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Metal cation‐doped lead halide perovskite (LHP) quantum dots (QDs) with photoluminescence quantum yields (PLQYs) higher than unity, due to quantum cutting phenomena, are an important building block of the next‐generation renewable energy technologies. However, synthetic route exploration and development of the highest‐performing QDs for device applications remain challenging. In this work, Smart Dope is presented, which is a self‐driving fluidic lab (SDFL), for the accelerated synthesis space exploration and autonomous optimization of LHP QDs. Specifically, the multi‐cation doping of CsPbCl3 QDs using a one‐pot high‐temperature synthesis chemistry is reported. Smart Dope continuously synthesizes multi‐cation‐doped CsPbCl3 QDs using a high‐pressure gas‐liquid segmented flow format to enable continuous experimentation with minimal experimental noise at reaction temperatures up to 255°C. Smart Dope offers multiple functionalities, including accelerated mechanistic studies through digital twin QD synthesis modeling, closed‐loop autonomous optimization for accelerated QD synthetic route discovery, and on‐demand continuous manufacturing of high‐performing QDs. Through these developments, Smart Dope autonomously identifies the optimal synthetic route of Mn‐Yb co‐doped CsPbCl3 QDs with a PLQY of 158%, which is the highest reported value for this class of QDs to date. Smart Dope illustrates the power of SDFLs in accelerating the discovery and development of emerging advanced energy materials. [ABSTRACT FROM AUTHOR]

In an effort to produce the materials of next‐generation photoelectronic devices, postsynthesis halide exchange reactions of perovskite quantum dots are explored to achieve enhanced bandgap tunability. However, comprehensive understanding of the multifaceted halide exchange reactions is inhibited by their vast relevant parameter space and complex reaction network. In this work, a facile room‐temperature strategy is presented for rapid halide exchange of inorganic perovskite quantum dots. A comprehensive understanding of the halide exchange reactions is provided by isolating reaction kinetics from precursor mixing rates utilizing a modular microfluidic platform, Quantum Dot Exchanger (QDExer). The effects of ligand composition and halide salt source on the rate and extent of the halide exchange reactions are illustrated. This fluidic platform offers a unique time‐ and material‐efficient approach for studies of solution phase‐processed colloidal nanocrystals beyond those studied here and may accelerate the discovery and optimization of next‐generation materials for energy technologies. [ABSTRACT FROM AUTHOR]