Comprehensive evaluation of structural stability and optoelectronic performance of double perovskites Cs2AuMCl6 (M = Sb, Bi): Insights from theoretical perspectives
IF 3.1 3区 材料科学Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Diwen Liu , Hongyan Zeng , Shuyun Huang , Helong Wu , Jianzhi Sun , Rongjian Sa , Si-Min Xu
{"title":"Comprehensive evaluation of structural stability and optoelectronic performance of double perovskites Cs2AuMCl6 (M = Sb, Bi): Insights from theoretical perspectives","authors":"Diwen Liu , Hongyan Zeng , Shuyun Huang , Helong Wu , Jianzhi Sun , Rongjian Sa , Si-Min Xu","doi":"10.1016/j.commatsci.2025.113988","DOIUrl":null,"url":null,"abstract":"<div><div>Low-cost and high-performance lead-based halide perovskites have garnered intense interest, yet there are still two key issues like intrinsic instability and toxicity that need to be resolved. In this study, first-principles calculations are utilized to systematically evaluate the stability and optoelectronic properties of lead-free double perovskites Cs<sub>2</sub>AuMCl<sub>6</sub> (M = Sb, Bi).<!--> <!-->Our calculations show that these two perovskites exhibit both thermodynamic and dynamic stability, suggesting their experimental synthesizability. Both compounds are characterized as indirect-gap semiconductors with fundamental gaps of 1.09 eV for Cs<sub>2</sub>AuSbCl<sub>6</sub> and 1.58 eV for Cs<sub>2</sub>AuBiCl<sub>6</sub>.<!--> <!-->Further analysis reveals that they demonstrate favorable properties, such as low effective mass (0.18–0.32 <em>m</em><sub>0</sub>) and small exciton binding energy (60–90 meV). Nevertheless, the significant mismatch between the optical absorption edge and fundamental gap in Cs<sub>2</sub>AuMCl<sub>6</sub> (M = Sb, Bi) severely limits its solar absorption efficiency. Consequently, their maximum conversion efficiencies remain relatively low (15.60 % for Cs<sub>2</sub>AuSbCl<sub>6</sub> and 7.75 % for Cs<sub>2</sub>AuBiCl<sub>6</sub>). Our comprehensive investigation of electronic structure and optical absorption uncovers the intrinsic mechanisms behind these efficiency limitations. This study provides valuable insights and guidance for the development of high-efficiency perovskite materials.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"256 ","pages":"Article 113988"},"PeriodicalIF":3.1000,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Computational Materials Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0927025625003313","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Low-cost and high-performance lead-based halide perovskites have garnered intense interest, yet there are still two key issues like intrinsic instability and toxicity that need to be resolved. In this study, first-principles calculations are utilized to systematically evaluate the stability and optoelectronic properties of lead-free double perovskites Cs2AuMCl6 (M = Sb, Bi). Our calculations show that these two perovskites exhibit both thermodynamic and dynamic stability, suggesting their experimental synthesizability. Both compounds are characterized as indirect-gap semiconductors with fundamental gaps of 1.09 eV for Cs2AuSbCl6 and 1.58 eV for Cs2AuBiCl6. Further analysis reveals that they demonstrate favorable properties, such as low effective mass (0.18–0.32 m0) and small exciton binding energy (60–90 meV). Nevertheless, the significant mismatch between the optical absorption edge and fundamental gap in Cs2AuMCl6 (M = Sb, Bi) severely limits its solar absorption efficiency. Consequently, their maximum conversion efficiencies remain relatively low (15.60 % for Cs2AuSbCl6 and 7.75 % for Cs2AuBiCl6). Our comprehensive investigation of electronic structure and optical absorption uncovers the intrinsic mechanisms behind these efficiency limitations. This study provides valuable insights and guidance for the development of high-efficiency perovskite materials.
期刊介绍:
The goal of Computational Materials Science is to report on results that provide new or unique insights into, or significantly expand our understanding of, the properties of materials or phenomena associated with their design, synthesis, processing, characterization, and utilization. To be relevant to the journal, the results should be applied or applicable to specific material systems that are discussed within the submission.