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Thick-Layer Lead Iodide Perovskites with Bifunctional Organic Spacers Allylammonium and Iodopropylammonium Exhibiting Trap-State Emission.

التفاصيل البيبلوغرافية
العنوان: Thick-Layer Lead Iodide Perovskites with Bifunctional Organic Spacers Allylammonium and Iodopropylammonium Exhibiting Trap-State Emission.
المؤلفون: Vasileiadou ES; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Jiang X; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Kepenekian M; Univ Rennes, ENSCR, CNRS, ISCR, UMR 6226, F-35000 Rennes, France., Even J; Univ Rennes, INSA Rennes, CNRS, Institut FOTON, UMR 6082, F-35000 Rennes, France., De Siena MC; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Klepov VV; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Friedrich D; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Spanopoulos I; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Tu Q; Department of Materials Science & Engineering, Texas A&M University, College Station, Texas 77840, United States., Tajuddin IS; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Weiss EA; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States., Kanatzidis MG; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
المصدر: Journal of the American Chemical Society [J Am Chem Soc] 2022 Apr 13; Vol. 144 (14), pp. 6390-6409. Date of Electronic Publication: 2022 Apr 05.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Publication: Washington, DC : American Chemical Society
Original Publication: Easton, Pa. [etc.]
مستخلص: The nature of the organic cation in two-dimensional (2D) hybrid lead iodide perovskites tailors the structural and technological features of the resultant material. Herein, we present three new homologous series of (100) lead iodide perovskites with the organic cations allylammonium (AA) containing an unsaturated C═C group and iodopropylammonium (IdPA) containing iodine on the organic chain: (AA) 2 MA n -1 Pb n I 3 n +1 ( n = 3-4), [(AA) x (IdPA) 1- x ] 2 MA n -1 Pb n I 3 n +1 ( n = 1-4), and (IdPA) 2 MA n -1 Pb n I 3 n +1 ( n = 1-4), as well as their perovskite-related substructures. We report the in situ transformation of AA organic layers into IdPA and the incorporation of these cations simultaneously into the 2D perovskite structure. Single-crystal X-ray diffraction shows that (AA) 2 MA 2 Pb 3 I 10 crystallizes in the space group P 2 1 / c with a unique inorganic layer offset (0, <1/2), comprising the first example of n = 3 halide perovskite with a monoammonium cation that deviates from the Ruddlesden-Popper (RP) halide structure type. (IdPA) 2 MA 2 Pb 3 I 10 and the alloyed [(AA) x (IdPA) 1- x ] 2 MA 2 Pb 3 I 10 crystallize in the RP structure, both in space group P 2 1 / c . The adjacent I···I interlayer distance in (AA) 2 MA 2 Pb 3 I 10 is ∼5.6 Å, drawing the [Pb 3 I 10 ] 4- layers closer together among all reported n = 3 RP lead iodides. (AA) 2 MA 2 Pb 3 I 10 presents band-edge absorption and photoluminescence (PL) emission at around 2.0 eV that is slightly red-shifted in comparison to (IdPA) 2 MA 2 Pb 3 I 10 . The band structure calculations suggest that both (AA) 2 MA 2 Pb 3 I 10 and (IdPA) 2 MA 2 Pb 3 I 10 have in-plane effective masses around 0.04 m 0 and 0.08 m 0 , respectively. IdPA cations have a greater dielectric contribution than AA. The excited-state dynamics investigated by transient absorption (TA) spectroscopy reveal a long-lived (∼100 ps) trap state ensemble with broad-band emission; our evidence suggests that these states appear due to lattice distortions induced by the incorporation of IdPA cations.
تواريخ الأحداث: Date Created: 20220405 Latest Revision: 20220413
رمز التحديث: 20221213
DOI: 10.1021/jacs.2c00571
PMID: 35378979
قاعدة البيانات: MEDLINE
الوصف
تدمد:1520-5126
DOI:10.1021/jacs.2c00571