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Tuning the Luminescence of Layered Halide Perovskites † † Matthew D

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Tuning the Luminescence of Layered Halide Perovskites † † Matthew D Review Cite This: Chem. Rev. XXXX, XXX, XXX−XXX pubs.acs.org/CR Tuning the Luminescence of Layered Halide Perovskites † † Matthew D. Smith, Bridget A. Connor, and Hemamala I. Karunadasa* Department of Chemistry, Stanford University, Stanford, California 94305, United States ABSTRACT: Layered halide perovskites offer a versatile platform for manipulating light through synthetic design. Although most layered perovskites absorb strongly in the ultraviolet (UV) or near-UV region, their emission can range from the UV to the infrared region of the electromagnetic spectrum. This emission can be very narrow, displaying high color purity, or it can be extremely broad, spanning the entire visible spectrum and providing high color rendition (or accurately reproducing illuminated colors). The origin of the photoluminescence can vary enormously. Strongly correlated electron−hole pairs, permanent lattice defects, transient light-induced defects, and ligand-field transitions in the inorganic layers and molecular chromophores in the organic layers can be involved in the emission mechanism. In this review, we highlight the different types of photoluminescence that may be attained from layered halide perovskites, with an emphasis on how the emission may be systematically tuned through changes to the bulk crystalline lattice: changes in composition, structure, and dimensionality. CONTENTS 6.1.2. Structural Distortion K 6.1.3. Excited-State Coupling L 1. Introduction B 6.2. Group 14 Perovskites with Thick (1 < n < ∞) 1.1. Background B Inorganic Layers L 1.1.1. Further Literature B 6.2.1. Luminescence M 1.2. History B 6.2.2. Compositional Heterogeneity in Films M 1.2.1. Three-Dimensional Halide Perovskites B 6.2.3. Excited-State Dynamics N 1.2.2. Two-Dimensional Halide Perovskites C 6.3. Rare-Earth Perovskites O 2. Structure E 7. Broad Emission O 2.1. Three-Dimensional Perovskites E 7.1. White-Light-Emitting Perovskites O 2.2. Two-Dimensional Perovskites E 7.1.1. (110) Perovskites with Corrugated In- 2.2.1. Connectivity of the Inorganic Layer E organic Layers O 2.2.2. Structural Distortions of the Inorganic 7.1.2. (001) Perovskites with Flat Inorganic Layer E Layers P 2.2.3. Thickness of the Inorganic Layer F 7.2. Proposed Mechanism of White-Light Emis- 2.2.4. The A Site F sion Q 2.2.5. The B Site F 7.2.1. Electronic Origins of White-Light Emis- 2.2.6. The X Site G Downloaded via STANFORD UNIV on February 8, 2019 at 22:16:15 (UTC). sion Q 3. Synthesis G 7.2.2. Mechanistic Insights Q 4. Electronic Structure G 7.2.3. Structural Origins of White-Light Emis- 4.1. Transition-Metal-Based 2D Perovskites G sion R See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles. 4.2. Semiconducting 2D Perovskites G fi 7.2.4. Structural Correlations with the Emis- 5. Electronic Con nement H sion Width S 5.1. Excitons H 7.3. Broadened Emission from Lead Halide 5.2. Electronic Confinement Effects H E Perovskites S 5.2.1. Tuning b through the Organic Layer I − E 7.3.1. Layered Pb I Perovskites: Emission 5.2.2. Tuning b through the Inorganic Layer I from Defects S 5.3. Trapped Excitons I 7.3.2. An Attempt at Unifying the Mechanism 5.3.1. Bound Excitons I of the Broad Emission from Pb−X 5.3.2. Self-Trapped Excitons I Perovskites (X = Cl, Br, and I) T 5.3.3. An Analogy for Intrinsic and Extrinsic 7.3.3. Layered Pb−I−SCN Perovskites T Self-Trapping J E 7.4. Broadened Emission from Other Metal 5.4. Determining the Band Gap ( g) and Exciton E Halide Perovskites T Binding Energy ( b)J 6. Narrow Emission J 6.1. Group 14 Perovskites with Thin (n =1) Special Issue: Perovskites Inorganic Layers K Received: July 28, 2018 6.1.1. Halide Substitution K © XXXX American Chemical Society A DOI: 10.1021/acs.chemrev.8b00477 Chem. Rev. XXXX, XXX, XXX−XXX Chemical Reviews Review 7.4.1. Layered Double Perovskites T emission with high color rendition. The luminescence may 7.4.2. Layered Cd−Cl Perovskites U originate from either the inorganic or the organic layers. 7.4.3. Layered Ge−I Perovskites U Within the inorganic layers, radiative recombination of 7.4.4. Layered Mn−X Perovskites U excitons (excited electron−hole pairs) that migrate freely in 7.4.5. (111) Perovskites with Trivalent Metals U the lattice (free excitons), interact with lattice defects (bound 7.5. Broad Emission from Low-Dimensional excitons), or create transient lattice deformations (self-trapped Non-Perovskite Lattices V excitons) have been invoked while describing the emission 7.6. Broad Emission from Dopants V mechanism. The emission from the inorganic layers can also 7.6.1. MnII Dopants V arise from localized transitions within the ligand-field manifold 7.6.2. BiIII Dopants V of a single metal incorporated either stoichiometrically or as a 8. Emission from the Organic Layer W dopant. In the organic layers, the emission may originate from 8.1. Weak Coupling between Organic and chromophores that are excited either directly by light or Inorganic Layers W indirectly through energy transfer from the inorganic layers. 