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

Shatnawi, Mouath; Bozin, Emil S.; Mitchell, J. F.; Billinge, Simon J. L.

doi:10.1103/PhysRevB.93.165138

Title: Non percolative nature of the metal-insulator transition and persistence of local Jahn-Teller distortions in the rhombohedral regime of La_1-xCa_xMnO₃

Journal Article · Mon Apr 25 00:00:00 EDT 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.93.165138· OSTI ID:1253277

Shatnawi, Mouath ^[1]; Bozin, Emil S. ^[2]; Mitchell, J. F. ^[3]; Billinge, Simon J. L. ^[4]

The Hashemite Univ., Zarqa (Jordan)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)

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 T_S~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 La_1₋xCa_xMnO₃ 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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704; AC52-06NA25396; AC02-06CH11357

OSTI ID:: 1253277

Alternate ID(s):: OSTI ID: 1249704; OSTI ID: 1302996; OSTI ID: 1339525

Report Number(s):: BNL-112098-2016-JA; BNL-112395-2016-JA; PRBMDO; R&D Project: PO011; PM032; KC0201060; KC0202010

Journal Information:: Physical Review B, Vol. 93, Issue 16; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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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

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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 La_1-xCa_xMnO₃