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Electrically assisted amplified spontaneous emission in perovskite light-emitting diodes

Nature Photonics volume 18, pages 132–138 (2024)Cite this article

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Abstract

Metal halide perovskites have emerged as promising gain materials for thin-film laser diodes. However, achieving electrically excited amplified spontaneous emission (ASE) in perovskite light-emitting diodes (PeLEDs), a pre-condition for perovskite laser diodes, is hindered by the conflicting requirements of high conductivity and high net modal gain of the device stack. Here we develop a transparent PeLED architecture that combines low optical losses with excellent current-injection properties. Using 2.3 ns optical pulses at 77 K, we achieve ASE with a threshold of 9.1 μJ cm−2. Upon submicrosecond electrical excitation at 77 K of the same device, we achieve current densities above 3 kA cm−2 with irradiance values above 40 W cm−2. Notably, co-pumping the PeLED with optical pulses that are synchronized with the leading edge of an intense electrical pulse results in a reduction of the ASE threshold by 1.2 ± 0.2 μJ cm−2, showing that electrically injected carriers contribute to optical gain. Furthermore, to assess the feasibility of a perovskite semiconductor optical amplifier, we probe the PeLED with 1-μs-long optical excitation and observe continuous-wave ASE at a threshold of 3.8 kW cm−2. Finally, we show that such intense electrical pulses generate electroluminescence brightness levels close to half the irradiance produced by continuous-wave optical pumping at the ASE threshold. This work shows that perovskite semiconductor optical amplifiers and injection lasers are within reach using this type of transparent PeLED.

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Fig. 1: Structural and optoelectronic properties of transparent PeLEDs.
Fig. 2: Co-pumping dynamics under sub-µs electrical and 2.3 ns optical biases.
Fig. 3: Stand-alone CW optical and CW photo-electrical co-excitation.
Fig. 4: Irradiance level comparison under 200 ns electrical and 500 ns CW optical biases in the transparent PeLED.

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All data that support the findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

The project leading to these results has received funding from the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grant agreement number 835133).

Author information

Author notes

  1. Weiming Qiu

    Present address: Guangzhou Chasing-Light Technology Co. Ltd, Guangzhou, China

  2. These authors contributed equally: Karim Elkhouly, Iakov Goldberg.

Authors and Affiliations

  1. IMEC, Leuven, Belgium

    Karim Elkhouly, Iakov Goldberg, Xin Zhang, Nirav Annavarapu, Sarah Hamdad, Guillaume Croes, Cedric Rolin, Jan Genoe, Weiming Qiu, Robert Gehlhaar & Paul Heremans

  2. Department of Electrical Engineering (ESAT), KU Leuven, Leuven, Belgium

    Karim Elkhouly, Iakov Goldberg, Xin Zhang, Nirav Annavarapu, Sarah Hamdad, Guillaume Croes, Jan Genoe & Paul Heremans

  3. Center for Micro Nano Systems, School of Information Science and Technology (SIST), Fudan University, Shanghai, China

    Xin Zhang

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Contributions

K.E. conceived the PeLED stack for operation at high current density, designed the experiments and conducted the photo-electrical characterization. I.G. conceived, designed and fabricated the double-ITO structure, performed optical modelling and optimized the stack design for low optical thresholds. X.Z. conceived and fabricated the device stack and functional layers. N.A. and S.H. aided in the optical design of the stack and in performing optical characterization and modal loss modelling. G.C. acquired the SEM image. W.Q. aided in conceiving the PeLED stack, supervision and design of the experiments. C.R., R.G., J.G. and P.H. supervised this work. K.E. and I.G. wrote the first draught of the manuscript. All authors revised and approved the final version of the manuscript.

Corresponding authors

Correspondence to Robert Gehlhaar or Paul Heremans.

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Extended data

Extended Data Fig. 1 Optical characterization of PeLED stacks with 2.3 ns Iopt,ns pump source.

PL output from a PeLED stack with a diameter (⌀) of 50 μm at (a) 77 K and (b) 291 K. PL output from a contact-free PeLED stack at (c) 77 K and (d) 291 K.

Source data

Extended Data Fig. 2 Optical characterization of PeLED stacks with Iopt,ns pump source.

a-c, PL output from the contacted PeLED stacks with different active areas at 77 K. d, Corresponding light output intensity as a function of input laser fluence (Iopt,ns).

