Jared D. Fletcher, Aaron M. Schankler, Cheng Liu, Yi Yang, Claudia Pereyra Huelmo, Craig C. Laing, Evan H. Oriel, Lin X. Chen, Richard D. Schaller, Edward H. Sargent, Andrew M. Rappe and Mercouri G. Kanatzidis*,
{"title":"两种间隔物,一种过氧化物:整合 Ruddlesden-Popper 和 Dion-Jacobson 卤化物包光体","authors":"Jared D. Fletcher, Aaron M. Schankler, Cheng Liu, Yi Yang, Claudia Pereyra Huelmo, Craig C. Laing, Evan H. Oriel, Lin X. Chen, Richard D. Schaller, Edward H. Sargent, Andrew M. Rappe and Mercouri G. Kanatzidis*, ","doi":"10.1021/acs.chemmater.4c00907","DOIUrl":null,"url":null,"abstract":"<p >Hybrid organic–inorganic perovskites are a rapidly developing class of materials due to their desirable properties for optoelectronic applications such as their ease of synthesis, solution-processable film formation, tunable band gap, strong photoluminescence, good charge carrier mobilities, and high defect tolerance. We present a novel 2D perovskite motif that seamlessly integrates the structural elements from both Ruddlesden–Popper and Dion–Jacobson halide perovskites. We demonstrate the incorporation of two different organic spacer cations in an ordered manner in 5 novel 2D perovskite iodide materials. Both a cyclic diammonium cation 3-(aminomethyl)piperidinium (3AMP) and a linear alkyl monoammonium cation (C<i>n</i> = C<sub><i>n</i></sub>H<sub>2<i>n</i>+4</sub>N, <i>n</i> = 4–8) are present in distinct alternating layers, making the new series (C<i>n</i>)<sub>2</sub>(3AMP)[PbI<sub>4</sub>]<sub>2</sub>. The crystallization of these materials was optimized through careful temperature control to obtain precise crystal structures via single-crystal X-ray diffraction (XRD) which confirmed the presence of the two cations in distinct layers. The influence of the two spacers on optical properties including the band gaps and photoluminescence spectra are found to more closely resemble (3AMP)PbI<sub>4</sub> than (C<i>n</i>)<sub>2</sub>PbI<sub>4</sub>, which can be attributed to the amount of distortion imposed by the 3AMP spacer on the lead iodide layers. The findings are supported by density functional theory calculations. The strong photoelectric response of solution-processed thin films shows the potential of these materials in photodetectors or photovoltaics. This unprecedented amalgamation of RP–DJ in (C<i>n</i>)<sub>2</sub>(3AMP)[PbI<sub>4</sub>]<sub>2</sub> in a structurally ordered fashion suggests a potential vastly underexplored phase space of 2D perovskites in which there are chemically different spacers in distinct layers of the structure, providing an additional parameter to tune perovskite properties.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Two Spacers, One Perovskite: Integrating Ruddlesden–Popper and Dion–Jacobson Halide Perovskites\",\"authors\":\"Jared D. Fletcher, Aaron M. Schankler, Cheng Liu, Yi Yang, Claudia Pereyra Huelmo, Craig C. Laing, Evan H. Oriel, Lin X. Chen, Richard D. Schaller, Edward H. Sargent, Andrew M. Rappe and Mercouri G. Kanatzidis*, \",\"doi\":\"10.1021/acs.chemmater.4c00907\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Hybrid organic–inorganic perovskites are a rapidly developing class of materials due to their desirable properties for optoelectronic applications such as their ease of synthesis, solution-processable film formation, tunable band gap, strong photoluminescence, good charge carrier mobilities, and high defect tolerance. We present a novel 2D perovskite motif that seamlessly integrates the structural elements from both Ruddlesden–Popper and Dion–Jacobson halide perovskites. We demonstrate the incorporation of two different organic spacer cations in an ordered manner in 5 novel 2D perovskite iodide materials. Both a cyclic diammonium cation 3-(aminomethyl)piperidinium (3AMP) and a linear alkyl monoammonium cation (C<i>n</i> = C<sub><i>n</i></sub>H<sub>2<i>n</i>+4</sub>N, <i>n</i> = 4–8) are present in distinct alternating layers, making the new series (C<i>n</i>)<sub>2</sub>(3AMP)[PbI<sub>4</sub>]<sub>2</sub>. The crystallization of these materials was optimized through careful temperature control to obtain precise crystal structures via single-crystal X-ray diffraction (XRD) which confirmed the presence of the two cations in distinct layers. The influence of the two spacers on optical properties including the band gaps and photoluminescence spectra are found to more closely resemble (3AMP)PbI<sub>4</sub> than (C<i>n</i>)<sub>2</sub>PbI<sub>4</sub>, which can be attributed to the amount of distortion imposed by the 3AMP spacer on the lead iodide layers. The findings are supported by density functional theory calculations. The strong photoelectric response of solution-processed thin films shows the potential of these materials in photodetectors or photovoltaics. This unprecedented amalgamation of RP–DJ in (C<i>n</i>)<sub>2</sub>(3AMP)[PbI<sub>4</sub>]<sub>2</sub> in a structurally ordered fashion suggests a potential vastly underexplored phase space of 2D perovskites in which there are chemically different spacers in distinct layers of the structure, providing an additional parameter to tune perovskite properties.</p>\",\"PeriodicalId\":33,\"journal\":{\"name\":\"Chemistry of Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2024-06-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry of Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.chemmater.4c00907\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.chemmater.4c00907","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Two Spacers, One Perovskite: Integrating Ruddlesden–Popper and Dion–Jacobson Halide Perovskites
Hybrid organic–inorganic perovskites are a rapidly developing class of materials due to their desirable properties for optoelectronic applications such as their ease of synthesis, solution-processable film formation, tunable band gap, strong photoluminescence, good charge carrier mobilities, and high defect tolerance. We present a novel 2D perovskite motif that seamlessly integrates the structural elements from both Ruddlesden–Popper and Dion–Jacobson halide perovskites. We demonstrate the incorporation of two different organic spacer cations in an ordered manner in 5 novel 2D perovskite iodide materials. Both a cyclic diammonium cation 3-(aminomethyl)piperidinium (3AMP) and a linear alkyl monoammonium cation (Cn = CnH2n+4N, n = 4–8) are present in distinct alternating layers, making the new series (Cn)2(3AMP)[PbI4]2. The crystallization of these materials was optimized through careful temperature control to obtain precise crystal structures via single-crystal X-ray diffraction (XRD) which confirmed the presence of the two cations in distinct layers. The influence of the two spacers on optical properties including the band gaps and photoluminescence spectra are found to more closely resemble (3AMP)PbI4 than (Cn)2PbI4, which can be attributed to the amount of distortion imposed by the 3AMP spacer on the lead iodide layers. The findings are supported by density functional theory calculations. The strong photoelectric response of solution-processed thin films shows the potential of these materials in photodetectors or photovoltaics. This unprecedented amalgamation of RP–DJ in (Cn)2(3AMP)[PbI4]2 in a structurally ordered fashion suggests a potential vastly underexplored phase space of 2D perovskites in which there are chemically different spacers in distinct layers of the structure, providing an additional parameter to tune perovskite properties.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.