Semiconductor colloidal quantum dots (CQDs) are being increasingly exploited in electronics, optoelectronics and solar energy harvesting, using a variety of different architectures, mostly based on ordered 2D or 3D arrays of these nanostructures.A crucial issue for optimising the performance of such devices is the ability to predict and tune the transport properties of these assemblies. In this work we provide general guidelines to precisely that effect, indicating specific materials, crystal structures, lattice arrangements, surface stoichiometries and morphologies which favour high electron mobilities in these systems, and, conversely, materials that will exhibit low mobilities if nanostructured. At the same time our results evidence a surprising independence of the film's transport properties from those of the bulk material from which the dots are made, highlighting the crucial role of theoretical modelling to guide device design.
Keywords: transport, nanocrystal quantum dots, films, dot arrays, pseudopotential methodColloidal quantum dots (CQDs) are attractive material systems characterized by outstanding properties, such as low manufacturing costs, high degree of uniformity and flexibility achieved in their synthesis, size-tunability of their electronic and optical properties, and even the ability to engineer their wave functions, enabling unprecedented control of the carriers' localization, that make them potentially ideally suited for a wide range of technological applications. Nevertheless the performance of CQD-based electronic and optoelectronic devices is still far from optimal, owing mainly to the poor transport properties displayed by their building blocks when arranged in arrays. The presence of countless interfaces, with associated traps 1 and potential steps, that the charge carriers need to cross in order to reach the electrodes where they can be collected, appears a daunting obstacle to efficient transport in these devices. Indeed measurements on early devices seemed to confirm this bleak scenario, and very low mobilities (of the order of 10 −2 cm 2 V −1 s −1 or less) were reported in CQD films. 2-5 These findings were supported by