Hybrid organic-inorganic perovskites (HOIPs) are now attracting significant attention as low-temperature depositable semiconductor materials with high (crystalline) structural precision. In particular, layered (so-called two-dimensional, 2D) HOIPs can be created by combining a wide range of possible inorganic components with an even broader range of organic molecules. The latter are functionalizable using the full arsenal of organic chemistry and thus offer considerable flexibility to fine-tune the synthesizability and properties of the eventual HOIP material. This talk focuses on computational predictions of the electronic (carrier, i.e., electron- and hole-like) energy levels of new 2D HOIP materials. Such predictions require rather high levels of theory and, for the large unit cells (hundreds of atoms) associated with typical 2D HOIPs, thus pose a considerable challenge. We here employ a combination of high-precision, all-electron hybrid density functional theory with a recent implementation of spin-orbit coupling, showing that this combination provides descriptions of the quantum-well like energy level alignment in lead halide based oligothiophene pwerovskites in excellent agreement with experiments. We then employ the same approach to predictively address the electronic properties of a broad range of further 2D HOIPs, including lead-free (Ag-Bi) based ones and chiral perovskites in which Rashba splitting can be introduced in the conduction bands. As a final point, we show that the details of the atomic structure used to predict electronic properties matter significantly, even in a qualitative sense, by determining energy level alignments and, therefore, which component (organic or inorganic) forms the band edges. Overall, a complete structural understanding of a given target 2D HOIP is thus essential for faithfully predicting the properties that can be leveraged within this promising new semiconductor materials space.

Tunable electronic structure of 2D hybrid organic-inorganic perovskites from a first principles approach

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.