气候变化领域集成服务门户(CCPortal): Tuning Electronic Structure in Layered Hybrid Perovskites with Organic Spacer Substitution

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DOI	10.1021/acs.nanolett.9b03427
	Tuning Electronic Structure in Layered Hybrid Perovskites with Organic Spacer Substitution
	Leveillee J.; Katan C.; Even J.; Ghosh D.; Nie W.; Mohite A.D.; Tretiak S.; Schleife A.; Neukirch A.J.
发表日期	2019
ISSN	15306984
起始页码	8732
结束页码	8740
卷号	19 期号:12
英文摘要	Two-dimensional layered halide organic perovskites (LHOPs) are promising candidates for many optoelectronic applications due to their interesting tunable properties. They provide a unique opportunity to control energy and charge dynamics via the independent tunability of the energy levels within the perovskite and the organic spacer for various optoelectronic applications. In the perovskite layer alone, one can replace the Pb (Sn), the halide (X = I, Br, Cl), the organic component, and the number of layers between the organic spacer layers. In addition, there are many possibilities for organic spacer layers between the perovskite layers, making it difficult for experimental methods to comprehensively explore such an extensive combinatorial space. Of particular technological interest is alignment of electronic levels between the perovskite layer and the organic spacer layer, leading to desired transfer of energy or charge carriers between perovskite and organic components. For example, as band edge absorption is almost entirely attributed to the perovskite layer, one way to demonstrate energy transfer is to observe triplet emission from organic spacers. State-of-the-art computational chemistry tools can be used to predict the properties of many stoichiometries in search for LHOPs that have the most promising electronic-structure features. In this first-principles study, we survey a group of Ï€-conjugated organic spacer candidates for use in triplet light-emitting LHOPs. Utilizing density functional theory (DFT) and time-dependent DFT, we calculate the first singlet (S1) and triplet (T1) excitation energy in the ground-state geometry and the first triplet excitation energy in the excited-triplet-state relaxed geometry (T1*). By comparing these energies to the known lowest exciton energy level of PbnX3n+1 perovskite layers (X = I, Br, Cl), we can identify organic spacer and perovskite layer pairings for possible transfer of Wannier excitons from the inorganic perovskite lattice to spin-triplet Frenkel excitons located on the organic cation. We successfully identify ten organic spacer candidates for possible pairing with perovskite layers of specific halide composition to achieve triplet light emission across the visible energy range. Molecular dynamics simulations predict that finite temperatures and perovskite environment have little influence on the average excitation energies of the two common organic spacers naphthylethylammonium (NEA) and phenelethylammonium (PEA). We find significant thermal broadening up to 0.5 eV of the optical excitation energies appearing due to finite temperature effects. The findings herein provide insights into alignment of electronic levels of the conjugated organic spacer with the layer. American Chemical Society.
英文关键词	exciton energy alignment; first-principles simulations; halide perovskite; Layered hybrid organic-inorganic perovskites; organic spacer substitution; triplet light emission
scopus关键词	Computation theory; Computational chemistry; Density functional theory; Electronic structure; Energy transfer; Excitation energy; Excited states; Excitons; Ground state; Light emission; Molecular dynamics; organic-inorganic materials; Tin compounds; Exciton energies; First-principles simulations; Halide perovskites; Hybrid organic-inorganic; Organic spacers; Perovskite
来源期刊	Nano Letters
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/176270
作者单位	Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, IL 61801, United States; Los Alamos National Laboratory, Los Alamos, NM 87545, United States; Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR - UMR 6226, Rennes, F-35000, France; Univ Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, Rennes, F-35000, France; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005, United States; Materials Research Laboratory, University of Illinois at Urbana-Champaign, Urbana, IL 61801, United States; National Center for Supercomputing Applications, University of Illinois at Urbana-Champaign, Urbana, IL 61801, United States
推荐引用方式 GB/T 7714	Leveillee J.,Katan C.,Even J.,et al. Tuning Electronic Structure in Layered Hybrid Perovskites with Organic Spacer Substitution[J],2019,19(12).
APA	Leveillee J..,Katan C..,Even J..,Ghosh D..,Nie W..,...&Neukirch A.J..(2019).Tuning Electronic Structure in Layered Hybrid Perovskites with Organic Spacer Substitution.Nano Letters,19(12).
MLA	Leveillee J.,et al."Tuning Electronic Structure in Layered Hybrid Perovskites with Organic Spacer Substitution".Nano Letters 19.12(2019).