Version 2 2022-04-19, 18:15Version 2 2022-04-19, 18:15
Version 1 2019-09-10, 13:35Version 1 2019-09-10, 13:35
dataset
posted on 2022-04-19, 18:15authored byRyan A. DeCrescent, Naveen R. Venkatesan, Clayton J. Dahlman, Rhiannon M. Kennard, Michael L. Chabinyc, Jon A. Schuller
Hybrid organic/inorganic perovskites (HOIPs) are of great interest
for optoelectronic applications due to their quality electronic and
optical properties and the exceptional ease of room-temperature synthesis.
Layered HOIP structures, e.g., Ruddlesden–Popper
phases, offer additional synthetic means to define self-assembling
multiple quantum well structures. Measurements of Ruddlesden–Popper
HOIP optical constants are currently lacking, but are critical for
both a fundamental understanding as well as optoelectronic device
design. Here, we use momentum-resolved optical techniques to measure
error-constrained complex uniaxial optical constants of layered lead-iodide
perovskites incorporating a variety of organic spacer molecules. We
demonstrate how large optical anisotropies measured in these materials
arise primarily from classical dielectric inhomogeneities rather than
the two-dimensional nature of the electronic states. We subsequently
show how variations among these materials can be understood within
a classical effective-medium model that accounts for dielectric inhomogeneity.
We find agreement between experimentally inferred dielectric properties
and quantum-mechanical calculations only after accounting for these
purely classical effects. This work provides a library of optical
constants for this class of materials and clarifies the origins of
large absorption and photoluminescence anisotropies witnessed in these
and other layered nanomaterials.