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Autonomous Microfluidic Synthesis of Metal Cation-Doped Perovskite Quantum Dots
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Autonomous Microfluidic Synthesis of Metal Cation-Doped Perovskite Quantum Dots
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Autonomous Microfluidic Synthesis of Metal Cation-Doped Perovskite Quantum Dots
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Dissertation
Autonomous Microfluidic Synthesis of Metal Cation-Doped Perovskite Quantum Dots
2023
Overview
Lead halide perovskite (LHP) quantum dots (QDs) have emerged as highly promising foundational nanomaterials for advanced energy and optoelectronic applications. This PhD thesis undertakes an extensive fundamental and applied studies of impurity metal cation doping of LHP QDs using modular microfluidic platform integrated with in-situcharacterization probes and assisted with machine learning tools. The PhD thesis presents the development and deployment of a self-driving fluidic lab (SDFL) for accelerated discovery, development, optimization, and fundamental mechanistic studies of metal cation-doped LHP QDs. We further leverage the reconfigurability of SDFLs to enable facile transition from fast-tracked parameter space navigation to on-demand continuous manufacturing of QDs. This PhD thesis encompasses QD synthesis and metal-cation doping chemistries operating at both room and high reaction temperatures, unlocking new possibilities for tailored material properties and applications.The first specific aim of this PhD thesis studies flow chemistry strategies for metal cation doping in LHP QDs. We then utilize the developed flow chemistry approach for funadametnal mechanistic studies of room-temperature manganese (Mn2+) doping of CsPbCl3 QDs by employing an automated modular microfluidic platform. This study is the first report of ultrafast metal-cation doping of LHP QDs at room temperature. Through real-time monitoring of the QD optical properties, we elucidate the kinetics and mechanism of a post-synthetic room-temperature metal cation doping process, enabling precise emission properties tuning of Mn-doped CsPbCl3 QDs through in-flow concentration adjustments of MnCl2 as the Mn2+ ion source. Leveraging the exceptional time resolution of monitoring the LHP QD doping process (as low as 60 ms), enabled by the microfluidic platform, we unveil a two-stage heterogeneous surface doping mechanism facilitated by vacancy-assisted migration of metal cations. Additionally, we utilize the room-temperature metal-cation doping chemistry for ultrafast continuous nanomanufacturing of Mn-doped CsPbCl3QDs. The results of the first specific aim of this PhD thesis enabled the development of an automated and modular flow chemistry platform for reproducible and precise synthesis of colloidal QDs, serving as the core physical infrastructure of SDFLs.The second specific aim of this PhD study, building upon the progress of the first specific aim, investigates integration of machine learning with flow chemistry to build an SDFL for autonomous development of metal-cation-doped LHP QDs via a sequential halide exchange and metal cation doping of LHP QDs using room-temperature chemistries. By integrating the modular flow chemistry platform with a Bayesian framework, we demonstrate constructing a digital twin of the two-stage halide exchange and metal-cation doping of CsPbBr3 QDs for fundamental mechanistic studies. Next, we utilize the digital twin as a surrogate model for ondemand tuning of the LHP QD properties and metal-cation doping level. The developed SDFL accelerates navigation through the multivariate reaction space of the synthesis and metal-cation doping of LHP QDs.In order to further enhance the quality of metal cation-doped LHP QDs, there exists a compelling need to explore and establish flow chemistry synthetic routes operating at high temperatures. Thus, the third specific aim of this PhD thesis focuses on the establishment of an SDFL for one-pot high-temperature metal-cation doping of LHP QDs. In the third specific aim of this PhD thesis, we unveil Smart Dope, that is a self-driving fluidic lab for autonomous hightemperature synthesis, development, and manufacturing of multi cation-doped LHP QDs.
