The significant performance
increase in nanocrystal (NC)-based
solar cells over the last decade is very encouraging. However, many
of these gains have been achieved by trial-and-error optimization,
and a systematic understanding of what limits the device performance
is lacking. In parallel, experimental and computational techniques
provide increasing insights into the electronic properties of individual
NCs and their assemblies in thin films. Here, we utilize these insights
to parameterize drift–diffusion simulations of PbS NC solar
cells, which enable us to track the distribution of charge carriers
in the device and quantify recombination dynamics, which limit the
device performance. We simulate both Schottky- and heterojunction-type
devices and, through temperature-dependent measurements in the light
and dark, experimentally validate the appropriateness of the parameterization.
The results reveal that Schottky-type devices are limited by surface
recombination between the PbS and aluminum contact, while heterojunction
devices are currently limited by NC dopants and electronic defects
in the PbS layer. The simulations highlight a number of opportunities
for further performance enhancement, including the reduction of dopants
in the nanocrystal active layer, the control over doping and electronic
structure in electron- and hole-blocking layers (e.g., ZnO), and the
optimization of the interfaces to improve the band alignment and reduce
surface recombination. For example, reduction in the percentage of
p-type NCs from the current 1–0.01% in the heterojunction device
can lead to a 25% percent increase in the power conversion efficiency.