Source data

Extended Data Fig. 3 PeLED optical constants and absorption/emission modeling.

a, Refractive indices and b, extinction coefficients of other PeLED functional layers. c, Layer stack with a broad isotropic dipole distribution in the perovskite layer (PVK) used for the multi-physics modeling. The perovskite reabsorption was set to 0, thereby excluding photon recycling effects. Me-4PACz /AlxOy HTL was not factored in due to negligible thickness. d, Simulated EL intensity as a function of viewing angle. e, Maximum simulated EQE from each device facet for IQE of 100%. f, Simulated absorption of the perovskite gain layer of the contacted PeLED as a function of excitation wavelength for the case of sapphire/top ITO light incidence. g, Simulated absorption of the perovskite gain layer as a function of excitation wavelength for the contacted and electrode-free PeLED stacks with light impinging from the sapphire side.

Source data

Extended Data Fig. 4 EL spectra from a ø 50 µm device recorded through the substrate at 77 K.

a, As-recorded. b, Normalized.

Source data

Extended Data Fig. 5 Photo-electrical co-excitation of contacted PeLED stacks at 77 K.

a-f, Standalone optical excitation with variable Iopt,ns (black solid lines), photo-electrical spectra at variable Iopt,ns and fixed Vp (dashed), and joint spectra adjusted by subtracting the reference EL signal (coloured solid lines). The Vp (J = 3.5 kA cm−2) was fixed across these measurements, producing the reference EL signal shown in (a) in the absence of optical excitation.

Source data

Extended Data Fig. 6 Deconvolution of PLns signals under standalone 2.3 ns optical bias and photo-electric co-excitation at the onset of the electrical pulse into two (without Vp) or three (with Vp) Gaussian contributions.

a-b, Exemplary fits at variable Iopt,ns without electrical bias. c-d, Exemplary fits at variable Iopt,ns with electrical bias. e, As-extracted, and f, right-shifted by 1.2 µJ cm−2 Gaussian amplitudes with and without Vp. For SE (PL) and ASE fits, both central energy (wavelength) and standard deviation are fixed. All the parameters of SE (EL) fit are fixed. SE (EL) signal was multiplied by a factor of 0.23 to account for EL contribution to the total signal and is displayed as SE (EL)*. The PL laser pulse duration is 2.3 ns (Supplementary Fig. 7a), whereas the EL + PL signal integration time was 10 ns. The horizontal error bars represent experimental input energy uncertainty, whereas vertical error bars represent one standard deviation for the fitted parameter.

Source data

Extended Data Fig. 7 Deconvolution of PLcw signals under standalone 1 µs CW optical bias and under photo-electric co-excitation into two (without Vp) or three (with Vp) Gaussian contributions.

a-b, Exemplary fits at variable Iopt,cw without Vp. c, SE (PL) and ASE Gaussian amplitudes as a function of input laser power Iopt,cw without Vp. d-e, Exemplary fits at variable Iopt,cw with Vp. f, SE (PL), SE (EL), and ASE Gaussian amplitudes as a function of input laser power Iopt,cw with Vp. For SE (PL) fit, only central energy (wavelength) is fixed; standard deviation and amplitude vary. For ASE fit, both central energy (wavelength) and standard deviation are fixed. All the parameters of SE (EL) fit are fixed. The vertical error bars represent one standard deviation for the fitted parameter.

Source data

Extended Data Fig. 8 Transient luminescence response at a constant CW Iopt,cw pulse (15 kW cm−2) and variable Vp from 140 to 3500 A cm−2.

300 ns-long electrical pulses are applied 300 ns after the onset of the CW optical pulse.

Source data

Supplementary information

Supplementary Information

Supplementary Figs. 1–8, Notes 1–4, Table 1 and Experimental methods.

Source data

Source Data Fig. 1

Raw data for experimental/simulated curves.

Source Data Fig. 2

Raw data for experimental/simulated curves.

Source Data Fig. 3

Raw data for experimental/simulated curves.

Source Data Fig. 4

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 1

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 2

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 3

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 4

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 5

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 6

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 7

Raw data for experimental/simulated curves.

Source Data Extended Data Fig. 8

Raw data for experimental/simulated curves.

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Elkhouly, K., Goldberg, I., Zhang, X. et al. Electrically assisted amplified spontaneous emission in perovskite light-emitting diodes. Nat. Photon. 18, 132–138 (2024). https://doi.org/10.1038/s41566-023-01341-7

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