Variational Photocarrier Radiometry Reconstruction of Exciton Lifetime Spectra for a Coupled PbS Colloidal Quantum Dot Thin Film Under Combined AC and DC Laser Excitation

Abstract

Colloidal quantum dots (CQDs) have attracted significant interest for applications in electronic and optoelectronic devices such as photodetectors, light emitting diodes, and solar cells. However, a poor understanding of charge transport in these nanocrystalline films hinders their practical applications. The photocarrier radiometry (PCR) technique, a frequency-domain photoluminescence method spectrally gated for radiative recombination photon emissions and exclusion of thermal infrared photons, has been applied to a coupled PbS CQD thin film with inter-dot spacing of 0.5 nm to 1 nm for the analysis of charge transport properties. As the nanoparticle bandgap depends on the size of the quantum dots, polydispersity of the CQD thin film causes bandgap variability leading to photoexcited carrier (exciton) decay lifetime broadening and temperature dependence. The carrier transport mechanisms of QDs are quite different from bulk semiconductors, so the conventional carrier-diffusion wave-based PCR theory was modified into a non-diffusive limit model. A developed variational discrete lifetime reconstruction approach was used to analyze PCR frequency scans under two optical excitation modes: a modulated laser source without, and with, an additional continuous laser source. Using this model, the CQD mean lifetime values were found and variational discrete lifetime spectra were reconstructed.