Electrical transport, magnetic, and thermodynamic properties of La-, Pr-, and Nd-doped BaSnO3-δ single crystals

McCalla, Eric; Phelan, Daniel; Krogstad, Matthew J.; Dabrowski, Bogdan; Leighton, Chris

doi:10.1103/PhysRevMaterials.2.084601

Title: Electrical transport, magnetic, and thermodynamic properties of La-, Pr-, and Nd-doped $BaSn O_{3 - δ}$ single crystals

Journal Article · Fri Aug 03 00:00:00 EDT 2018 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.2.084601· OSTI ID:1466372

McCalla, Eric ^[1]; Phelan, Daniel ^[2]; Krogstad, Matthew J. ^[3]; Dabrowski, Bogdan ^[4]; Leighton, Chris ^[5]

Univ. of Minnesota, Minneapolis, MN (United States); McGill Univ., Montreal, QC (Canada)
Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)
Northern Illinois Univ., DeKalb, IL (United States)
Univ. of Minnesota, Minneapolis, MN (United States)

Due to outstanding room temperature electron mobility, the wide-gap perovskite semiconductor BaSnO₃ is of high current interest. Although n doping with Sb and O vacancies has been reported, most work has focused solely on La doping. Here we report bulk single crystals of Ba_1–xR_xSnO_3–δ with R = La,Pr, and Nd, as well as unintentionally doped BaSnO_3–δ, thus exploring new rare earth (magnetic) dopants in addition to O vacancy doping. Consistent with recent results on epitaxial films, O vacancies are shown capable of generating mid-10¹⁹cm^–3 Hall electron densities, with single crystal mobilities ~100–150cm²V^–1s^–1. Despite apparent solubility limits below ~0.5at.%, Pr and Nd are also shown to be effective n dopants, yielding Hall electron densities >1 × 10²⁰ cm^–3, and ambient and low temperature mobilities up to 175 and 430 cm² V^–1s^–1, respectively. In contrast to the La-doped case, clear paramagnetism occurs with Pr and Nd doping, allowing for direct estimates of dopant concentrations for quantitative comparison with Hall densities. We show that dopant and Hall densities can be approximately reconciled, but only after accounting for O vacancy doping. Specific heat measurements were also performed, confirming the BaSnO₃ Debye temperature, and revealing electronic contributions roughly consistent with reported effective masses. Interestingly, and likely related to crystalline electric field effects, Pr-doped BaSnO₃ exhibits large deviations from simple Curie-Weiss susceptibility, and a pronounced Schottky anomaly, which we analyze in detail. Furthermore, these results provide significant insight into doping in BaSnO₃, establishing new rare earth magnetic dopants, clarifying the role of O vacancies, and determining dopant concentrations and solubility limits.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; FG02-06ER46275; SC0016371

OSTI ID:: 1466372

Alternate ID(s):: OSTI ID: 1462786

Journal Information:: Physical Review Materials, Vol. 2, Issue 8; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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