Abstract

Ce1−xPrxOBiS2 (0. 1 ≤ x ≤ 0.9) single crystals were grown using a CsCl flux method. Their structural and physical properties were examined by X-ray diffraction, X-ray absorption, transmission electron microscopy, and electrical resistivity. All of the Ce1−xPrxOBiS2 single crystals with 0.1 ≤ x ≤ 0.9 exhibited tetragonal phase. With increasing Pr content, the a-axis and c-axis lattice parameters decreased and increased, respectively. Transmission electron microscope analysis of Ce0.1Pr0.9OBiS2 (x = 0.9) single crystal showed no stacking faults. Atomic-resolution energy dispersive X-ray spectrometry mapping revealed that Bi, Ce/Pr, O, and S occupied different crystallographic sites, while Ce and Pr randomly occupied the same sites. X-ray absorption spectra showed that an increase of the Pr ratio increased the ratio of Ce4+/Ce3+. All of the Ce1−xPrxOBiS2 crystals showed superconducting transition, with a maximum transition temperature of ~4 K at x = 0.9.

Highlights

  • Flux synthesis has been utilized widely for the synthesis of solid-state materials (Oishi et al, 2004; Akira et al, 2019), especially for discovering compounds with complex structures (DiSalvo and Clarke, 1996; Bugaris and zur Loye, 2012) an interesting feature of synthesis using a flux, in addition to structural determination, is to explore various properties (Yamane et al, 1997; Mizuno et al, 2014; Miura et al, 2016; Chiang et al, 2018)

  • The valence state of the Cerium and Praseodymium component in the obtained single crystals was estimated by X-ray absorption fine spectroscopy (XAFS) analysis of Ce-L3 and PrL3 edges using an Aichi XAS beamline with a synchrotron Xray radiation (BL11S2: Experimental No.201801025)

  • Qualitative analysis by energy dispersive X-ray spectrometry (EDS) showed that the estimated atomic ratios of Bi and S elements in the single crystals were almost stoichiometric, with Bi:S = 1.01 ± 0.06

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Summary

INTRODUCTION

Flux synthesis has been utilized widely for the synthesis of solid-state materials (Oishi et al, 2004; Akira et al, 2019), especially for discovering compounds with complex structures (DiSalvo and Clarke, 1996; Bugaris and zur Loye, 2012) an interesting feature of synthesis using a flux, in addition to structural determination, is to explore various properties (Yamane et al, 1997; Mizuno et al, 2014; Miura et al, 2016; Chiang et al, 2018). The crystals with high Pr contents showed superconducting properties with a maximum transition temperature of ∼4 K, which could not be observed in powder samples synthesized without using the flux (Miura et al, 2018). The valence state of the Cerium and Praseodymium component in the obtained single crystals was estimated by X-ray absorption fine spectroscopy (XAFS) analysis of Ce-L3 and PrL3 edges using an Aichi XAS beamline with a synchrotron Xray radiation (BL11S2: Experimental No.201801025). The ρ–T characteristics of Ce0.1Pr0.9OBiS2 (x = 0.9) single crystal under a magnetic field (H) parallel to the c-plane with range of 0.1–9.0 T and the c-axis with range of 0.1–0.3 T were measured in the temperature range of 2.0–10.0 K. We measured the angular (θ ) dependence of resistivity (ρ) in the flux liquid state under various magnetic fields (H) and calculated superconducting anisotropy (γ s) using the effective mass model (Blatter et al, 1992; Iwasaki et al, 1995)

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