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Published January 20, 2021 | Supplemental Material
Journal Article Open

Upconversion Plasmonic Lasing from an Organolead Trihalide Perovskite Nanocrystal with Low Threshold


The understanding of nonlinear light–matter interactions at the nanoscale has fueled worldwide interest in upconversion emission for imaging, lasing, and sensing. Upconversion lasers with anti-Stokes-type emission with various designs have been reported. However, reducing the volume and lasing threshold of such lasers to the nanoscale level is a fundamental photonics challenge. Here, we demonstrate that the upconversion efficiency can be improved by exploiting single-mode upconversion lasing from a single organo-lead halide perovskite nanocrystal in a resonance-adjustable plasmonic nanocavity. This upconversion plasmonic nanolaser has a very low lasing threshold (10 μJ cm⁻²) and a calculated ultrasmall mode volume (∼0.06 λ³) at 6 K. To provide the unique feature for lasing action, a temporal coherence signature of the upconversion plasmonic nanolasing was determined by measuring the second-order correlation function. The localized-electromagnetic-field confinement can be tailored in titanium nitride resonance-adjustable nanocavities, enhancing the pump-photon absorption and upconverted photon emission rate to achieve lasing. The proof-of-concept results significantly expand the performance of upconversion nanolasers, which are useful in applications such as on-chip, coherent, nonlinear optics, information processing, data storage, and sensing.

Additional Information

© 2020 American Chemical Society. Received 12 October 2020. Published online 27 December 2020. We thank Prof. Mikhail A. Noginov, Prof. Shangjr Gwo and Dr. Ruzan Sokhoyan for useful suggestions. The authors would like to thank Wen-Hui Cheng, Jing-Shun Huang, Cora Went, Wei-Hsiang Lin, Anya Mitskovets, and Meng-Ju Yu for useful discussions. We also acknowledge use of spectroscopic ellipsometry supported by Prof. Yia-Chung Chang. We acknowledge financial support from the Ministry of Science and Technology, Taiwan (Grant No. MOST-106-2112-M-001-036-MY3 (Y.J.L.); MOST-109-2112-M-001-043-MY3 (Y.J.L.); MOST-108-2221-E-001-018-MY3(S.W.C.); MOST 108-2113-M-006-005-MY3 (T.F.G.); MOST-109-2636-E-007-017 (M.Y.L.)) and Academia Sinica (Grant No. AS-CDA-108-M08 (Y.J.L.)), and also by the "Photonics at Thermodynamic Limits" Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0019140 (H.A.A.). Author Contributions. Y.J.L. proposed the original idea, developed the theoretical aspects, and performed all experiments, calculations, and data analysis. Y.J.L., P.J.C., and S.W.C. carried out the simulations. T.L.S. and K.N.P. fabricated the perovskite samples, performed the optical measurements, and helped in discussion. M.Y.L. carried out the TEM analyses. C.W.C., T.F.G., S.W.C., and H.A.A. contributed to the discussion and revised the manuscript. Y.J.L. organized the project and wrote the paper. All authors discussed the results and commented on the manuscript. The authors declare no competing financial interest.

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August 20, 2023
October 23, 2023