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Zusammenfassung:
High-quality single crystals of MnBi 2 Te 4 are grown for the first time by slow cooling within a narrow range between the melting points of Bi 2 Te 3 (586 °C) and MnBi 2 Te 4 (600 °C). Single-crystal X-ray diffraction and electron microscopy reveal ubiquitous antisite defects in both cation sites and, possibly, Mn vacancies (Mn 0.85(3) Bi 2.10(3) Te 4 ). Thermochemical studies complemented with high-temperature X-ray diffraction establish a limited high-temperature range of phase stability and metastability at room temperature. Nevertheless, the synthesis of MnBi 2 Te 4 can be scaled-up as powders can be obtained at subsolidus temperatures and quenched at room temperature. Bulk samples exhibit long-range antiferromagnetic ordering below 24 K. The Mn(II) out-of-plane magnetic state is confirmed by the magnetization, X-ray photoemission, X-ray absorption, and linear dichroism measurements. The compound shows a metallic type of resistivity in the range 4.5-300 K and is an n-type conductor that reaches a thermoelectric figure of merit up to ZT = 0.17. Angle-resolved photoemission experiments show a surface state forming a gapped Dirac cone, thus strengthening MnBi 2 Te 4 as a promising candidate for the intrinsic magnetic topological insulator, in accordance with theoretical predictions. The developed synthetic protocols enable further experimental studies of a crossover between magnetic ordering and nontrivial topology in bulk MnBi 2 Te 4 . © 2019 American Chemical Society.
