<p></p><p>Hybrid organic-inorganic perovskites have
attracted immense interest as a promising material for a variety of optoelectronic
and sensing applications. However, issues regarding long-term stability have emerged
as the key bottleneck for applications and still require further study. Here, we
develop automated experimental workflow based on combinatorial synthesis and
rapid throughput characterization to explore long-term stability of these
materials in ambient conditions, and apply it to four model perovskite systems:
<a></a><a>MA<i><sub>x</sub></i>FA<i><sub>y</sub></i>Cs<sub>1-<i>x</i>-<i>y</i></sub>PbBr<sub>3</sub>,
MA<i><sub>x</sub></i>FA<i><sub>y</sub></i>Cs<sub>1-<i>x</i>-<i>y</i></sub>PbI<sub>3</sub>,
Cs<i><sub>x</sub></i>FA<i><sub>y</sub></i>MA<sub>1-<i>x</i>-<i>y</i></sub>Pb(Br<i><sub>x</sub></i><sub>+<i>y</i></sub>I<sub>1-<i>x</i>-<i>y</i></sub>)<sub>3</sub>
and Cs<i><sub>x</sub></i>MA<i><sub>y</sub></i>FA<sub>1-<i>x</i>-<i>y</i></sub>Pb(I<i><sub>x</sub></i><sub>+<i>y</i></sub>Br<sub>1-<i>x</i>-<i>y</i></sub>)<sub>3</sub></a>. We have both established a new
workflow and found out the main tendencies in the mixed cation and anion
systems, which led to the discovery of non-trivial composition regions with
high stability. The Non-negative Matrix Factorization and Gaussian
Process regression are used <i>to</i> <i>interpolate the photoluminescent
behavior of vast compositional space</i> and <i>to study the overall behavior
of the phase diagram</i>. This interpolative regression analysis helps to
distinguish mixtures that form solid solutions from those that segregate into
multiple materials, pointing out the most stable regions of the phase diagram. We find the
stability dependence on composition to be extremely non-uniform within the
composition space, suggesting the presence of potential preferential
compositional regions. <a>This proposed workflow is
universal and can be applied to other perovskite systems and
solution-processable materials. </a>Furthermore, incorporation of experimental
optimization methods, e.g., those based on Gaussian Processes, will enable the
transition from combinatorial synthesis to guide materials research and
optimization.</p><p></p>