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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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.
References
Min, H. et al. Perovskite solar cells with atomically coherent interlayers on SnO2 electrodes. Nature 598, 444–450 (2021).
Zhang, T. et al. Ion-modulated radical doping of spiro-OMeTAD for more efficient and stable perovskite solar cells. Science 377, 495–501 (2022).
Sidhik, S. et al. Deterministic fabrication of 3D/2D perovskite bilayer stacks for durable and efficient solar cells. Science 377, 1425–1430 (2022).
Cao, Y. et al. Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures. Nature 562, 249–253 (2018).
Wang, K. et al. Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes. Nat. Commun. 14, 397 (2023).
Guo, B. et al. Ultrastable near-infrared perovskite light-emitting diodes. Nat. Photonics 16, 637–643 (2022).
Kim, J. S. et al. Ultra-bright, efficient and stable perovskite light-emitting diodes. Nature 611, 688–694 (2022).
Liu, Z. et al. Perovskite light-emitting diodes with EQE exceeding 28% through a synergetic dual-additive strategy for defect passivation and nanostructure regulation. Adv. Mater. 33, 2103268 (2021).
Bao, C. et al. Bidirectional optical signal transmission between two identical devices using perovskite diodes. Nat. Electron. 3, 156–164 (2020).
Ollearo, R. et al. Ultralow dark current in near-infrared perovskite photodiodes by reducing charge injection and interfacial charge generation. Nat. Commun. 12, 7277 (2021).
Lei, L., Dong, Q., Gundogdu, K. & So, F. Metal halide perovskites for laser applications. Adv. Funct. Mater. 31, 2010144 (2021).
Tatarinov, D. A. et al. High-quality CsPbBr3 perovskite films with modal gain above 10 000 cm−1 at room temperature. Adv. Opt. Mater. 11, 2202407 (2023).
Liu, Y. et al. Ligand assisted growth of perovskite single crystals with low defect density. Nat. Commun. 12, 1686 (2021).
Gao, Y. et al. High-performance perovskite light-emitting diodes enabled by passivating defect and constructing dual energy-transfer pathway through functional perovskite nanocrystals. Adv. Mater. 34, 2207445 (2022).
Braly, I. L. et al. Hybrid perovskite films approaching the radiative limit with over 90% photoluminescence quantum efficiency. Nat. Photonics 12, 355–361 (2018).
Pourdavoud, N. et al. Room-temperature stimulated emission and lasing in recrystallized cesium lead bromide perovskite thin films. Adv. Mater. 31, 1903717 (2019).
Huang, C. Y. et al. CsPbBr3 perovskite quantum dot vertical cavity lasers with low threshold and high stability. ACS Photonics 4, 2281–2289 (2017).
Kim, H. et al. Optically pumped lasing from hybrid perovskite light-emitting diodes. Adv. Opt. Mater. 8, 1901297 (2019).
Cho, C. et al. Electrical pumping of perovskite diodes: toward stimulated emission. Adv. Sci. 8, 2101663 (2021).
Jia, Y., Kerner, R. A., Grede, A. J., Rand, B. P. & Giebink, N. C. Continuous-wave lasing in an organic–inorganic lead halide perovskite semiconductor. Nat. Photonics 11, 784–788 (2017).
Qin, C. et al. Stable room-temperature continuous-wave lasing in quasi-2D perovskite films. Nature 585, 53–57 (2020).
Allegro, I. et al. Distributed feedback lasers by thermal nanoimprint of perovskites using gelatin gratings. ACS Appl. Mater. Interfaces 15, 8436–8445 (2023).
Cegielski, P. J. et al. Monolithically integrated perovskite semiconductor lasers on silicon photonic chips by scalable top-down fabrication. Nano Lett. 18, 6915–6923 (2018).
Roh, K. et al. Widely tunable, room temperature, single-mode lasing operation from mixed-halide perovskite thin films. ACS Photonics 6, 3331–3337 (2019).
Goldberg, I. et al. Multimode lasing in all-solution-processed UV-nanoimprinted distributed feedback MAPbI3 perovskite waveguides. ACS Photonics 10, 1591–1600 (2023).
