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Title: Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo 2F 7 and NaSrCo 2F 7 with magnetic pair distribution function analysis

Here, we present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo 2F 7 and NaSrCo 2F 7, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 Å, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [4] ;  [7]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
  3. Colorado State Univ., Fort Collins, CO (United States); Canadian Institute for Advanced Research, Toronto, ON (Canada)
  4. Princeton Univ., Princeton, NJ (United States)
  5. Institut Laue-Langevin, Grenoble (France); Rutherford Appleton Lab., Didcot (United Kingdom)
  6. Institut Laue-Langevin, Grenoble (France)
  7. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Report Number(s):
BNL-114814-2017-JA; BNL-114815-2017-JAAM
Journal ID: ISSN 2475-9953; R&D Project: PM032; KC0202010; TRN: US1800368
Grant/Contract Number:
SC0012704; FG02-08ER46544; AC02-05-CH11231; AC03-76SF008; SC00112704; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 7; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1412789
Alternate Identifier(s):
OSTI ID: 1416440; OSTI ID: 1425012; OSTI ID: 1466710

Frandsen, Benjamin A., Billinge, Simon J. L., Ross, Kathryn A., Krizan, Jason W., Nilsen, Goran J., Wildes, Andrew R., Cava, Robert J., and Birgeneau, Robert J.. Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo2F7 and NaSrCo2F7 with magnetic pair distribution function analysis. United States: N. p., Web. doi:10.1103/PhysRevMaterials.1.074412.
Frandsen, Benjamin A., Billinge, Simon J. L., Ross, Kathryn A., Krizan, Jason W., Nilsen, Goran J., Wildes, Andrew R., Cava, Robert J., & Birgeneau, Robert J.. Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo2F7 and NaSrCo2F7 with magnetic pair distribution function analysis. United States. doi:10.1103/PhysRevMaterials.1.074412.
Frandsen, Benjamin A., Billinge, Simon J. L., Ross, Kathryn A., Krizan, Jason W., Nilsen, Goran J., Wildes, Andrew R., Cava, Robert J., and Birgeneau, Robert J.. 2017. "Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo2F7 and NaSrCo2F7 with magnetic pair distribution function analysis". United States. doi:10.1103/PhysRevMaterials.1.074412.
@article{osti_1412789,
title = {Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo2F7 and NaSrCo2F7 with magnetic pair distribution function analysis},
author = {Frandsen, Benjamin A. and Billinge, Simon J. L. and Ross, Kathryn A. and Krizan, Jason W. and Nilsen, Goran J. and Wildes, Andrew R. and Cava, Robert J. and Birgeneau, Robert J.},
abstractNote = {Here, we present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo2F7 and NaSrCo2F7, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 Å, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.},
doi = {10.1103/PhysRevMaterials.1.074412},
journal = {Physical Review Materials},
number = 7,
volume = 1,
place = {United States},
year = {2017},
month = {12}
}