Photoluminescence intermittency is a ubiquitous phenomenon, reducing the temporal emission intensity stability of single colloidal quantum dots (QDs) and the emission quantum yield of their ensembles. Despite efforts to achieve blinking reduction by chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate a deterministic all-optical suppression of QD blinking using a compound technique of visible and mid-infrared excitation. We show that moderate-field ultrafast mid-infrared pulses (5.5 μm, 150 fs) can switch the emission from a charged, low quantum yield grey trion state to the bright exciton state in CdSe/CdS core–shell QDs, resulting in a significant reduction of the QD intensity flicker. Quantum-tunnelling simulations suggest that the mid-infrared fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced photoluminescence intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials.
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The data that support the findings of this study are available from the corresponding author upon request.
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J.S., A.F., F.Y.G., Z.Z., U.B., A.P.W., K.A.N. and M.G.B. acknowledge support from the US Army Research Lab (ARL) and the US Army Research Office through the Institute for Soldier Nanotechnologies, under Cooperative Agreement number W911-NF-18-2-0048. W.S., H.U. and M.G.B. acknowledge support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (H.U. under award no. DE-FG02-07ER46454, W.S. and M.G.B under award nos DE-FG02-07ER46454 and DE-SC0021650). J.S., F.Y.G., Z.Z. and K.A.N. acknowledge additional support from the Samsung Global Outreach Program.
The authors declare no competing interests.
Peer review information Nature Nanotechnology thanks Efrat Lifshitz and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Notes 1–5, Figs. 1–17 and Table 1.
Supplementary Video 1
Video of MIR effects on CdSe/CdS QDs.
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Shi, J., Sun, W., Utzat, H. et al. All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses. Nat. Nanotechnol. 16, 1355–1361 (2021). https://doi.org/10.1038/s41565-021-01016-w
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