We present our results of the spin‐polarized calculations on the structural, magneto‐electronic, thermodynamic, and thermoelectric properties of vacancy‐ordered double perovskites A2OsX6 (A = Rb/Cs; X = Cl/Br). We utilized the Wu‐Cohen generalized gradient approximation (Wu‐GGA) and the mBJ scheme to determine a more reliable electronic structure. The compounds exhibit negative formation energy, suitable tolerance factor, and a stable phonon spectrum, indicating their stability. The compounds show half‐metallicity, acting as semiconductors with direct band gaps between 2 and 3 eV in the spin‐up orientation while metallic in the spin‐down. Each compound shows a total spin magnetic moment of 2.00 μB per formula unit, with Os‐t2g states contributing the most (~1.5 μB). The computed thermoelectric coefficient indicates the usability of these compounds across a wide temperature range (200–800 K) with high electrical conductivity and low electronic thermal conductivity. The compounds exhibit high Seebeck coefficient and figure of merit (ZT), making them suitable for thermoelectric applications. With ferromagnetic and half‐metallic characteristics, these compounds could be promising candidates for spintronics, thermoelectronic, and data storage applications.

中文翻译：

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用于自旋电子和热电应用的半金属变体钙钛矿 A2OsX6（A = Rb/Cs；X = Cl/Br）的 DFT 研究

我们展示了空位有序双钙钛矿 A 的结构、磁电子、热力学和热电性质的自旋极化计算结果2操作系统6（A = Rb/Cs；X = Cl/Br）。我们利用 Wu-Cohen 广义梯度近似（Wu-GGA）和 mBJ 方案来确定更可靠的电子结构。该化合物表现出负的形成能、合适的耐受因子和稳定的声子谱，表明它们的稳定性。这些化合物表现出半金属性，在自旋向上方向上充当直接带隙在 2 到 3 eV 之间的半导体，而在自旋向下方向上具有金属性。每个化合物的总自旋磁矩为每分子式单元 2.00 μB，Os-t2g 状态贡献最大（~1.5 μB）。计算出的热电系数表明这些化合物在较宽的温度范围（200-800 K）内具有高电导率和低电子热导率的可用性。这些化合物具有高塞贝克系数和品质因数 (ZT)，使其适合热电应用。这些化合物具有铁磁和半金属特性，可能成为自旋电子学、热电子学和数据存储应用的有希望的候选者。