Kim, H. et al. Hybrid perovskite light emitting diodes under intense electrical excitation. Nat. Commun. 9, 4893 (2018).
Zhao, L. et al. Thermal management enables bright and stable perovskite light-emitting diodes. Adv. Mater. 32, 2000752 (2020).
Zhao, L. et al. Nanosecond-pulsed perovskite light-emitting diodes at high current density. Adv. Mater. 33, 2104867 (2021).
Elkhouly, K. et al. Intense electrical pulsing of perovskite light emitting diodes under cryogenic conditions. Adv. Opt. Mater. 10, 2200024 (2022).
Zou, C., Liu, Y., Ginger, D. S. & Lin, L. Y. Suppressing efficiency roll-off at high current densities for ultra-bright green perovskite light-emitting diodes. ACS Nano 14, 6076–6086 (2020).
Zhao, L. et al. Thermal properties of polymer hole-transport layers influence the efficiency roll-off and stability of perovskite light-emitting diodes. Nano Lett. 23, 4785–4792 (2023).
Ahn, N. et al. Optically excited lasing in a cavity-based, high-current-density quantum dot electroluminescent device. Adv. Mater. 35, 2206613 (2023).
Slowik, I. et al. Novel organic light-emitting diode design for future lasing applications. Org. Electron. 48, 132–137 (2017).
Lee, J. H., Ke, T. H., Genoe, J., Heremans, P. & Rolin, C. Overlapping-gate organic light-emitting transistors. Adv. Electron. Mater. 5, 1800437 (2019).
Schols, S. et al. An organic light-emitting diode with field-effect electron transport. Adv. Funct. Mater. 18, 136–144 (2008).
Goldberg, I. et al. Active area dependence of optoelectronic characteristics of perovskite LEDs. J. Mater. Chem. C 9, 12661–12670 (2021).
Elkhouly, K. et al. Operationally stable perovskite light emitting diodes with high radiance. Adv. Opt. Mater. 9, 2100586 (2021).
He, Y. et al. Perovskite light-emitting diodes with near unit internal quantum efficiency at low temperatures. Adv. Mater. 33, 2006302 (2021).
Jia, Y., Kerner, R. A., Grede, A. J., Rand, B. P. & Giebink, N. C. Factors that limit continuous-wave lasing in hybrid perovskite semiconductors. Adv. Opt. Mater. 8, 1901514 (2020).
Brenner, P. et al. Continuous wave amplified spontaneous emission in phase-stable lead halide perovskites. Nat. Commun. 10, 988 (2019).
Ahn, N. et al. Electrically driven amplified spontaneous emission from colloidal quantum dots. Nature 617, 79–85 (2023).
Peters, G. I. & Allen, L. Amplified spontaneous emission I. The threshold condition. J. Phys. A Gen. Phys. 4, 238–243 (1971).
Frolov, S. V., Vardeny, Z. V. & Yoshino, K. Cooperative and stimulated emission in poly(p-phenylene-vinylene) thin films and solutions. Phys. Rev. B 57, 9141 (1998).
Bourdakos, K. N., Cury, L. A. & Monkman, A. P. The dependence of the amplified spontaneous emission on the waveguide excitation length for high quantum efficiency conjugated polymers. Org. Electron. 12, 1142–1145 (2011).
Xie, M. et al. High-efficiency pure-red perovskite quantum-dot light-emitting diodes. Nano Lett. 22, 8266–8273 (2022).
Whitworth, G. L., Dalmases, M., Taghipour, N. & Konstantatos, G. Solution-processed PbS quantum dot infrared laser with room-temperature tunable emission in the optical telecommunications window. Nat. Photonics 15, 738–742 (2021).
Zhang, X. et al. Minimizing the interface-driven losses in inverted perovskite solar cells and modules. ACS Energy Lett. 8, 2532–2542 (2023).
Cho, C. et al. The role of photon recycling in perovskite light-emitting diodes. Nat. Commun. 11, 611 (2020).
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).
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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.
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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.
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).
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.
Extended Data Fig. 4 EL spectra from a ø 50 µm device recorded through the substrate at 77 K.
a, As-recorded. b, Normalized.
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.
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.
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.
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.
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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DOI: https://doi.org/10.1038/s41566-023-01341-7
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