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Optical gain and lasing from bulk cadmium sulfide nanocrystals through bandgap renormalization

Nature Nanotechnology volume 18, pages 1423–1429 (2023)Cite this article

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Abstract

Strongly confined colloidal quantum dots have been investigated for low-cost light emission and lasing for nearly two decades. However, known materials struggle to combine technologically relevant metrics of low-threshold and long inverted-state lifetime with a material gain coefficient fit to match cavity losses, particularly under electrical excitation. Here we show that bulk nanocrystals of CdS combine an exceptionally large material gain of 50,000 cm−1 with best-in-class gain thresholds below a single exciton per nanocrystal and 3 ns gain lifetimes not limited by non-radiative Auger processes. We quantitatively account for these findings by invoking a strong bandgap renormalization effect, unobserved in nanocrystals to date, to the best of our knowledge. Next, we demonstrate broadband amplified spontaneous emission and lasing under quasi-continuous-wave conditions. Our results highlight the prospects of bulk nanocrystals for lasing from solution-processable materials.

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Fig. 1: Photophysical properties of CdS BNCs.
Fig. 2: ASE in thin-film CdS BNCs.
Fig. 3: Optically pumped lasing.
Fig. 4: Quantitative bulk gain model.
Fig. 5: Gain threshold and dynamics of CdS BNCs.

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Data availability

The datasets are available from the corresponding author upon reasonable request.

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Acknowledgements

I.T. acknowledges support from FWO-Vlaanderen, grant no. 1S96819N. Z.H., P.G. and M.S. acknowledge funding from the Research Foundation—Flanders (FWO-Vlaanderen) under the SBO PROCEED project (no. S0002019N). Z.H. acknowledges Ghent University for funding (BOF-GOA 01G01019 MANAWORK, FWO Project G0B2921N). D.V.T. acknowledges funding through FWO (G0B2921N). I.W., J.H. and K.C. acknowledge support from the Marsden Fast-Start Fund by the Royal Society of New Zealand through contract VUW1715. I.M., P.G. and S.A.C. acknowledge funding from the Research Foundation—Flanders (FWO-Vlaanderen under grant no. G037221N—HITEC). The TEM measurements were performed at the UGent TEM Core Facility and the spectroscopic measurements at the UGent NoLIMITS Core Facility.

Author information

Author notes

  1. Ali Hossain Khan

    Present address: Ghent University, Physics and Chemistry of Nanostructures, Gent, Belgium

Authors and Affiliations

  1. Photonics Research Group, Ghent University, Gent, Belgium

    Ivo Tanghe & Dries Van Thourhout

  2. NoLIMITS Center For Non-Linear Microscopy and Spectroscopy, Ghent University, Gent, Belgium

    Ivo Tanghe, Servet Ataberk Cayan, Dries Van Thourhout, Zeger Hens & Pieter Geiregat

  3. Physics and Chemistry of Nanostructures, Ghent University, Gent, Belgium

    Ivo Tanghe, Margarita Samoli, Servet Ataberk Cayan, Iwan Moreels, Zeger Hens & Pieter Geiregat

  4. School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, New Zealand

    Isabella Wagner & Justin Hodgkiss

  5. MacDiarmid Institute for Advanced Materials and Nanotechnology, Wellington, New Zealand

    Isabella Wagner, Kai Chen & Justin Hodgkiss

  6. Department of Chemical and Biological Sciences, S. N. Bose National Centre for Basic Sciences, Kolkata, India

    Ali Hossain Khan

  7. Robinson Research Institute, Victoria University of Wellington, Wellington, New Zealand

    Kai Chen

  8. The Dodd-Walls Centre for Photonic and Quantum Technologies, University of Otago, Dunedin, New Zealand

    Kai Chen

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Contributions

I.T. measured the transient absorption data; developed the modelling framework; fabricated and measured the chips for the ASE, VSL and laser measurements; and analysed the data. M.S. and A.H.K. developed the CdS nanocrystal synthesis and carried out the structural characterization. I.W. and K.C. performed the transient PL measurements. S.A.C. fabricated the CdS thin films for the ASE, VSL and lasing experiments. K.C., J.H., I.M., D.V.T., Z.H. and P.G. were involved to analyse and discuss the results and supervise the research. P.G. wrote the manuscript together with I.T.

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Correspondence to Pieter Geiregat.

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Nature Nanotechnology thanks Sergio Brovelli and the other, anonymous, reviewers for their contribution to the peer review of this work.

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Supplementary Sections 1–11, Figs. 1–17, Tables 1–4 and discussion.

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Tanghe, I., Samoli, M., Wagner, I. et al. Optical gain and lasing from bulk cadmium sulfide nanocrystals through bandgap renormalization. Nat. Nanotechnol. 18, 1423–1429 (2023). https://doi.org/10.1038/s41565-023-01521-0

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