Monolayer suppression of transport imaged in annealed PbSe nanocrystal arrays

We use correlated electrostatic force, transmission electron, and atomic force microscopy (EFM, TEM, and AFM) to visualize charge transport in monolayers and up to five layers of PbSe nanocrystal arrays drop-cast on electrode devices. Charge imaging reveals that current paths are dependent on the locally varying thickness and continuity of an array. Nanocrystal monolayers show suppressed conduction compared to bilayers and other multilayers, suggesting a departure from linear scaling of conductivity with array thickness. Moreover, multilayer regions appear electrically isolated if connected solely by a monolayer. Partial suppression is also observed within multilayer regions that contain narrow junctions only several nanocrystals wide. High-resolution TEM structural imaging of the measured devices reveals a larger reduction of inter-nanocrystal spacing in multilayers compared to monolayers upon vacuum-annealing, offering a likely explanation for the difference in conductivity between these two cases. This restriction of transport by monolayers and narrow junctions is an important factor that must be addressed in future designs of optoelectronic devices based on nanocrystals.