On the interplay of electronic and lattice screening on exciton binding in two-dimensional lead halide perovskites

Kavli Affiliate: David T. Limmer

| First 5 Authors: Rohit Rana, David T. Limmer, , ,

| Summary:

We use path integral Monte Carlo to study the energetics of excitons in
layered, hybrid organic-inorganic perovskites in order to elucidate the
relative contributions of dielectric confinement and electron-phonon coupling.
While the dielectric mismatch between polar perovskite layers and non-polar
ligand layers significantly increases the exciton binding energy relative to
their three dimensional bulk crystal counterparts, formation of exciton
polarons attenuates this effect. The contribution from polaron formation is
found to be a non-monotonic function of the lead halide layer thickness, which
is clarified by a general variational theory. Accounting for both of these
effects provides a description of exciton binding energies in good agreement
with experimental measurements. By studying isolated layers and stacked layered
crystals of various thicknesses, with ligands of varying polarity, we provide a
systematic understanding of the excitonic behavior of this class of materials
and how to engineer their photophysics.

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