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Synthesis and transport properties of van der Waals-type quasi-two-dimensional pnictide, EuSn2As2 (本文)

坂上, 良介 慶應義塾大学

2021.09.21

概要

Quasi-two-dimensional pnictides are layered compounds that exhibit various functional properties including high thermoelectricity, superconductivity, and topological features. The present study aims application of van der Waals-type quasi-two-dimensional pnictide, EuSn2As2 to thermoelectric (TE) materials to reveal its transport properties. Furthermore, the present study examines its chemical bonding states by Mo¨ssbauer spectroscopy, magneti- zation measurements, and electrinic state calculations to discuss relations between chemical bonding states and transport properties.

In order to obtain near-single-phase polycrystalline samples of SnAs-based layered com- pound EuSn2As2 as a candidate for TE materials, we have established a method of synthesis procedure in which a sample was prepared from Eu ingot and Sn-As pellet in a carbon cru- cible. As far as our trials were concerned, this synthesis method produced polycrystalline samples free from second phases other than Sn, unlike another syntehsis method in which a sample was prepared from Eu ingot, Sn powder, and As powder in alumina tube. In the method using carbon crucible, 0.8050 g of the 0.9812 g of raw material was recovered. Sev- eral trial of this synthesis method will yield an adequate amounts of samples of EuSn2As2 for TE transport measurements.

Automation of measurements were necessary for experimental competitive development research of the TE materials and superconductors. Automated measurements in our labo- ratory of electrical resistivity (ρ) above and below room temperature (RT), Seebeck coeffi-cient (S ) above RT, and steady-state thermal conductivity (SSκ) at RT were realized using the Laboratory Virtual Instrument Engineering Workbench (LabVIEW) programs for controlling electronic test equipments and temperature controllers. Obtained measurement raw data were processed using Python code to obtain physical quantities. Particularly, we established calcu-lation processes for obtaining SSκ considering loss of thermal radiation. The above-mentioned work will achieve reduction in working hours and also will prevent careless mistakes.

The electrical and thermal transport properties of densified polycrystalline sample of EuSn2As2 with porosity (ϕ) of 2.4(9) vol.% were measured from RT to ∼673 K perpendicu- lar to the pressing direction of hot pressing; i.e. the crystallographic phase of EuSn2As2 in the sample was weakly oriented to the a-b plane of the hexagonal coordinate system during our measurements.
The plot of temperature (T ) dependence of the electrical resistivity (ρ) shows metallic be-havior. The ρ is probably affected by the multiband. The ρ includes T 2 term. The T 2 term is probably derived from spectral conductivity (sc) as a function of energy (ε) relative to the band edge, electron–electron scattering, ionized impurity scattering related to the displace- ment of participating elements, and/or intervalley scattering. The plot of T dependence of the Seebeck coefficient (S ) shows that the carriers exhibit p-type polarity. The measurement values of (ρ, S ) was (0.50(3) mΩ cm, 50(4) µV K−1) at T ∼ 673 K. The power factor (P) was 0.51(8) mW m−1 K−2 at 673(4) K. The direct thermal transport measurement reveals that the thermal conductivity (κ) decreases with increasing T . Using the WFL law, the ratio of phonon thermal conductivity (κph) to κ, defined as κph/κ, was 0.56(8) at T = 374(4) K and 0.35(7) at 673(6) K. The ZT value was 0.067(8) at T = 673(3) K. EuSn2As2 seems to be over-doped as a TE material. Suppression of the hole concentration will be a possible route for improving the TE properties of EuSn2As2-based compounds.

Magnetization measurements and Mo¨ssbauer spectroscopy for EuSn2As2 were demon- strated for experimental examination of chemical bonding states and further discussion on the chemical bonding and transport properties. 151Eu Mo¨ssbauer spectra indicate both Eu2+ and Eu3+ components at temperatures from 4.2 to 297 K. This was consistent with measure- ment values of magnetization of EuSn2As2 in high magnetic field. The Eu2+ component shows magnetic splitting at 4.2 K. 119Sn Mo¨ssbauer spectra at 4.2 K also demonstrate mag- netic splitting caused by internal magnetic field (Bint) of Eu. In EuSn2As2, Eu atoms are not isolated as cations but rather supply charge carriers to SnAs anionic bilayers. Although this model are not emphasized in previous reports on EuSn2As2, it will be useful for optimization of charge carrier density in EuSn2As2-based materials with high thermoelectric properties by means of partial substitution of the Eu atom for other lanthanides.

Electronic state calculations based on density functional theory (DFT) examines applica-tion of EuSn2As2 to the Zintl–Klemm concept. The spatial distribution of the charge density difference (CDD; ∆σch) of EuSn2As2 suggested the possible existence of the lone-pair elec- trons near the both Sn and As sites. The chemical bonding states of EuSn2As2 is partly explainable in terms of the Zintl–Klemm concept.

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