Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering
Abstract Phase instability poses a serious challenge to the commercialization of formamidinium lead iodide (FAPbI3)-based solar cells and optoelectronic devices. Here, we combine density functional theory and machine learning molecular dynamics simulations, to investigate the mechanism driving the u...
| Main Authors: | , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2024-02-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-46044-x |
| _version_ | 1797274012827516928 |
|---|---|
| author | Yuhang Liang Feng Li Xiangyuan Cui Taoyuze Lv Catherine Stampfl Simon P. Ringer Xudong Yang Jun Huang Rongkun Zheng |
| author_facet | Yuhang Liang Feng Li Xiangyuan Cui Taoyuze Lv Catherine Stampfl Simon P. Ringer Xudong Yang Jun Huang Rongkun Zheng |
| author_sort | Yuhang Liang |
| collection | DOAJ |
| description | Abstract Phase instability poses a serious challenge to the commercialization of formamidinium lead iodide (FAPbI3)-based solar cells and optoelectronic devices. Here, we combine density functional theory and machine learning molecular dynamics simulations, to investigate the mechanism driving the undesired α-δ phase transition of FAPbI3. Prevalent iodine vacancies and interstitials can significantly expedite the structural transition kinetics by inducing robust covalency during transition states. Extrinsically, the detrimental roles of atmospheric moisture and oxygen in degrading the FAPbI3 perovskite phase are also rationalized. Significantly, we discover the compositional design principles by categorizing that A-site engineering primarily governs thermodynamics, whereas B-site doping can effectively manipulate the kinetics of the phase transition in FAPbI3, highlighting lanthanide ions as promising B-site substitutes. A-B mixed doping emerges as an efficient strategy to synergistically stabilize α-FAPbI3, as experimentally demonstrated by substantially higher initial optoelectronic characteristics and significantly enhanced phase stability in Cs-Eu doped FAPbI3 as compared to its Cs-doped counterpart. This study provides scientific guidance for the design and optimization of long-term stable FAPbI3-based solar cells and other optoelectronic devices through defect control and synergetic composition engineering. |
| first_indexed | 2024-03-07T14:52:19Z |
| format | Article |
| id | doaj.art-29360906ac1c463d933e474d934fa47c |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-07T14:52:19Z |
| publishDate | 2024-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-29360906ac1c463d933e474d934fa47c2024-03-05T19:36:24ZengNature PortfolioNature Communications2041-17232024-02-0115111210.1038/s41467-024-46044-xToward stabilization of formamidinium lead iodide perovskites by defect control and composition engineeringYuhang Liang0Feng Li1Xiangyuan Cui2Taoyuze Lv3Catherine Stampfl4Simon P. Ringer5Xudong Yang6Jun Huang7Rongkun Zheng8School of Chemical and Biomolecular Engineering, The University of SydneySchool of Physics, The University of SydneySchool of Aerospace, Mechanical and Mechatronic Engineering, The University of SydneySchool of Physics, The University of SydneySchool of Physics, The University of SydneySchool of Aerospace, Mechanical and Mechatronic Engineering, The University of SydneyState Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong UniversitySchool of Chemical and Biomolecular Engineering, The University of SydneySchool of Physics, The University of SydneyAbstract Phase instability poses a serious challenge to the commercialization of formamidinium lead iodide (FAPbI3)-based solar cells and optoelectronic devices. Here, we combine density functional theory and machine learning molecular dynamics simulations, to investigate the mechanism driving the undesired α-δ phase transition of FAPbI3. Prevalent iodine vacancies and interstitials can significantly expedite the structural transition kinetics by inducing robust covalency during transition states. Extrinsically, the detrimental roles of atmospheric moisture and oxygen in degrading the FAPbI3 perovskite phase are also rationalized. Significantly, we discover the compositional design principles by categorizing that A-site engineering primarily governs thermodynamics, whereas B-site doping can effectively manipulate the kinetics of the phase transition in FAPbI3, highlighting lanthanide ions as promising B-site substitutes. A-B mixed doping emerges as an efficient strategy to synergistically stabilize α-FAPbI3, as experimentally demonstrated by substantially higher initial optoelectronic characteristics and significantly enhanced phase stability in Cs-Eu doped FAPbI3 as compared to its Cs-doped counterpart. This study provides scientific guidance for the design and optimization of long-term stable FAPbI3-based solar cells and other optoelectronic devices through defect control and synergetic composition engineering.https://doi.org/10.1038/s41467-024-46044-x |
| spellingShingle | Yuhang Liang Feng Li Xiangyuan Cui Taoyuze Lv Catherine Stampfl Simon P. Ringer Xudong Yang Jun Huang Rongkun Zheng Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering Nature Communications |
| title | Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| title_full | Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| title_fullStr | Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| title_full_unstemmed | Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| title_short | Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| title_sort | toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering |
| url | https://doi.org/10.1038/s41467-024-46044-x |
| work_keys_str_mv | AT yuhangliang towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT fengli towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT xiangyuancui towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT taoyuzelv towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT catherinestampfl towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT simonpringer towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT xudongyang towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT junhuang towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering AT rongkunzheng towardstabilizationofformamidiniumleadiodideperovskitesbydefectcontrolandcompositionengineering |