Optical and Electronic Properties of Nonconcentric PbSe/CdSe Colloidal Quantum Dots

Lead chalcogenide colloidal quantum dots are attractive candidates for applications operating in the near infrared spectral range. However, their function is forestalled by limited stability under ambient conditions. Prolonged temperature-activated cation-exchange of Cd2+ for Pb2+ forms PbSe/CdSe core/shell heterostructures, unveiling a promising surface passivation route and a method to modify the dots' electronic properties. Here, we follow early stages of an-exchange process, using spectroscopic and structural characterization tools, as well as numerical calculations. We illustrate that preliminary-exchange stages involve the formation of nonconcentric heterostructures, presumably due to a facet selective reaction, showing a pronounced change in the optical properties upon the increase of the degree of nonconcentricity or/and plausible creation of core/shell interfacial alloying. However, progressive-exchange stages lead to rearrangement of the shell segment into uniform coverage, providing tolerance to oxygen exposure with a spectral steadiness already on the formation of a monolayer shell.