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Stable room-temperature continuous-wave lasing in quasi-2D perovskite films

Abstract

Organic–inorganic lead halide quasi-two-dimensional (2D) perovskites are promising gain media for lasing applications because of their low cost, tunable colour, excellent stability and solution processability1,2,3. Optically pumped continuous-wave (CW) lasing is highly desired for practical applications in high-density integrated optoelectronics devices and constitutes a key step towards electrically pumped lasers4,5,6. However, CW lasing has not yet been realized at room temperature because of the ‘lasing death’ phenomenon (the abrupt termination of lasing under CW optical pumping), the cause of which remains unknown. Here we study lead halide-based quasi-2D perovskite films with different organic cations and observe that long-lived triplet excitons considerably impede population inversion during amplified spontaneous emission and optically pumped pulsed and CW lasing. Our results indicate that singlet–triplet exciton annihilation is a possible intrinsic mechanism causing lasing death. By using a distributed-feedback cavity with a high quality factor and applying triplet management strategies, we achieve stable green quasi-2D perovskite lasers under CW optical pumping in air at room temperature. We expect that our findings will pave the way to the realization of future current-injection perovskite lasers.

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Fig. 1: Chemical structures and ASE properties of P2F8 and N2F8 films on fused silica.
Fig. 2: DFB cavity and pulsed lasing properties of P2F8 and N2F8 films.
Fig. 3: CW lasing characteristics of P2F8 and N2F8 films.

Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

We thank M. R. Leyden, T. Cheng and S. Terakawa for their support and discussion. We thank W. J. Potscavage Jr at Kyushu University for assistance with the preparation of this manuscript. This work was supported by the Japan Science and Technology Agency (JST), ERATO, Adachi Molecular Exciton Engineering Project under JST ERATO grant number JPMJER1305, and the International Institute for Carbon Neutral Energy Research (WPI-I2CNER) sponsored by the Ministry of Education, Culture, Sports, Science and Technology (MEXT) and the Canon Foundation. C.Q. thanks the Changchun Institute of Applied Chemistry and the Chinese Academy of Sciences.

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Contributions

C.Q. and C.A. conceived the idea for the study. C.Q., A.S.D.S., C.Z., T.F., D.Z. and T.M. performed the experiments and analysed the data. C.Q. and T.M. prepared the manuscript. C.A. and C.Q. managed the projects. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Chuanjiang Qin or Chihaya Adachi.

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The authors declare no competing interests.

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Peer review information Nature thanks Jianpu Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data figures and tables

Extended Data Fig. 1 Proposed energy-transfer mechanisms in a quasi-2D perovskite system under photoexcitation.

All components of the quasi-2D perovskite can be excited by ultraviolet light. The excitons are formed in the inorganic layer [PbBr6]4−, with 2D (n = 1) and quasi-2D (n = 2–8) perovskites producing both singlet (S1) and triplet (T1) states. The singlets are rapidly transferred to high-dimensionality perovskite emitters (n = 8). In the case of N2F8, the triplets efficiently transfer to the NMA because of its lower triplet energy, and become confined because of the short distance of Dexter energy transfer. Transfer of triplet excitons to the PEA is negligible because of its high triplet energy, so the triplets can transfer to higher-dimensionality grains and remain in the P2F8 emitter. Γ1 and Γ2 are the triplet energy levels of the inorganic layer [PbBr6]4−; Γ5 is the singlet energy level of the inorganic layer [PbBr6]4−; VB, valence band.

Extended Data Fig. 2 Photoluminescence (PL) decay curves of N2F8 and P2F8 films.

Data taken at room temperature under vacuum.

Extended Data Fig. 3 X-ray diffraction patterns of N2F8 and P2F8 films.

a.u., arbitrary units.

Extended Data Fig. 4 Temperature dependence of ASE spectra for P2F8 and N2F8 films with amplified ASE peak region.

The data shown were obtained at temperatures from 20 to 300 K in 20-K steps.

Extended Data Fig. 5 DFB cavity for N2F8- and P2F8-based laser devices and lasing spectra.

a, Gratings with grating pitches of 240–260 nm in 5-nm steps. b, c, Atomic force microscopy images of the P2F8 film on a grating (b) and a bare area (c). d, e, Lasing spectra of N2F8 (d) and P2F8 (e) on different gratings using film thicknesses of 70−110 nm. We note that the lasing of some DFB gratings is absent owing to a high threshold or bad perovskite morphology.

Extended Data Fig. 6 Refractive index curves of N2F8 and P2F8.

Measured by spectroscopic ellipsometry.

Extended Data Fig. 7 P2F8 lasing under pulse pumping.

a, Operational stability of the P2F8 laser under continuous pulse pumping with an intensity of 10 μJ cm−2. b, Lasing behaviour of P2F8 in oxygen and nitrogen.

Extended Data Fig. 8 CW operation of the P2F8 laser.

a, Operational stability of the P2F8 laser under CW excitation with an intensity of 2 kW cm−2. b, Lasing spectra before (black) and after (red) continuous pumping.

Extended Data Fig. 9 Lasing stability under CW operation in alternating air and nitrogen atmospheres with an excitation intensity over the threshold at room temperature.

a, P2F8; b, N2F8.

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Qin, C., Sandanayaka, A.S.D., Zhao, C. et al. Stable room-temperature continuous-wave lasing in quasi-2D perovskite films. Nature 585, 53–57 (2020). https://doi.org/10.1038/s41586-020-2621-1

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