Structure-transport correlation reveals anisotropic charge transport in coupled PbS nanocrystal superlattices

Semiconductive nanocrystals (NCs) can be self-assembled into ordered superlattices (SLs) to create artificial solids with emerging collective properties. Computational studies have predicted that properties such as electronic coupling or charge transport are determined not only by the individual NCs but also by the degree of their organization and structure. However, experimental proof for a correlation between structure and charge transport in NC SLs is still pending. Here, we perform X-ray nano-diffraction and apply Angular X-ray Cross-Correlation Analysis (AXCCA) to characterize the structures of coupled PbS NC SLs, which are directly correlated with the electronic properties of the same SL microdomains. We find strong evidence for the effect of SL crystallinity on charge transport and reveal anisotropic charge transport in highly ordered monocrystalline hexagonal close-packed PbS NC SLs, caused by the dominant effect of shortest interparticle distance. This implies that transport anisotropy should be a general feature of weakly coupled NC SLs.
Comment: 49 pages, 20 Figures