Exploration of B-site alloying in partially reducing Pb toxicity and regulating thermodynamic stability and electronic properties of halide perovskites

作     者：Xinjiang Wang Muhammad Faizan Kun Zhou Hongshuai Zou Qiaoling Xu Yuhao Fu Lijun Zhang 

作者机构：State Key Laboratory of Superhard MaterialsCollege of PhysicsJilin UniversityChangchun 130012China State Key Laboratory of Integrated OptoelectronicsKey Laboratory of Automobile Materials of MOECollege of Materials Science and EngineeringJilin UniversityChangchun 130012China College of Physics and Electronic EngineeringCenter for Computational SciencesSichuan Normal UniversityChengdu 610068China International Center of Computational Method and SoftwareJilin UniversityChangchun 130012China 

出 版 物：《Science China(Physics,Mechanics & Astronomy)》 (中国科学：物理学、力学、天文学（英文版）)

年 卷 期：2023年第66卷第3期

页      面：130-138页

核心收录：

学科分类：08[工学] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Natural Science Foundation of China(Grant Nos.12004131,and 22090044) the Jilin Province Science and Technology Development Program(Grant No.20210508044RQ) 

主　　题：lead-based halide perovskites alloying thermodynamic stability first-principles calculations optoelectronic applications 

摘      要：Alloying strategies provide a high degree of freedom for reducing lead toxicity,improving thermodynamic stability, tuning the optoelectronic properties of ABX3 halide perovskites by varying the alloying element species and their *** the key role of B-site cations in contributing band edge states and modulating structure factors in halide perovskites,the partial replacement of Pb2+with different B-site metal ions has been *** several experimental attempts have been made to date,the effect of B-site alloying on the stability and electronic properties of halide perovskites has not been fully ***,we take cubic CsPbBr3 perovskite as the prototype material and systematically explore the effects of B-site alloying on Pb-containing *** to the presence or absence of the corresponding perovskite phase,the ten alloying elements investigated are classified into three types(i.e.,Type Ⅰ:Sn Ge,Ca,Sr;Type Ⅱ:Cd,Mg,Mn;Type Ⅲ:Ba,Zn,Cu).Based on the first-principles calculations,we obtain the following ***,these B-site alloys will exist as disordered solid solutions rather than ordered structures at room temperature throughout the composition ***,the alloying of Sn and Ge enhances the thermodynamic stability of the cubic perovskite host,whereas the alloying of the other elements has no remarkable effect on the thermodynamic stability of the cubic perovskite ***,the underlying physical mechanism for bandgap tuning can be attributed to the atomic orbital energy mismatch or quantum confinement ***,the alloying of different elements demonstrates the diversity in the regulation of crystal structure and electronic properties,indicating potential applications in photovoltaic s and self-trapped exciton-based light-emitting *** work provides theoretical guidance for using alloying strategies to reduce lead toxicity,enhance stability,and optimize the electronic properties of halide perovsk