Size-dependent Dielectric Permittivity of Perovskite Nanocrystals

TL;DR

This paper presents a method to determine the size-dependent dielectric permittivity of individual perovskite nanocrystals from ensemble absorbance spectra, enabling better design of quantum photonic devices.

Contribution

The authors develop a novel approach combining spectral fitting and effective medium theory to extract intrinsic permittivity of single nanocrystals from ensemble measurements.

Findings

Successfully reconstructed size-dependent permittivity of CsPbBr3 PNCs.

Demonstrated consistency with single nanocrystal emission linewidths.

Showed enhanced absorption when coupled with nanoantennas.

Abstract

Perovskite nanocrystals (PNCs) are promising building blocks for quantum photonic devices. Optical properties of PNCs can be enhanced by integration with optical cavities or nanoantennas. Designing such structures requires accurate size dependent dielectric permittivity of PNCs. However, current reports provide primarily ensemble averaged values with limited access to the intrinsic response of individual PNCs. Here we suggest a methodology to reconstruct the size dependent complex dielectric permittivity of CsPbBr3 PNCs from the measured absorbance spectrum of colloidal solution. The permittivity of PNCs is modeled as a sum of Voigt profile oscillators, with the size dependent transition energies governed by the exciton effective mass. Using a transmission electron microscopy derived size distribution of the PNCs, the solution permittivity is obtained via Maxwell Garnett effective medium approximation. This permittivity is used in a transfer matrix method to simulate and fit the absorbance spectrum, from which the permittivity of PNCs is reconstructed. The extracted spectral linewidth from the imaginary part of the permittivity (78.4 meV) is consistent with single nanocrystal emission linewidths at room temperature. Finite element simulations show enhanced absorption cross section of a single PNC coupled to a nanoantenna, demonstrating applicability of the extracted permittivity. More generally, these findings provide a route to extract intrinsic permittivity of individual nanocrystals from absorbance measurements of their ensembles.