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Kameel Abdel-Latif1 Robert Epps1 Michael Bowen1 Corwin Kerr1 Milad Abolhasani1

1, Chemical Engineering, North Carolina State University, Raleigh, North Carolina, United States

Since the discovery of the colloidal perovskite nanocrystals three years ago, they have rapidly grown to become one of the most promising classes of nanomaterials for large-scale applications in optoelectronic devices. Anion exchange reactions of the highly luminescent cesium lead halide perovskites (CLHPs) provide a facile post-synthetic route for the tuning of the absorption/emission band-gap of CLHPs. These post-synthetic reactions allow the utilization of CLHPs in various optoelectronic applications including third-generation photovoltaic cells and light emitting diodes. Studies of anion-exchange reactions are typically conducted using the time- and material-intensive flask-based synthesis approach. Batch scale synthesis strategies are notorious due to (a) batch-to-batch variation, (b) inefficient and irreproducible mixing timescales, (c) manual sampling and characterization at room temperature, and (d) poor size distribution of the resulting nanocrystals after scale-up. Here, we present a modular multiphase microfluidic strategy with an in situ spectral monitoring capability that enables the systematic kinetic study of anion-exchange reactions of CLHP nanocrystals. Utilizing the microfluidic nanocrystal synthesis platform, we monitor absorption and emission spectra of CLHPs, in real-time, over residence times ranging between 100 ms and 17 min. In-situ monitoring of the optoelectronic properties of CLHPs over different synthesis conditions enables fundamental and applied studies of structural tuning of CLHPs via anion-exchange reactions. The enhanced mixing feature of the multiphase flow along with the novel anion-exchange framework using ZnX2 (X=I or Cl) facilitates on-demand bandgap tuning of high-quality CLHPs (i.e., narrow size distribution with high quantum yield) via a positive feedback loop in which synthesis parameters are varied until the target optoelectronic characteristics are achieved.

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