Layered, so-called "2D" hybrid organic-inorganic perovskites (HOIPs) are the focus of a very large community as tunable semiconductor materials, by using selective organic and/or inorganic substitutions to control phenomena such as the band gap, absorption and emission, or spin selective transport. While the materials feature crystallographic supercell sizes of several hundred atoms, high-level first principles calculations are now able to predictively capture the important electronic features, importantly including functional characteristics such as Rashba-Dresselhaus (RD) splitting to manipulate the spin characteristics of the associated energy bands. This work shows how hybrid density functional theory including spin-orbit coupling, a rather demanding but appropriate level of theory for energy band structures, can be employed to predict the quantum-well nature of different materials, the impact of detailed molecular conformation, and the presence, absence and/or strength of RD splitting as a consequence of symmetry breaking elements, particularly chiral molecules. We finally demonstrate the feasibility of studying much larger unit cells at the same level of theory, containing deliberately introduced defects to understand their impact as dopants in layered HOIPs.

Tuning the electronic structure of layered hybrid organic-inorganic perovskites from first principles

ACS Spring Meeting 2021

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