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Excitonic properties and solar harvesting performance of Cs2ZnY2X2 as quasi-2D mixed-halide perovskites
Journal of Alloys and Compounds ( IF 5.8 ) Pub Date : 2024-09-11 , DOI: 10.1016/j.jallcom.2024.176434
Danilo Neves Silveira , Alexandre C. Dias , Luis Octavio de Araujo , Marco A.A. Queiroz , Jônatas Favotto Dalmedico , Carlos Maciel de Oliveira Bastos , Celso R.C. Rêgo , Maurício J. Piotrowski , Diego Guedes-Sobrinho
Journal of Alloys and Compounds ( IF 5.8 ) Pub Date : 2024-09-11 , DOI: 10.1016/j.jallcom.2024.176434
Danilo Neves Silveira , Alexandre C. Dias , Luis Octavio de Araujo , Marco A.A. Queiroz , Jônatas Favotto Dalmedico , Carlos Maciel de Oliveira Bastos , Celso R.C. Rêgo , Maurício J. Piotrowski , Diego Guedes-Sobrinho
Due to their low toxicity and high-temperature stability, lead-free quasi-2D metal halide perovskites (MHPs) are promising materials for optoelectronic applications. However, understanding their structural and optoelectronic properties, especially excitonic effects (electron-hole pair, e -h ), is challenging due to their quantum well topology. We propose an efficient protocol for band gap correction of Cs2 ZnX (X = Cl4 , Br2 Cl2 , and I2 Cl2 ) and Cs2 PbI2 Cl2 (used as a benchmark) quasi-2D MHPs. This protocol is based on a relativistic quasiparticle approach (DFT-1/2) using density functional theory (DFT). We first examined the hybrid contributions of the halide alloys, leading to excitonic characterization using the Bethe–Salpeter equation within the maximally localized Wannier functions tight-binding method. This method provides a cost-effective approach for describing e -h quasiparticle effects. Additionally, we analyzed the crystal structure, thermodynamic stability, and optoelectronic properties of the newly synthesized Zn-based systems, focusing on their structural stability mechanisms. We found a correlation between the allocation of Cs+ cations in the crystal structure and the formation of two distinct stabilization patterns, influenced by the radii of the metal (Zn or Pb) and halide components. The relativistic correction of the band gap energies yielded results within 10 % of the experimental values. Furthermore, incorporating e -h quasiparticle effects for Cs2 PbI2 Cl2 resulted in an exciton binding energy of 0.160 eV, in excellent agreement with experimental data. This work represents a significant advance in the optoelectronic characterization of Cs2 ZnX systems, previously unexplored for their excitonic properties.
中文翻译:
准二维混合卤化物钙钛矿 Cs2ZnY2X2 的激子特性和太阳能收集性能
由于其低毒性和高温稳定性,无铅准二维金属卤化物钙钛矿(MHP)是用于光电应用的有前途的材料。然而,由于其量子阱拓扑结构,了解它们的结构和光电特性,特别是激子效应(电子空穴对,eh)具有挑战性。我们提出了一种有效的 Cs2ZnX(X = Cl4、Br2Cl2 和 I2Cl2)和 Cs2PbI2Cl2(用作基准)准二维 MHP 带隙校正协议。该协议基于使用密度泛函理论 (DFT) 的相对论准粒子方法 (DFT-1/2)。我们首先研究了卤化物合金的混合贡献,从而在最大局域 Wannier 函数紧束缚方法中使用 Bethe-Salpeter 方程进行激子表征。该方法为描述准粒子效应提供了一种经济高效的方法。此外,我们分析了新合成的锌基体系的晶体结构、热力学稳定性和光电性能,重点关注其结构稳定机制。我们发现晶体结构中 Cs+ 阳离子的分配与两种不同稳定模式的形成之间存在相关性,受金属(Zn 或 Pb)和卤化物成分半径的影响。带隙能量的相对论校正产生的结果在实验值的 10% 以内。此外,结合 Cs2PbI2Cl2 的 eh 准粒子效应,产生了 0.160 eV 的激子结合能,与实验数据非常吻合。这项工作代表了 Cs2ZnX 系统光电表征方面的重大进步,此前该系统的激子特性尚未被探索。
更新日期:2024-09-11
中文翻译:
准二维混合卤化物钙钛矿 Cs2ZnY2X2 的激子特性和太阳能收集性能
由于其低毒性和高温稳定性,无铅准二维金属卤化物钙钛矿(MHP)是用于光电应用的有前途的材料。然而,由于其量子阱拓扑结构,了解它们的结构和光电特性,特别是激子效应(电子空穴对,eh)具有挑战性。我们提出了一种有效的 Cs2ZnX(X = Cl4、Br2Cl2 和 I2Cl2)和 Cs2PbI2Cl2(用作基准)准二维 MHP 带隙校正协议。该协议基于使用密度泛函理论 (DFT) 的相对论准粒子方法 (DFT-1/2)。我们首先研究了卤化物合金的混合贡献,从而在最大局域 Wannier 函数紧束缚方法中使用 Bethe-Salpeter 方程进行激子表征。该方法为描述准粒子效应提供了一种经济高效的方法。此外,我们分析了新合成的锌基体系的晶体结构、热力学稳定性和光电性能,重点关注其结构稳定机制。我们发现晶体结构中 Cs+ 阳离子的分配与两种不同稳定模式的形成之间存在相关性,受金属(Zn 或 Pb)和卤化物成分半径的影响。带隙能量的相对论校正产生的结果在实验值的 10% 以内。此外,结合 Cs2PbI2Cl2 的 eh 准粒子效应,产生了 0.160 eV 的激子结合能,与实验数据非常吻合。这项工作代表了 Cs2ZnX 系统光电表征方面的重大进步,此前该系统的激子特性尚未被探索。