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

Journal Article · · Physical Review B
 [1];  [2];  [3];  [4]
  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)
+ Show Author Affiliations
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. As a result, their magnitude and subnanometer spatial extent remain unchanged.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357; AC52-06NA25396
OSTI ID:
1253277
Alternate ID(s):
OSTI ID: 1302996
OSTI ID: 1339525
OSTI ID: 1249704
Report Number(s):
BNL--112098-2016-JA; BNL--112395-2016-JA; KC0201060; KC0202010
Journal Information:
Physical Review B, Journal Name: Physical Review B Journal Issue: 16 Vol. 93; ISSN 2469-9950; ISSN PRBMDO
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Jahn-Teller distortion effects on the transport properties of La 0.7 Ca 0.3 Mn 1−x Fe x O 3 perovskite NPs journal July 2019
Resonant inelastic x-ray scattering study of B i 6 F e 2 T i 3 O 18 ,   B i 6 FeCoT i 3 O 18 , and LaB i 5 FeCoT i 3 O 18 Aurivillius-phase oxides journal May 2017

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