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Understanding macroscale functionality of metal halide perovskites in terms of nanoscale heterogeneities
摘要： Hybrid metal halide perovskites have shown an unprecedented rise as semiconductor building blocks for solar energy conversion and light-emitting applications. Currently, the field moves empirically towards more and more complex chemical compositions, including mixed halide quadruple cation compounds that allow optical properties to be tuned and show promise for better stability. Despite tremendous progress in the field, there is a need for better understanding of mechanisms of efficiency loss and instabilities to facilitate rational optimization of composition. Starting from the device level and then diving into nanoscale properties, we highlight how structural and compositional heterogeneities affect macroscopic optoelectronic characteristics. Furthermore, we provide an overview of some of the advanced spectroscopy and imaging methods that are used to probe disorder and non-uniformities. A unique feature of hybrid halide perovskite compounds is the propensity for these heterogeneities to evolve in space and time under relatively mild illumination and applied electric fields, such as those found within active devices. This introduces an additional challenge for characterization and calls for application of complimentary probes that can aid in correlating the properties of local disorder with macroscopic function, with the ultimate goal of rationally tailoring synthesis towards optimal structures and compositions.
关键词： halide perovskites,structure-function relationship,nanoscale heterogeneities,recombination
更新于2025-09-09 09:28:46
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Structural and thermodynamic limits of layer thickness in 2D halide perovskites
摘要： In the fast-evolving field of halide perovskite semiconductors, the 2D perovskites (A′)2(A)n?1MnX3n+1 [where A = Cs+, CH3NH3+, HC(NH2)2+; A′ = ammonium cation acting as spacer; M = Ge2+, Sn2+, Pb2+; and X = Cl?, Br?, I?] have recently made a critical entry. The n value defines the thickness of the 2D layers, which controls the optical and electronic properties. The 2D perovskites have demonstrated preliminary optoelectronic device lifetime superior to their 3D counterparts. They have also attracted fundamental interest as solution-processed quantum wells with structural and physical properties tunable via chemical composition, notably by the n value defining the perovskite layer thickness. The higher members (n > 5) have not been documented, and there are important scientific questions underlying fundamental limits for n. To develop and utilize these materials in technology, it is imperative to understand their thermodynamic stability, fundamental synthetic limitations, and the derived structure–function relationships. We report the effective synthesis of the highest iodide n-members yet, namely (CH3(CH2)2NH3)2(CH3NH3)5Pb6I19 (n = 6) and (CH3(CH2)2NH3)2(CH3NH3)6Pb7I22 (n = 7), and confirm the crystal structure with single-crystal X-ray diffraction, and provide indirect evidence for “(CH3(CH2)2NH3)2(CH3NH3)8Pb9I28” (“n = 9”). Direct HCl solution calorimetric measurements show the compounds with n > 7 have unfavorable enthalpies of formation (ΔHf), suggesting the formation of higher homologs to be challenging. Finally, we report preliminary n-dependent solar cell efficiency in the range of 9–12.6% in these higher n-members, highlighting the strong promise of these materials for high-performance devices.
关键词： Ruddlesden–Popper halide perovskites,homologous series,photovoltaics,formation enthalpy,layered compounds
更新于2025-09-04 15:30:14
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Enhanced Temperature-Tunable Narrow-Band Photoluminescence from Resonant Perovskite Nanograting
摘要： Tunable light-emitting nanostructures are prospective for reconfigurable compact optoelectronic devices. In this regard, halide perovskites are one of the most efficient class of materials, because of their outstanding electronic and optical properties as well as low cost of fabrication and nanostructuring. Here, we study the temperature-tunable reconfiguration of photonic modes in periodically nanostructured perovskite (MAPbI3) film probed by enhanced photoluminescence. We achieved the quality factors of resonances around 500 at wavelengths 750–760 nm. The experimental results are in well agreement with theoretical simulations. Our study reveals the origin of the emission enhancement from such kind of perovskite nanostructures and paves the way to highly directional, efficient, and tunable narrowband emission from optoelectronic devices.
关键词： Optoelectronic devices,Photoluminescence,Tunable light-emitting nanostructures,Halide perovskites,Nanogratings
更新于2025-09-04 15:30:14