Mapping Defect Relaxation in Quantum Dot Solids upon In Situ Heating.

Abstract

Epitaxially connected quantum dot solids have emerged as an interesting class of quantum confined materials with the potential for highly tunable electronic structures. Realization of the predicted emergent electronic properties has remained elusive due in part to defective interdot epitaxial connections. Thermal annealing has shown potential to eliminate such defects, but a direct understanding of this mechanism hinges on determining the nature of defects in the connections and how they respond to heating. Here, we use in situ heating in the scanning transmission electron microscope to probe the effect of heating on distinct defect types. We apply a real space, local strain mapping technique, which allows us to identify tensile and shear strain in the atomic lattice, highlighting tensile, shear, and bending defects in interdot connections. We also track the out-of-plane orientation of individual QDs and infer the prevalence of out-of-plane twisting and bending defects as a function of annealing. We find that tensile and shear defects are fully relaxed upon mild thermal annealing, while bending defects persist. Additionally, out-of-plane orientation tracking reveals an increase in correctly oriented QDs, pointing to a relaxation of either twisting defects or out-of-plane bending defects. While bending defects remain, highlighting the need for further study of orientational ordering during the preattachment phase of superlattice formation, these atomic-scale insights show that annealing can effectively eliminate tensile and shear defects, a promising step toward delocalization of charge carriers and tunable electronic properties.