Sequential Crystallization of Two-Dimensional Layered Perovskite Heterostructures
Alexander Schleusener a, Mehrdad Faraji a b, Roman Krahne a
a Istituto Italiano di Tecnologia, via Morego 30, 16163 Genova, Italy
b Dipartimento di Chimica e Chimica Industriale, Università degli Studi di Genova, Via Dodecaneso 31, 16146 Genova, Italy
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
From halide perovskites to perovskite-inspired materials –Synthesis and Applications - #PeroMat
Sevilla, Spain, 2025 March 3rd - 7th
Organizers: Raquel Galian, Thomas Stergiopoulos and Paola Vivo
Oral, Alexander Schleusener, presentation 250
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.250
Publication date: 16th December 2024

Two-dimensional layered metal-halide perovskites (2DLPs) are an emerging class of materials, characterized by a semiconducting metal-halide octahedral layer sandwiched between two layers of bulky organic cations. This unique structural arrangement allows for high in-plane mobility of excitons and charge carriers, while the predominantly insulating nature of the organic cations restricts out-of-plane mobility [1], [2]. The latter prevents studies of charge and energy transfer processes in vertical heterostructures. On the other hand, lateral heterostructures, where compositional changes occur along the in-plane direction, offer an interesting platform to explore potential charge transfer mechanisms at the junction interface [3].

To improve the accessibility and quality of heterostructures in 2DLPs, we developed a one-pot synthesis strategy for preparing lateral heterostructures that consist of different halide compositions. Compared to our previous solution-based anion exchange method [4], the presented approach produces consistently heterostructures with high-quality crystalline interfaces between the Br-rich core and the I-rich frame. We systematically investigated the effects of antisolvent, concentration, injection rates, and the Br-to-I ratio. Interestingly, when the iodine content in the precursor solution is increased, the core is eventually consumed, resulting in an I-rich frame-only structure. We attribute this to a combination of partial ion migration on top of the stepwise crystallization process. Additionally, we extended this concept to 2DLPs heterostructures featuring different metal cations including lead-free heterostructure.

The formation of heterojunctions within the in-plane semiconducting layer offers the potential to direct charge carriers or energy flow toward either the edges or the center of these microstructures, which is appealing for applications in energy harvesting and photocatalysis.

A.S. acknowledges the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Funding Program (Project TOGETHER, grant agreement No.101067869)

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