2:45 PM - CH04.13.07
High-Throughput Study of Antisolvents on the Stability of Multicomponent Metal Halide Perovskites Through Robotics-Based Synthesis and Machine Learning Approaches
Mahshid Ahmadi1,Kate Higgins1,Maxim A. Ziatdinov2,Sergei Kalinin2
University of Tennessee, Knoxville1,Oak Ridge National Laboratory2
Considerable research attention has focused on metal halide perovskites (MHPs) over the recent years because of the combination of exceptional optoelectronic properties and low fabrication cost, making them ideal candidates for a variety of applications1-4. Even so, the development of MHPs for commercialization must overcome an obstacle, namely stability in the pure or device-integrated form5. Overcoming adverse effects stemming from external stimuli can be minimized or avoided by utilizing established encapsulation techniques and device engineering6,7. Simultaneously, another strategy is to improve the intrinsic stability by cation and/or halide alloying to synthesis multicomponent MHPs8,9. A multitude of studies have demonstrated how the incorporation of other cations, particularly Cs+ and formamidinium (FA+) into methylammonium (MA+) systems, leads to improve stability in ambient and operational conditions. Mixing halides, has also proven to be an effective strategy toward stable perovskite materials.
Antisolvent crystallization methods are frequently used to fabricate high quality perovskite thin films, to produce sizable single crystals, and to synthesize nanoparticles at room temperature. However, a systematic exploration of the effect of specific antisolvents on the intrinsic stability of multicomponent metal halide perovskites has yet to be demonstrated. We have previously reported the development of a workflow for materials discovery utilizing both automated synthesis and machine learning (ML)10,11. Similarly in this study, we develop a high-throughput experimental workflow that incorporates robotic synthesis, automated characterization, and ML techniques to explore how the choice of antisolvent affects the intrinsic stability of binary perovskite systems in ambient conditions12. Different combinations of the endmembers are used to synthesize 15 combinatorial libraries, each with 96 unique combinations. In total, roughly 1100 different compositions are synthesized. Each library is fabricated twice using two different antisolvents: toluene and chloroform. Once synthesized, photoluminescence spectroscopy is automatically performed every 5 minutes for approximately 6 hrs. Non-negative Matrix Factorization (NMF) is then utilized to map the time- and compositional-dependent optoelectronic properties. Through the utilization of this workflow for each library, we demonstrate that the selection of antisolvent is critical to the stability of MHPs in ambient conditions. We explore possible dynamical processes, such as halide segregation, responsible for either the stability or eventual degradation as caused by the choice of antisolvent. Overall, this high-throughput study demonstrates the vital role that antisolvents play in the synthesis of high quality multicomponent MHP systems.
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