DOI: https://doi.org/10.29363/nanoge.hpatom.2022.009
Publication date: 30th October 2021
In this talk, taking inspiration from the hierarchical organization of nature, we describe a hierarchical approach to materials engineering of organic metal-halide semiconductors. We demonstrate that organo-metal halide semiconductors’ dimensionality, composition, and morphology dictate their optoelectronic properties and can be exploited in defining more explicit relationships between structure and function. Here, we traverse three-dimensional (3D), two-dimensional (2D), and one-dimensional (1D) organo-metal halide semiconductors, detailing the morphological and compositional differences in each and the implications that can be drawn within each domain on the engineering process. Control over ion migration pathways via morphology engineering as well as control over charge formation in organic–inorganic semiconductors is demonstrated. Fundamental insights into the amount of static and dynamic disorder in the MHP lattice are provided, which can be continuously tuned as a function of composition and morphology. Using electroabsorption spectroscopy on 2D MHPs, a disorder-induced dipole moment in the exciton proportional to the summed value of static and dynamic disorder is measured. Spectroscopic isolation of exciton features in 2D MHP electroabsorption spectra allows us to obtain precise, model-independent measurements of exciton binding energies to study the effect of chemical substitutions, such as Sn2+ → Pb2+, on the value of the exciton binding energy. Finally, we conclude that this multidimensional platform will be foundational in accurately predicting structure–property–device relationships in organo-metal halide semiconductors in the future.
This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-SC0019041. L.W.B. would also like to acknowledge the Sloan Foundation through an Alfred P. Sloan Research Fellowship in Chemistry, The Dreyfus Foundation through a Dreyfus Teacher Scholar Award, and the Research Corporation for Science Advancement through a Cottrell Scholar Award.
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