From colloidal CdSe quantum dots to microscale optically anisotropic supercrystals through bottom-up self-assembly

This is the author accepted manuscript. The final version is available on open access from Royal Society of Chemistry via the DOI in this recordThe development of fabrication techniques for novel nanostructured materials is one of the key tasks of modern materials science. One pathway to successfully complete this task is the bottom-up assembly of colloidal nanoparticles into ordered superstructures, possessing both the properties of individual nanoparticles and further novel properties resulting from their interactions. However, nanoparticle self-assembly depends on a variety of parameters, which makes the precise control of this process a complicated problem. Here, the time course of quantum dot (QD) self-assembly into ordered superstructures has been analyzed, along with the evolution of their morphological and optical properties. QD self-assembly occurs through two distinct stages (homo- and hetero-geneous), leading to the formation of supercrystals with a layered morphology. Analysis of the optical properties throughout the superstructures’ growth has shown that the absorption and photoluminescence (PL) bands are blue shifted, retaining almost the same PL lifetimes as in the initial QD solution. The supercrystals formed possess a further unique optical property caused by their layered morphology; namely, a four-fold symmetry characterized by strong birefringence. Such supercrystals may be used for the fabrication of microscale optical paths with high extinction coefficients and specific polarization properties for novel optoelectronic devices.This study was supported by the Ministry of Education and Science of the Russian Federation through the grant No. 14.584.21.0032 (ID RFMEFI58417X0032), the Engineering and Physical Sciences Research Council (EPSRC) of the United Kingdom via the EPSRC Centre for Doctoral Training in Electromagnetic Metamaterials (Grant No. EP/L015331/1) and via EP/N035569/1, and the Royal Society via International Exchange Grant No. 2016/R1