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All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses

Nature Nanotechnology volume 16, pages 1355–1361 (2021)Cite this article

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Abstract

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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Fig. 1: Experimental scheme and single dot verification.
Fig. 2: MIR blinking control in single QDs.
Fig. 3: MIR fields alter PL lifetime, blinking statistics and spectrum of single QDs.
Fig. 4: MIR responses of QDs with different shell thicknesses.
Fig. 5: Simulations and illustrations of the MIR-driven blinking control model.

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Data availability

The data that support the findings of this study are available from the corresponding author upon request.

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Acknowledgements

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.

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Author notes

  1. Hendrik Utzat

    Present address: Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

  2. These authors contributed equally: Jiaojian Shi, Weiwei Sun, Hendrik Utzat.

Authors and Affiliations

  1. Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA

    Jiaojian Shi, Weiwei Sun, Hendrik Utzat, Ardavan Farahvash, Frank Y. Gao, Zhuquan Zhang, Ulugbek Barotov, Adam P. Willard, Keith A. Nelson & Moungi G. Bawendi

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Contributions

J.S. and H.U. conceived the study and initiated the experiments. J.S., F.Y.G. and Z.Z. conducted and refined the infrared excitation measurements, developed the data acquisition and image processing software and analysed the experimental data. W.S. performed the solution biexciton experiments and contributed to data analysis and interpretation. A.F. (under the supervision of A.P.W.) performed the quantum-tunnelling simulations. U.B. synthesized CdSe/CdS QDs. J.S., W.S. and H.U. led the manuscript preparation. M.G.B. and K.A.N. supervised the project.

Corresponding authors

Correspondence to Keith A. Nelson or Moungi G. Bawendi.

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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 information

Supplementary Information

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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