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Inorganic halide double perovskites with optoelectronic properties modulated by sublattice mixing
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-02-24 , DOI: 10.1021/jacs.9b12440
Christopher J Bartel 1 , Jacob M Clary 1 , Christopher Sutton 2 , Derek Vigil-Fowler 3 , Bryan R Goldsmith 4 , Aaron M Holder 1, 3 , Charles B Musgrave 1, 3, 5, 6, 7
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-02-24 , DOI: 10.1021/jacs.9b12440
Christopher J Bartel 1 , Jacob M Clary 1 , Christopher Sutton 2 , Derek Vigil-Fowler 3 , Bryan R Goldsmith 4 , Aaron M Holder 1, 3 , Charles B Musgrave 1, 3, 5, 6, 7
Affiliation
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All-inorganic halide double perovskites have emerged as a promising class of materials that are potentially more stable and less toxic than lead-containing hybrid organic-inorganic perovskite optoelectronic materials. In this work, 311 cesium chloride double perovskites (Cs2BB'Cl6) were selected from a set of 903 compounds as likely being stable based on a statistically learned tolerance factor (τ) for perovskite stability. First-principles calculations on these 311 double perovskites were then performed to assess their stability and identify candidates with band gaps appropriate for optoelectronic applications. We predict that 261 of the 311 Cs2BB'Cl6 compounds are likely synthesizable based on a thermodynamic analysis of their decomposition to competing compounds (decomposition enthalpy < 0.05 eV/atom). Of these 261 likely synthesizable compounds, 47 contain no toxic elements and have direct or nearly direct (within 100 meV) band gaps between 1 and 3 eV as computed with hybrid density functional theory (HSE06). Within this set, we identify the triple alkali perovskites Cs2[Alk]+[TM]3+Cl6, where Alk is a group 1 alkali cation and TM is a transition metal cation, as a class of Cs2BB'Cl6 double perovskites with remarkable optical properties, including large and tunable exciton binding energies as computed by the GW-Bethe Salpeter Equation (GW-BSE) method. We attribute the unusual electronic structure of these compounds to the mixing of the Alk-Cl and TM-Cl sublattices, leading to materials with small band gaps, large exciton binding energies, and absorption spectra that are strongly influenced by the identity of the transition metal. The role of the double perovskite structure in enabling these unique properties is probed through analysis of the electronic structures and chemical bonding of these compounds as compared with other transition metal and alkali transition metal halides.
中文翻译：
通过亚晶格混合调制具有光电特性的无机卤化物双钙钛矿
全无机卤化物双钙钛矿已成为一类有前途的材料，与含铅杂化有机-无机钙钛矿光电材料相比，它们可能更稳定且毒性更小。在这项工作中，基于钙钛矿稳定性的统计学习耐受因子 (τ)，从一组 903 种化合物中选择了 311 种氯化铯双钙钛矿 (Cs2BB'Cl6)，它们可能是稳定的。然后对这 311 个双钙钛矿进行第一性原理计算，以评估它们的稳定性并确定具有适合光电应用的带隙的候选物。我们预测 311 种 Cs2BB'Cl6 化合物中的 261 种可能是可合成的，这是基于对它们分解为竞争化合物的热力学分析（分解焓 < 0.05 eV/原子）。在这 261 种可能合成的化合物中，有 47 种不含有毒元素，并且根据混合密度泛函理论 (HSE06) 计算，带隙在 1 到 3 eV 之间直接或接近直接（在 100 meV 内）。在这组中，我们确定了三重碱钙钛矿 Cs2[Alk]+[TM]3+Cl6，其中 Alk 是第 1 族碱金属阳离子，TM 是过渡金属阳离子，是一类具有显着光学性能的 Cs2BB'Cl6 双钙钛矿属性，包括由 GW-Bethe Salpeter 方程 (GW-BSE) 方法计算的大且可调谐的激子结合能。我们将这些化合物的不寻常电子结构归因于 Alk-Cl 和 TM-Cl 亚晶格的混合，导致材料具有小带隙、大激子结合能和受过渡金属特性强烈影响的吸收光谱.
更新日期：2020-02-24
中文翻译：
通过亚晶格混合调制具有光电特性的无机卤化物双钙钛矿
全无机卤化物双钙钛矿已成为一类有前途的材料，与含铅杂化有机-无机钙钛矿光电材料相比，它们可能更稳定且毒性更小。在这项工作中，基于钙钛矿稳定性的统计学习耐受因子 (τ)，从一组 903 种化合物中选择了 311 种氯化铯双钙钛矿 (Cs2BB'Cl6)，它们可能是稳定的。然后对这 311 个双钙钛矿进行第一性原理计算，以评估它们的稳定性并确定具有适合光电应用的带隙的候选物。我们预测 311 种 Cs2BB'Cl6 化合物中的 261 种可能是可合成的，这是基于对它们分解为竞争化合物的热力学分析（分解焓 < 0.05 eV/原子）。在这 261 种可能合成的化合物中，有 47 种不含有毒元素，并且根据混合密度泛函理论 (HSE06) 计算，带隙在 1 到 3 eV 之间直接或接近直接（在 100 meV 内）。在这组中，我们确定了三重碱钙钛矿 Cs2[Alk]+[TM]3+Cl6，其中 Alk 是第 1 族碱金属阳离子，TM 是过渡金属阳离子，是一类具有显着光学性能的 Cs2BB'Cl6 双钙钛矿属性，包括由 GW-Bethe Salpeter 方程 (GW-BSE) 方法计算的大且可调谐的激子结合能。我们将这些化合物的不寻常电子结构归因于 Alk-Cl 和 TM-Cl 亚晶格的混合，导致材料具有小带隙、大激子结合能和受过渡金属特性强烈影响的吸收光谱.
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