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Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence.

ABSTRACT: Trap states play a crucial role in the design of colloidal quantum dot (QD)-based technologies. The presence of these in-gap states can either significantly limit the efficiency of devices (e.g., in solar cells or LEDs) or play a pivotal role in the functioning of the technology (e.g., in catalysis). Understanding the atomistic nature of traps is therefore of the highest importance. Although the mechanism through which undercoordinated chalcogenide atoms can lead to trap states in II-VI QDs is generally well understood, the nature of metal-based traps remains more elusive. Previous research has shown that reduction of metal sites in negatively charged QDs can lead to in-gap states. Here, we use density functional theory to show that metal-based traps are also formed in charge-neutral but photoexcited CdSe QDs. It is found that Cd-Cd dimers and the concomitant trap states are transient in nature and appear and disappear on the picosecond time scale. Subsequent nonradiative recombination from the trap is shown to be much faster than radiative recombination, indicating that dimer-related trap states can quench the photoluminescence. These results are expected to be transferable to other II-VI materials and highlight the importance of surface redox reactions for the optical properties of QDs. Moreover, they show that photoexcitation can lead to atomic rearrangements on the surface and thus create transient in-gap states.

SUBMITTER: du Fosse I

PROVIDER: S-EPMC8154315 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

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Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence.

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