RESUMEN

Plentiful research of InP semiconductor quantum dots (QDs) has been launched over the past few decades for their excellent photoluminescence properties and environmentally friendly characteristics in various applications. However, InP QDs show inferior photostability because they are extremely sensitive to the ambient environment. In this study, we propose a novel method to enhance the photostability of InP/ZnSe/ZnS QDs by doping zirconium into the ZnS layer. We certify that Zr can be oxidized to Zr oxides, which can prevent the QDs from suffering oxidation during light irradiation. The InP/ZnSe/ZnS:Zr QDs maintained 78% of the original photoluminescence quantum yields without significant photodegradation under the irradiation of LED light (450 nm, 3.0 W power intensity) for 14 h, while conventional InP/ZnSe/ZnS QDs dramatically decreased to 29%.

RESUMEN

The excellent performance of InP/ZnSe/ZnS core/shell/shell quantum dots (CSS-QDs) in light-emitting diodes benefits from the introduction of a ZnSe midshell. Understanding the changes of ultrafast carrier dynamics caused by the ZnSe midshell is important for their optoelectronic applications. Herein, we have compared the ultrafast carrier dynamics in CSS-QDs and InP/ZnS core/shell QDs (CS-QDs) using femtosecond transient absorption spectroscopy. The results show that the ZnSe midshell intensifies the electron delocalization and prolongs the in-band relaxation time of electrons from 238 fs to 350 fs, and that of holes from hundreds of femtoseconds to 1.6 ps. We also found that the trapping time caused by deep defects increased from 25.6 ps to 76 ps, and there were significantly reduced defect emissions in CSS-QDs. Moreover, the ZnSe midshell leads to a significantly increased density of higher-energy hole states above the valence band-edge, which may reduce the probability of Auger recombination caused by the positive trion. This work enhances our understanding of the excellent performance of the CSS-QDs applied to light-emitting diodes, and is likely to be helpful for the further optimization and design of optoelectronic devices based on the CSS-QDs.

RESUMEN

Isotropic InP/ZnSe/ZnS quantum dots (QDs) are prepared at a high reaction temperature, which facilitates ZnSe shell growth on random facets of the InP core. Fast crystal growth enables stacking faults elimination, which induces anisotropic growth, and as a result, improves the photoluminescence (PL) quantum yield by nearly 20%. Herein, the effect of the QD morphology on photophysical properties is investigated by observing the PL blinking and ultrafast charge carrier dynamics. It is found that hot hole trapping is considerably suppressed in isotropic InP QDs, indicating that the stacking faults in the anisotropic InP/ZnSe structures act as defects for luminescence. These results highlight the importance of understanding the correlation between QD shapes and hot carrier dynamics, and present a way to design highly luminescent QDs for further promising display applications.

RESUMEN

Non-toxic InP-based nanocrystals have been developed for promising candidates for commercial optoelectronic applications and they still require further improvement on photophysical properties, compared to Cd-based quantum dots (QDs), for better device efficiency and long-term stability. It is, therefore, essential to understand the precise mechanism of carrier trapping even in the state-of-the-art InP-based QD with near-unity luminescence. Here, it is shown that using time-resolved spectroscopic measurements of systematically size-controlled InP/ZnSe/ZnS core/shell/shell QDs with the quantum yield close to one, carrier trapping decreases with increasing the energy difference between band-edge and trap states, indicating that the process follows the energy gap law, well known in molecular photochemistry for nonradiative internal conversion between two electronic states. Similar to the molecular view of the energy gap law, it is found that the energy gap between the band-edge and trap states is closely associated with ZnSe phonons that assist carrier trapping into defects in highly luminescent InP/ZnSe/ZnS QDs. These findings represent a striking departure from the generally accepted view of carrier trapping mechanism in QDs in the Marcus normal region, providing a step forward understanding how excitons in nanocrystals interact with traps, and offering valuable guidance for making highly efficient and stable InP-based QDs.

Asunto(s)

RESUMEN

Upon demonstrating self-luminescing quantum dot based light-emitting devices (QD-LEDs), rapid Auger recombination acts as one of the performance limiting factors. Here, we report the Auger processes of highly luminescent InP/ZnSe/ZnS QDs with different midshell structures that affect the performances of QD-LEDs. Transient PL measurements reveal that exciton-exciton binding energy is dependent on the midshell thickness, which implies that the intercarrier Coulomb interaction caused by the introduction of excess charges may come under the influence of midshell thickness which is in contrast with the nearly stationary single exciton behavior. Photochemical electron-doping and optical measurements of a single QD show that negative trion Auger recombination exhibits strong correlation with midshell thickness, which is supported by the dynamics of a hot electron generated in the midshell. These results highlight the role of excess electrons and the effects of engineered shell structures in InP/ZnSe/ZnS QDs, which eventually determine the Auger recombination and QD-LED performances.

RESUMEN

The effects of the ZnS shell layer on the memory performances of flexible memristive devices based on quantum dots (QDs) with an InP/ZnSe/ZnS core-multishell structure embedded in a poly(methylmethacrylate) layer were investigated. The on/off ratios of the devices based on QDs with an InP/ZnSe core-shell structure and with an InP/ZnSe/ZnS core-multishell structure were approximately 4.2 × 102 and 8.5 × 103, respectively, indicative of enhanced charge storage capability in the latter. After bending, the memory characteristics of the memristive devices based on QDs with the InP/ZnSe/ZnS structure were similar to those before bending. In addition, those devices maintained the same on/off ratios for retention time of 1 × 104 s, and the number of endurance cycles was above 1 × 102. The reset voltages ranged from -2.3 to -3.1 V, and the set voltages ranged from 1.3 to 2.1 V, indicative of reliable electrical characteristics. Furthermore, the possible operating mechanisms of the devices are presented on the basis of the electron trapping and release mode.