Journal
ACS NANO
Volume 13, Issue 9, Pages 10745-10753Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b05504
Keywords
2D materials; optical constants; momentum-resolved; electric dipoles; optical anisotropies; effective medium; hybrid perovskites
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC-0012541]
- National Science Foundation [DMR-1454260, OIA- 1538893]
- Air Force Office of Scientific Research [FA9550-16-1-0393]
- National Defense Science and Engineering Graduate fellowship
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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.
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