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Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots

Nature Materials volume 17, pages 35–42 (2018)Cite this article

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Abstract

Colloidal quantum dots (QDs) raise more and more interest as solution-processable and tunable optical gain materials. However, especially for infrared active QDs, optical gain remains inefficient. Since stimulated emission involves multifold degenerate band-edge states, population inversion can be attained only at high pump power and must compete with efficient multi-exciton recombination. Here, we show that mercury telluride (HgTe) QDs exhibit size-tunable stimulated emission throughout the near-infrared telecom window at thresholds unmatched by any QD studied before. We attribute this unique behaviour to surface-localized states in the bandgap that turn HgTe QDs into 4-level systems. The resulting long-lived population inversion induces amplified spontaneous emission under continuous-wave optical pumping at power levels compatible with solar irradiation and direct current electrical pumping. These results introduce an alternative approach for low-threshold QD-based gain media based on intentional trap states that paves the way for solution-processed infrared QD lasers and amplifiers.

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Figure 1: Structural and linear optical properties of HgTe quantum dots (QDs).
Figure 2: Ultrafast spectroscopy.
Figure 3: Optical gain in hybrid PMMA-1%HgTe nanocomposites under continuous-wave (CW) excitation at 447 nm.
Figure 4: HgTe gain model and surface chemistry.

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Acknowledgements

This research is funded by Ghent University (Special Research Fund BOF), BelSPo (IAP 7.35, photonics@be), EU-FP7 (Navolchi), NWO (Vidi grant, No. 723.013.002) Horizon 2020 ITN Phonsi and ERC-ULPICC and ERC-PoC Interdot. P.G. acknowledges the FWO Vlaanderen for a postdoctoral fellowship. S. Flamee is acknowledged for TEM imaging of the QDs and R. Van Deun and P. Smet are acknowledged for the use of the steady-state and time-resolved photoluminescence set-up and the cryogenic spectroscopy, respectively.

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Authors and Affiliations

  1. Physics and Chemistry of Nanostructures group, Ghent University, B-9000 Gent, Belgium

    Pieter Geiregat, Arjan J. Houtepen, Laxmi Kishore Sagar, Valeriia Grigel & Zeger Hens

  2. Photonics Research Group, Ghent University, B-9000 Gent, Belgium

    Pieter Geiregat & Dries Van Thourhout

  3. Center for Nano and Biophotonics, Ghent University, B-9000 Gent, Belgium

    Pieter Geiregat, Laxmi Kishore Sagar, Valeriia Grigel, Dries Van Thourhout & Zeger Hens

  4. Opto-Electronic Materials Section, Delft University of Technology, 2628 BL Delft, The Netherlands

    Arjan J. Houtepen

  5. Department of Theoretical Chemistry and Amsterdam Center for Multiscale Modeling (ACMM), VU University Amsterdam, 1081 HV Amsterdam, The Netherlands

    Ivan Infante & Felipe Zapata

  6. Département Institut Supérieur d’Electronique et du Numérique, IEMN, UMR CNRS, 8520 Lille, France

    Guy Allan & Christophe Delerue

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Contributions

P.G. carried out the steady-state and time-resolved photoluminescence, and the ultrafast experiments, analysed the data, aided in theory development and wrote the manuscript; A.J.H. supervised the experiments, aided in theory discussions and wrote the manuscript; I.I. and F.Z. performed the DFT calculations and wrote the manuscript; L.K.S. synthesized the HgTe QDs and performed structural characterization (TEM, XRD); C.D. and G.A. carried out the tight-binding simulations and aided in theory development; D.V.T. aided in theory discussions and supervised the research; Z.H. initiated and supervised the research, aided in the theory development and wrote the manuscript.

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Correspondence to Pieter Geiregat.

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Geiregat, P., Houtepen, A., Sagar, L. et al. Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots. Nature Mater 17, 35–42 (2018). https://doi.org/10.1038/nmat5000

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