Semiconductor colloidal quantum dots (CQDs) have attracted vast scientific and technological interest throughout the past three decades, due to the unique tuneability of their optoelectronic properties by variation of size and composition. However, the nanoscale size brings about a large surface-to-bulk volume ratio, where exterior surfaces have a pronounced influence on the chemical stability and on the physical properties of the semiconductor. Therefore, numerous approaches have been developed to gain efficient surface passivation, including a coverage by organic or inorganic molecular surfactants as well as the formation of core/shell heterostructures (a semiconductor core epitaxially covered by another semiconductor shell). This review focuses on special designs of core/shell heterostructures from the IV-VI and II-VI semiconductor compounds, and on synthetic approaches and characterization of the optical properties. Experimental observations revealed the formation of core/shell structures with type-I or quasi-type-II band alignment between the core and shell constituents. Theoretical calculations of the electronic band structures, which were also confirmed by experimental work, exposed surplus electronic tuning (beyond the radial diameter) with adaptation of the composition and control of the interface properties. The studies also considered strain effects that are created between two different semiconductors. It was disclosed experimentally and theoretically that the strain can be released via the formation of alloys at the core-shell interface. Overall, the core/shell and core/alloyed-shell heterostructures showed enhancement in luminescence quantum efficiency with respect to that of pure cores, extended lifetime, uniformity in size and in many cases good chemical sustainability under ambient conditions.
Quantum dot (QD) solids and arrays hold a great potential for novel applications which are aimed at exploiting quantum properties in room-temperature devices. Careful tailoring of the QD energy levels and coupling between dots could lead to efficient energy-harvesting devices. Here, we used a self-assembly method to create a disordered layered structure of QDs, coupled by covalently bonded organic molecules. Energy transfer rates from small (donor) to large (acceptor) QDs are measured. Best tailoring of the QDs energy levels and the length of the linking molecules results in an energy transfer rate as high as 30 ps–1. Such rates approach energy transfer rates of the highly efficient photosynthesis complexes and are compatible with a coherent mechanism of energy transfer. These results may pave way for new controllable building blocks for future technologies.
The rates of elementary photophysical processes in nanocrystals, such as carrier cooling, multiexciton generation, Auger recombination etc., are determined by monitoring the transient occupation of the lowest exciton band. The underlying assumption is that hot carriers relax rapidly to their lowest quantum level. Using femtosecond transient absorption spectroscopy in CdSe/CdS nanodots we challenge this assumption. Results show, that in nanodots containing a preexisting cold "spectator exciton", only half of the photoexcited electrons relax directly to the band-edge and the rest are blocked in an excited state due to Pauli exclusion. Full relaxation occurs only after˜15 ps, as the blocked electrons flip spin. This requires review of numerous studies unaware of this ubiquitous and novel effect, which may facilitate hot carrier energy utilization as well.arXiv:1809.08581v2 [cond-mat.mes-hall]
The incorporation of magnetic impurities into semiconductor nanocrystals with size confinement promotes enhanced spin exchange interaction between photogenerated carriers and the guest spins. This interaction stimulates new magnetooptical properties with significant advantages for emerging spin-based technologies. Here we observe and elaborate on carrier−guest interactions in magnetically doped colloidal nanoplatelets with the chemical formula CdSe/Cd 1−x Mn x S, explored by optically detected magnetic resonance and magneto-photoluminescence spectroscopy. The host matrix, with a quasi-type II electronic configuration, introduces a dominant interaction between a photogenerated electron and a magnetic dopant. Furthermore, the data convincingly presents the interaction between an electron and nuclear spins of the doped ions located at neighboring surroundings, with consequent influence on the carrier's spin relaxation time. The nuclear spin contribution by the magnetic dopants in colloidal nanoplatelets is considered here for the first time.
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