Screening of Excitons by Organic Cations in Quasi-Two-Dimensional Organic-Inorganic Lead-Halide Perovskites

Interlayer organic cations in quasi-two-dimensional halide perovskites are a versatile tuning vehicle for the optoelectronic properties of these complex systems, but chemical intuition for this design route is yet to be established. Here, we use density functional theory, the GW approximation, and the Bethe-Salpeter equation approach to understand the contribution of the organic cation to the quasiparticle band gap and exciton binding energy of layered perovskites. We show that organic cations in quasi-twodimensional perovskites contribute significantly to the dielectric screening in these systems, countering quantum confinement effects on the quasiparticle band gap and the exciton binding energy. Using a simple electrostatics model inspired by parallel-plate capacitors, we decouple the organic cation and inorganic layer contributions to the effective dielectric constants and show that dielectric properties of layered perovskites are broadly tunable via the interlayer cation, providing a direct means of tuning photophysical properties for a variety of applications.

Automated summary

Interlayer organic cations play a crucial role in tuning the optoelectronic properties of quasi-two-dimensional halide perovskites, and their effects can be controlled by adjusting the dielectric properties.