{"title":"探索锡-锗基混合有机-无机过氧化物的潜力:基于密度泛函理论的计算筛选研究。","authors":"Adem Tekin, Merve Kalpar, Emine Tekin","doi":"10.1063/5.0220297","DOIUrl":null,"url":null,"abstract":"<p><p>Hybrid organic-inorganic perovskite solar cells have attracted significant attention in the field of optoelectronics due to their exceptional photovoltaic and optoelectronic properties. Although lead (Pb)-based perovskites exhibit the highest power conversion efficiencies, concerns about their toxicity and environmental impact have prompted significant research activities to explore alternative compositions. In this regard, a special emphasis has been devoted to tin (Sn) and germanium (Ge) based perovskites. In order to reveal the full potential of Sn-Ge based perovskites, we computationally screened perovskites with a general formula of A0.5A0.5'SnyGe1-yX3 (y = 0.00, 0.25, 0.50, 0.75, 1.00) at the density functional theory level, particularly using the HSE06 hybrid functional. By using 18 A/A'-cations, four X-anions, and five different y compositions, a total of 7695 perovskites in cubic (C), orthogonal (O), and tetragonal (T) phases were considered, and the most promising ones have been filtered out based on their formation energy and bandgap. More specifically, 596, 525, and 542 C-, O-, and T-phase perovskites have been identified with a HSE06 bandgap range of 1.0-2.0 eV. While the Sn1.00Ge0.00 composition was dominated for both C- and O-phases, for the T-phase, a higher number of promising perovskites were obtained with the Sn0.75Ge0.25 composition. It has also been found that Sn-rich perovskites exhibit more favorable bandgap characteristics compared to Ge-rich ones. FA, MS, MA, K, Cs, and Rb are the most favored A/A'-cations in these promising perovskites. Moreover, I- overwhelmingly prevails as the dominant anion. Further experimental validation may uncover the true capabilities and practical applicability of these promising perovskites.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1000,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Exploring the potential of Sn-Ge based hybrid organic-inorganic perovskites: A density functional theory based computational screening study.\",\"authors\":\"Adem Tekin, Merve Kalpar, Emine Tekin\",\"doi\":\"10.1063/5.0220297\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Hybrid organic-inorganic perovskite solar cells have attracted significant attention in the field of optoelectronics due to their exceptional photovoltaic and optoelectronic properties. Although lead (Pb)-based perovskites exhibit the highest power conversion efficiencies, concerns about their toxicity and environmental impact have prompted significant research activities to explore alternative compositions. In this regard, a special emphasis has been devoted to tin (Sn) and germanium (Ge) based perovskites. In order to reveal the full potential of Sn-Ge based perovskites, we computationally screened perovskites with a general formula of A0.5A0.5'SnyGe1-yX3 (y = 0.00, 0.25, 0.50, 0.75, 1.00) at the density functional theory level, particularly using the HSE06 hybrid functional. By using 18 A/A'-cations, four X-anions, and five different y compositions, a total of 7695 perovskites in cubic (C), orthogonal (O), and tetragonal (T) phases were considered, and the most promising ones have been filtered out based on their formation energy and bandgap. More specifically, 596, 525, and 542 C-, O-, and T-phase perovskites have been identified with a HSE06 bandgap range of 1.0-2.0 eV. While the Sn1.00Ge0.00 composition was dominated for both C- and O-phases, for the T-phase, a higher number of promising perovskites were obtained with the Sn0.75Ge0.25 composition. It has also been found that Sn-rich perovskites exhibit more favorable bandgap characteristics compared to Ge-rich ones. FA, MS, MA, K, Cs, and Rb are the most favored A/A'-cations in these promising perovskites. Moreover, I- overwhelmingly prevails as the dominant anion. 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引用次数: 0
摘要
有机-无机混合型过氧化物太阳能电池因其卓越的光伏和光电特性而在光电领域备受关注。虽然以铅(Pb)为基础的包晶体具有最高的功率转换效率,但人们对其毒性和环境影响的担忧促使人们开展了大量研究活动,探索替代成分。在这方面,人们特别关注锡(Sn)和锗(Ge)基的包晶石。为了揭示锡-锗基包晶石的全部潜力,我们在密度泛函理论水平上,特别是利用 HSE06 混合函数,对通式为 A0.5A0.5'SnyGe1-yX3(y = 0.00、0.25、0.50、0.75、1.00)的包晶石进行了计算筛选。通过使用 18 个 A/A'阳离子、4 个 X 阴离子和 5 种不同的 y 成分,共考虑了立方(C)、正交(O)和四方(T)相中的 7695 种包晶石,并根据其形成能和带隙筛选出了最有前途的包晶石。更具体地说,已经确定了 596、525 和 542 个 C 相、O 相和 T 相包晶石,其 HSE06 带隙范围为 1.0-2.0 eV。虽然在 C 相和 O 相中,Sn1.00Ge0.00 成分占主导地位,但在 T 相中,Sn0.75Ge0.25 成分的包晶石数量更多。研究还发现,与富含 Ge 的包晶石相比,富含 Sn 的包晶石表现出更有利的带隙特性。FA、MS、MA、K、Cs 和 Rb 是这些前景广阔的包晶石中最受欢迎的 A/A'- 阳离子。此外,I- 作为主要的阴离子占据了压倒性的优势。进一步的实验验证可能会揭示这些前景广阔的包晶的真正能力和实际应用性。
Exploring the potential of Sn-Ge based hybrid organic-inorganic perovskites: A density functional theory based computational screening study.
Hybrid organic-inorganic perovskite solar cells have attracted significant attention in the field of optoelectronics due to their exceptional photovoltaic and optoelectronic properties. Although lead (Pb)-based perovskites exhibit the highest power conversion efficiencies, concerns about their toxicity and environmental impact have prompted significant research activities to explore alternative compositions. In this regard, a special emphasis has been devoted to tin (Sn) and germanium (Ge) based perovskites. In order to reveal the full potential of Sn-Ge based perovskites, we computationally screened perovskites with a general formula of A0.5A0.5'SnyGe1-yX3 (y = 0.00, 0.25, 0.50, 0.75, 1.00) at the density functional theory level, particularly using the HSE06 hybrid functional. By using 18 A/A'-cations, four X-anions, and five different y compositions, a total of 7695 perovskites in cubic (C), orthogonal (O), and tetragonal (T) phases were considered, and the most promising ones have been filtered out based on their formation energy and bandgap. More specifically, 596, 525, and 542 C-, O-, and T-phase perovskites have been identified with a HSE06 bandgap range of 1.0-2.0 eV. While the Sn1.00Ge0.00 composition was dominated for both C- and O-phases, for the T-phase, a higher number of promising perovskites were obtained with the Sn0.75Ge0.25 composition. It has also been found that Sn-rich perovskites exhibit more favorable bandgap characteristics compared to Ge-rich ones. FA, MS, MA, K, Cs, and Rb are the most favored A/A'-cations in these promising perovskites. Moreover, I- overwhelmingly prevails as the dominant anion. Further experimental validation may uncover the true capabilities and practical applicability of these promising perovskites.
期刊介绍:
The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance.
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