Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.063
Publication date: 18th December 2023
Future quantum technologies promise to deliver unprecedented computing power, secure communications and ultra-high precision measurements. A very promising way for realising these applications is via quantum optics, and single photon emitters are the key element of quantum optical technologies [1]. Among the various known methods for generating single photons, the use of optical transitions between quantum confined and isolated electronic states in semiconductor quantum dots (QDs) is one of the most promising approaches. Nowadays, after more than two decades of intensive development, epitaxial QDs have reached high fidelity performance; however, it appears that the best performance of these materials as quantum light sources is only achieved when operated at cryogenic temperatures. Instead, colloidal QDs have been much less explored as single photon emitters, but have the potential for operation beyond cryogenic temperatures (>4 K) due to stronger quantum confinement of carriers. Colloidal QDs can be synthesized in a variety of compositions, in particular metal chalcogenides such as CdSe, CdS, ZnSe, etc. and perovskite QDs are the most promising in terms of single photon emission properties. One of the fundamental technological difficulties for the realisation of single photon sources based on colloidal QDs is their slow decay rate at room temperature, since core-shell cadmium chalcogenide QDs have a typical lifetime in the range of tens of ns and perovskite QDs in the order of a few ns [2]. However, these lifetimes are too long to achieve ultrafast emission rates in the range of 100 Mph/s [1]. So far, various methods have been tried to increase the decay rate of colloidal QDs, e.g. by using a nanophotonic approach; experimental studies have shown an increase of the decay rate by a factor of 6 for a QD encapsulated in a plasmonic shell [3] and about 80 in plasmonic nanogaps [4] and patch antennas [5]. Another interesting method is based on exciton charging to enhance the QD emission rate itself, which can be realised by electrochemical or photochemical charge injection. Recent work by Morozov et al. [6] has shown a dramatic increase in the recombination rate for CdSe/CdS QDs using an electrochemical cell, from an initial lifetime of about 100-200 ns down to 1 ns at the highest applied voltage bias. Our study aims to exploit these results to further increase the room temperature decay rate of colloidal QDs by applying an exciton charging approach to CsPbBr3 perovskite QDs. Since perovskite QDs are not stable in polar solvents, an electrochemical method as used by Morozov et al. [6] cannot be applied here. For this reason, we investigate a novel approach based on a solid state device where an external electric field is applied directly to the perovskite QDs using a parent structure of a field effect transistor (FET) to generate highly charged excitons with a fast decay rate. Two alternative structures will be explored: one with an indium tin oxide (ITO) electrode to inject holes into the QDs, and the other with an aluminium layer to introduce electrons into the QDs. This will allow us to study the recombination of excitons in two different scenarios, the first with an excess of holes and the second with an excess of electrons. So far, we have investigated the performance of the device structure using a thin film of CsPbBr3 perovskite QDs. By applying a voltage bias to the device up to 40 V, we have observed a decrease in the lifetime of about 20% of the perovskite QDs that is reversible by returning to 0 V. These preliminary results are promising for moving on to the study of individual QDs.