., Clarke, Samantha  M., Liu, Zhenxian, Alp, E. Ercan, Bi, Wenli, Meng, Yue, Altman, Alison  B., Chow, Paul, Xiao, Yuming, Norman, M. R., Rondinelli, James  M., Jacobsen, Steven  D., Puggioni, Danilo, & Freedman, Danna E. Pressure-Induced Collapse of Magnetic Order in Jarosite. United States. https://doi.org/10.1103/physrevlett.125.077202
Klein, Ryan  A., Walsh, James P. S., Clarke, Samantha  M., Liu, Zhenxian, Alp, E. Ercan, Bi, Wenli, Meng, Yue, Altman, Alison  B., Chow, Paul, Xiao, Yuming, Norman, M. R., Rondinelli, James  M., Jacobsen, Steven  D., Puggioni, Danilo, and Freedman, Danna E. Thu . "Pressure-Induced Collapse of Magnetic Order in Jarosite". United States. https://doi.org/10.1103/physrevlett.125.077202. https://www.osti.gov/servlets/purl/1650655.
@article{osti_1650655,
title = {Pressure-Induced Collapse of Magnetic Order in Jarosite},
author = {Klein, Ryan  A. and Walsh, James P. S. and Clarke, Samantha  M. and Liu, Zhenxian and Alp, E. Ercan and Bi, Wenli and Meng, Yue and Altman, Alison  B. and Chow, Paul and Xiao, Yuming and Norman, M. R. and Rondinelli, James  M. and Jacobsen, Steven  D. and Puggioni, Danilo and Freedman, Danna E.},
abstractNote = {We report a pressure-induced phase transition in the frustrated kagomé material jarosite at ~45 GPa, which leads to the disappearance of magnetic order. Using a suite of experimental techniques, we characterize the structural, electronic, and magnetic changes in jarosite through this phase transition. Synchrotron powder x-ray diffraction and Fourier transform infrared spectroscopy experiments, analyzed in aggregate with the results from density functional theory calculations, indicate that the material changes from a R3¯m structure to a structure with a R3¯c space group. The resulting phase features a rare twisted kagomé lattice in which the integrity of the equilateral Fe3+ triangles persists. Based on symmetry arguments we hypothesize that the resulting structural changes alter the magnetic interactions to favor a possible quantum paramagnetic phase at high pressure.},
doi = {10.1103/physrevlett.125.077202},
journal = {Physical Review Letters},
number = 7,
volume = 125,
place = {United States},
year = {2020},
month = {8}
}

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