8.2. Strong Coupling between Organic and These various emission pathways may also mix, with the Inorganic Layers W photoluminescence showing signatures of both free and 8.3. Mechanism of Energy Transfer X trapped excitons, self-trapped excitons that interact with lattice 8.4. Effects of the Inorganic Lattice X defects or that evolve into lattice defects, and excitation 8.4.1. Packing Effects X transfer between the lattice and dopants and between the 8.4.2. Energetic Effects X organic and inorganic components. 9. Applications in Luminescence Y In this article we review the substantial research on studying, 9.1. Phosphors Y understanding, and then synthetically tuning the various 9.1.1. Narrow Emission Y radiative recombination pathways in layered halide perovskites. 9.1.2. Broad Emission Y Although the focus here is on 2D perovskites (and their close 9.2. Light-Emitting Diodes Z relatives), we note that many of the mechanistic insights 9.3. Scintillators Z gained from the photophysical studies of these materials are 10. Summary and Outlook AA broadly applicable to other low-dimensional inorganic lattices. 10.1. Gaining Synthetic Control over “Excited- Importantly, the high degree of crystallinity of halide ” State Defects AA perovskites, coupled with the precise tunability of the “ 10.2. Gaining Synthetic Control over Ground- constituent organic molecules, affords a very large phase ” State Defects AA space of compounds for careful study (Figure 1). Over the past 10.3. Navigating the Excited State AA century, these materials have evolved from scientific 10.4. Controlling and Using Film Heterogeneity AB curiosities1 and model compounds2 to functional materials 10.5. Mixing Metals and Ligands AB whose applications span technologies including photovoltaics,3 − 10.6. Further Activating the Organic Layer AB light-emitting diodes,4 9 and phosphors.10,11 Indeed, early 10.7. Shining Brighter and for Longer AB interest in the photophysics of halide perovskites rested Author Information AB primarily with the layered or 2D materials. However, the Corresponding Author AB exemplary performance of 3D lead halide perovskites as solar- ORCID AB cell absorbers12,13 motivates a timely return to their 2D Author Contributions AB congeners. We restrict our discussion to how the luminescence Notes AB of the bulk material can be tuned through synthetic design and Biographies AB refer the interested reader to other articles for the effects of Acknowledgments AB nanostructuring.14,15 References AB 1.1.1. Further Literature. With over a century of research behind halide perovskites,1,16,17 there are a large number of reviews that stand alongside the development of the layered 1. INTRODUCTION perovskites, covering a number of specialized topics in detail. 1.1. Background In particular, we refer the interested reader to early reviews of synthesis and crystal growth,18 the optical properties of 2D Layered halide perovskites are crystalline solids that comprise Pb−I perovskites,19 the seminal introduction20 to layered anionic metal halide sheets partitioned by arrays of cations. perovskites and a more recent review,21 the electronic structure Often, these cations are organic molecules, giving rise to a and its optoelectronic consequences,22 and layered perovskites’ diverse family of organic−inorganic hybrid materials (Figure postsynthetic transformations,23 high-pressure properties,24 1). Layered halide perovskites are related to the perovskite (or and white-light emission,25 as well as a general introduction calcium titanate) structure type through dimensional reduc- to the material family.26 tion: the conceptual slicing of a three-dimensional (3D) lattice 1.2. History along a certain index to yield a two-dimensional (2D) lattice (Figure 2). 1.2.1. Three-Dimensional Halide Perovskites. The Photoluminescence, the emission of photons following light history of the 3D halide perovskites is contemporaneous absorption, from layered halide perovskites encompasses a with their layered congeners, and both classes of materials have striking diversity. The emission covers a range of energies/ similarly experienced peaks and troughs in study (Figure 3). I II colors near-UV, purple, blue, green, orange, red, white, and The early 3D halide perovskites, with the formula A B X3 (see near-IR (Table 1)and a range of widthsfrom narrow blue section 2.1), which were structurally characterized by X-ray ff 27 II II emission with high color purity to broadband white-light di raction, include KMgF3 in 1925 and CsBCl3 (B =Cd, B DOI: 10.1021/acs.chemrev.8b00477 Chem. Rev. XXXX, XXX, XXX−XXX Chemical Reviews Review 107 Figure 1.
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