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Title: Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La1-xCaxMnO3

Abstract

Evolution of the average and local crystal structure of Ca-doped LaMnO3 has been studied across the metal to insulator (MI) and the orthorhombic to rhombohedral (OR) structural phase transitions over a broad temperature range for two Ca concentrations (x=0.18,0.22). Combined Rietveld and high real space resolution atomic pair distribution function (PDF) analysis of neutron total scattering data was carried out with aims of exploring the possibility of nanoscale phase separation (PS) in relation to MI transition, and charting the evolution of local Jahn-Teller (JT) distortion of MnO6 octahedra across the OR transition at TS~720 K. The study utilized explicit two-phase PDF structural modeling, revealing that away from TMI there is no evidence for nanoscale phase coexistence. The local JT distortions disappear abruptly upon crossing into the metallic regime both with doping and temperature, with only a small temperature-independent signature of quenched disorder being observable at low temperature as compared to CaMnO3. The results hence do not support the percolative scenario for the MI transition in La1₋xCaxMnO3 based on PS, and question its ubiquity in the manganites. In contrast to LaMnO3 that exhibits long-range orbital correlations and sizable octahedral distortions at low temperature, the doped samples with compositions straddling the MImore » boundary exhibit correlations (in the insulating regime) limited to only ~1 nm with observably smaller distortions. In the x=0.22 sample local JT distortions are found to persist across the OR transition and deep into the R phase (up to ~1050 K), where they are crystallographically prohibited. Lastly, their magnitude and subnanometer spatial extent remain unchanged.« less

Authors:
 [1];  [2];  [3];  [4]
+ Show Author Affiliations
  1. The Hashemite Univ., Zarqa (Jordan)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1253277
Alternate Identifier(s):
OSTI ID: 1249704; OSTI ID: 1302996; OSTI ID: 1339525
Report Number(s):
BNL-112098-2016-JA; BNL-112395-2016-JA
Journal ID: ISSN 2469-9950; PRBMDO; R&D Project: PO011; PM032; KC0201060; KC0202010
Grant/Contract Number:  
SC00112704; AC52-06NA25396; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; Journal Issue: 16; 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; 36 MATERIALS SCIENCE

Citation Formats

Shatnawi, Mouath, Bozin, Emil S., Mitchell, J. F., and Billinge, Simon J. L. Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La1-xCaxMnO3. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.93.165138.
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Shatnawi, Mouath, Bozin, Emil S., Mitchell, J. F., & Billinge, Simon J. L. Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La1-xCaxMnO3. United States. https://doi.org/10.1103/PhysRevB.93.165138
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Shatnawi, Mouath, Bozin, Emil S., Mitchell, J. F., and Billinge, Simon J. L. Mon . "Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La1-xCaxMnO3". United States. https://doi.org/10.1103/PhysRevB.93.165138. https://www.osti.gov/servlets/purl/1253277.
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@article{osti_1253277,
title = {Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La1-xCaxMnO3},
author = {Shatnawi, Mouath and Bozin, Emil S. and Mitchell, J. F. and Billinge, Simon J. L.},
abstractNote = {Evolution of the average and local crystal structure of Ca-doped LaMnO3 has been studied across the metal to insulator (MI) and the orthorhombic to rhombohedral (OR) structural phase transitions over a broad temperature range for two Ca concentrations (x=0.18,0.22). Combined Rietveld and high real space resolution atomic pair distribution function (PDF) analysis of neutron total scattering data was carried out with aims of exploring the possibility of nanoscale phase separation (PS) in relation to MI transition, and charting the evolution of local Jahn-Teller (JT) distortion of MnO6 octahedra across the OR transition at TS~720 K. The study utilized explicit two-phase PDF structural modeling, revealing that away from TMI there is no evidence for nanoscale phase coexistence. The local JT distortions disappear abruptly upon crossing into the metallic regime both with doping and temperature, with only a small temperature-independent signature of quenched disorder being observable at low temperature as compared to CaMnO3. The results hence do not support the percolative scenario for the MI transition in La1₋xCaxMnO3 based on PS, and question its ubiquity in the manganites. In contrast to LaMnO3 that exhibits long-range orbital correlations and sizable octahedral distortions at low temperature, the doped samples with compositions straddling the MI boundary exhibit correlations (in the insulating regime) limited to only ~1 nm with observably smaller distortions. In the x=0.22 sample local JT distortions are found to persist across the OR transition and deep into the R phase (up to ~1050 K), where they are crystallographically prohibited. Lastly, their magnitude and subnanometer spatial extent remain unchanged.},
doi = {10.1103/PhysRevB.93.165138},
journal = {Physical Review B},
number = 16,
volume = 93,
place = {United States},
year = {Mon Apr 25 00:00:00 EDT 2016},
month = {Mon Apr 25 00:00:00 EDT 2016}
}
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https://doi.org/10.1103/PhysRevB.93.165138
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