Colloidal quantum dots (QDs) are vital fluorescent probes with several optical features superior to those found in organic dyes for microscopy imaging. However, the emission blinking behavior of a single QD is an intrinsic drawback for stimulated emission depletion microscopy (STED) or structured illumination microscopy techniques. Herein, we present a rational strategy for the synthesis of a type of deterministic, environmentally friendly, small nonblinking core–multishell InP/ZnSe/ZnS QD using a hydrofluoric acid (HF) etching passivation. The strategy includes four steps: synthesis of the InP core, synthesis of oil-phase core–multishell InP/ZnSe/ZnS QDs using hydrogen fluoride and trioctylphosphine etching passivation, promotion of the water solubility of QDs modified by 3-mercaptopropionic acid (MPA), and enhanced biotargeting of core–multishell InP/ZnSe/ZnS QDs by surface coupling technology. The suppressed blinking mechanism was primarily attributed to surface wrapping shells and HF etching passivation of surface dangling bonds, which reduced surface nonradiative recombination. Nonblinking QDs exhibit high fluorescence efficiency (∼90%), good photostability (>20 min), a large Stokes shift (>135 nm), biocompatibility of the cell viability (>90%), and high targeting. Furthermore, super-resolution multifocal structured illumination microscopy imaging of subcellular structures labeled using these QDs confirmed a resolution improvement of greater than 2.6-fold compared to wide-field microscopy. The results indicate that the nonblinking QDs can function as excellent probes for use in the long-term super-resolution visualization of subcellular dynamics.
Wei Fu,Jiefu Yin,Huaqiang Cao,Zhongfu Zhou,Junying Zhang,Jingjing Fu,Jamie H. Warner,Cheng Wang,Xiaofang Jia,G. Neville Greaves,Anthony K. Cheetham
Photoluminescence blinking behavior from single quantum dots under steady illumination is an important but controversial topic. Its occurrence has impeded the use of single quantum dots in bioimaging. Different mechanisms have been proposed to account for it, although controversial, the most important of which is the non-radiative Auger recombination mechanism whereby photocharging of quantum dots can lead to the blinking phenomenon. Here, the singly charged trion, which maintains photon emission, including radiative recombination and non-radiative Auger recombination, leads to fluorescence non-blinking which is observed in photocharged single graphene quantum dots (GQDs). This phenomenon can be explained in terms of different energy levels in the GQDs, caused by various oxygen-containing functional groups in the single GQDs. The suppressed blinking is due to the filling of trap sites owing to a Coulomb blockade. These results provide a profound understanding of the special optical properties of GQDs, affording a reference for further in-depth research.
Single-molecular spectroscopy reveals that photoluminescence (PL) of a single quantum dot blinks, randomly switching between bright and dim/dark states under constant photoexcitation, and quantum dots photobleach readily. These facts cast great doubts on potential applications of these promising emitters. After ∼20 years of efforts, synthesis of nonblinking quantum dots is still challenging, with nonblinking quantum dots only available in red-emitting window. Here we report synthesis of nonblinking quantum dots covering most part of the visible window using a new synthetic strategy, i.e., confining the excited-state wave functions of the core/shell quantum dots within the core quantum dot and its inner shells (≤ ∼5 monolayers). For the red-emitting ones, the new synthetic strategy yields nonblinking quantum dots with small sizes (∼8 nm in diameter) and improved nonblinking properties. These new nonblinking quantum dots are found to be antibleaching. Results further imply that the PL blinking and photobleaching of quantum dots are likely related to each other.
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