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Electric-field-induced colour switching in colloidal quantum dot molecules at room temperature

Nature Materials volume 22, pages 1210–1217 (2023)Cite this article

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Abstract

Colloidal semiconductor quantum dots are robust emitters implemented in numerous prototype and commercial optoelectronic devices. However, active fluorescence colour tuning, achieved so far by electric-field-induced Stark effect, has been limited to a small spectral range, and accompanied by intensity reduction due to the electron–hole charge separation effect. Utilizing quantum dot molecules that manifest two coupled emission centres, we present a unique electric-field-induced instantaneous colour-switching effect. Reversible emission colour switching without intensity loss is achieved on a single-particle level, as corroborated by correlated electron microscopy imaging. Simulations establish that this is due to the electron wavefunction toggling between the two centres, induced by the electric field, and affected by the coupling strength. Quantum dot molecules manifesting two coupled emission centres may be tailored to emit distinct colours, opening the path for sensitive field sensing and colour-switchable devices such as a novel pixel design for displays or an electric-field-induced colour-tunable single-photon source.

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Fig. 1: EF modulation of fluorescence in CQDM versus mono-QD.
Fig. 2: EF-induced colour switching at 10 Hz modulation rate.
Fig. 3: Effective mass calculations of electron and hole states under applied EF.
Fig. 4: Correlation between g2(0) and colour switching.
Fig. 5: Calculations of colour switching for different band offsets and different neck widths (fusion).
Fig. 6: Broadband colour switching in hetero-sized CQDMs.

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Data availability

The data that support the findings of this study are available within the Article and its Supplementary Information. Source data are provided with this paper. Any additional data are available from the corresponding author upon request.

Code availability

The home-written MATLAB code used for the analysis of the measurements performed is not deemed central to the conclusions, and follows spectral analysis standards of the field (and previous works). It is available from the corresponding author upon reasonable request.

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Acknowledgements

The study has received financial support from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (project CoupledNC, grant agreement no. [741767]; project CQDplay, grant agreement no. [101069322]) (U.B., Y.O., A.L., Y.E.P., E.S., N.C. and S.K.). Y.O. and E.S. acknowledge support from the Hebrew University Center for Nanoscience and Technology. Y.E.P. acknowledges support from the Ministry of Science and Technology and the National Foundation for Applied and Engineering Sciences, Israel. S.K. acknowledges support from the Planning and Budgeting Committee of the higher board of education in Israel through a fellowship. U.B. thanks the Alfred & Erica Larisch memorial chair. We thank G. Chechelinsky, M. Saidian, I. Shweki and S. Eliav from the Unit for Nano Characterization (UNC) of the Hebrew University of Jerusalem, Center for Nanoscience and Nanotechnology, for assistance in the electrode device fabrication. We thank S. Gigi for helpful discussions.

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Authors and Affiliations

  1. Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel

    Yonatan Ossia, Adar Levi, Yossef E. Panfil, Somnath Koley, Einav Scharf, Nadav Chefetz & Uri Banin

  2. The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem, Israel

    Yonatan Ossia, Adar Levi, Yossef E. Panfil, Somnath Koley, Einav Scharf, Sergei Remennik, Atzmon Vakahi & Uri Banin

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Contributions

U.B., Y.E.P. and Y.O. conceived this study. A.L. developed and synthesized all the CQDM samples for this study. Y.O. fabricated the electrode devices with assistance from N.C.; conducted the optical experiments with assistance from S.K., E.S. and N.C.; and performed the numerical simulations in consultation with Y.E.P. The idea for the FIB lift-out-assisted optical electron microscopy–single-particle correlations was conceived and realized by A.V. and Y.O. A.V. operated the FIB and developed the sample preparation technique for STEM imaging. S.R. conducted the electron microscopy characterization of single CQDMs. Y.O. analysed the experimental data and simulations with inputs from all other authors. U.B. and Y.O. wrote the paper in consultation with all authors.

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Correspondence to Uri Banin.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–31, Text 1 (on self-consistent effective mass calculations), Table 1 and captions for Videos 1–3.

Supplementary Video 1

Step-by-step lift out and TEM grid preparation (using the SEM–dual-beam FIB system).

Supplementary Video 2

Raw measurement of PL emission wavelength on the EMCCD of the CQDM (Figs. 1c and 2), with periodic EF modulation from +180 to 0 V at 10 Hz rate.

Supplementary Video 3

Measurement of PL emission wavelength on the EMCCD of the CQDM (Fig. 6a and Supplementary Fig. 26) with periodic EF modulation between +180 and −180 V at 10 Hz rate.

Source data

Source Data Figs. 1–6

Experimental and analysis data for Figs. 1–6.

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Ossia, Y., Levi, A., Panfil, Y.E. et al. Electric-field-induced colour switching in colloidal quantum dot molecules at room temperature. Nat. Mater. 22, 1210–1217 (2023). https://doi.org/10.1038/s41563-023-01606-0

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