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Giant nonlinear optical responses from photon-avalanching nanoparticles

Author

Listed:
  • Changhwan Lee

    (Columbia University)

  • Emma Z. Xu

    (Columbia University)

  • Yawei Liu

    (Lawrence Berkeley National Laboratory
    Changchun Institute of Applied Chemistry, Chinese Academy of Sciences)

  • Ayelet Teitelboim

    (Lawrence Berkeley National Laboratory)

  • Kaiyuan Yao

    (Columbia University)

  • Angel Fernandez-Bravo

    (Lawrence Berkeley National Laboratory
    University of St Andrews
    University of St Andrews)

  • Agata M. Kotulska

    (Polish Academy of Sciences)

  • Sang Hwan Nam

    (Laboratory for Advanced Molecular Probing (LAMP), Korea Research Institute of Chemical Technology (KRICT))

  • Yung Doug Suh

    (Laboratory for Advanced Molecular Probing (LAMP), Korea Research Institute of Chemical Technology (KRICT)
    Sungkyunkwan University (SKKU))

  • Artur Bednarkiewicz

    (Polish Academy of Sciences)

  • Bruce E. Cohen

    (Lawrence Berkeley National Laboratory
    Lawrence Berkeley National Laboratory)

  • Emory M. Chan

    (Lawrence Berkeley National Laboratory)

  • P. James Schuck

    (Columbia University)

Abstract

Avalanche phenomena use steeply nonlinear dynamics to generate disproportionately large responses from small perturbations, and are found in a multitude of events and materials1. Photon avalanching enables technologies such as optical phase-conjugate imaging2, infrared quantum counting3 and efficient upconverted lasing4–6. However, the photon-avalanching mechanism underlying these optical applications has been observed only in bulk materials and aggregates6,7, limiting its utility and impact. Here we report the realization of photon avalanching at room temperature in single nanostructures—small, Tm3+-doped upconverting nanocrystals—and demonstrate their use in super-resolution imaging in near-infrared spectral windows of maximal biological transparency. Avalanching nanoparticles (ANPs) can be pumped by continuous-wave lasers, and exhibit all of the defining features of photon avalanching, including clear excitation-power thresholds, exceptionally long rise time at threshold, and a dominant excited-state absorption that is more than 10,000 times larger than ground-state absorption. Beyond the avalanching threshold, ANP emission scales nonlinearly with the 26th power of the pump intensity, owing to induced positive optical feedback in each nanocrystal. This enables the experimental realization of photon-avalanche single-beam super-resolution imaging7 with sub-70-nanometre spatial resolution, achieved by using only simple scanning confocal microscopy and without any computational analysis. Pairing their steep nonlinearity with existing super-resolution techniques and computational methods8–10, ANPs enable imaging with higher resolution and at excitation intensities about 100 times lower than other probes. The low photon-avalanching threshold and excellent photostability of ANPs also suggest their utility in a diverse array of applications, including sub-wavelength imaging7,11,12 and optical and environmental sensing13–15.

Suggested Citation

  • Changhwan Lee & Emma Z. Xu & Yawei Liu & Ayelet Teitelboim & Kaiyuan Yao & Angel Fernandez-Bravo & Agata M. Kotulska & Sang Hwan Nam & Yung Doug Suh & Artur Bednarkiewicz & Bruce E. Cohen & Emory M. C, 2021. "Giant nonlinear optical responses from photon-avalanching nanoparticles," Nature, Nature, vol. 589(7841), pages 230-235, January.
  • Handle: RePEc:nat:nature:v:589:y:2021:i:7841:d:10.1038_s41586-020-03092-9
    DOI: 10.1038/s41586-020-03092-9
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    Citations

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    Cited by:

    1. Xin Zhang & Hao Suo & Yang Guo & Jiangkun Chen & Yu Wang & Xiaohe Wei & Weilin Zheng & Shuohan Li & Feng Wang, 2024. "Continuous tuning of persistent luminescence wavelength by intermediate-phase engineering in inorganic crystals," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    2. Rui Pu & Qiuqiang Zhan & Xingyun Peng & Siying Liu & Xin Guo & Liangliang Liang & Xian Qin & Ziqing Winston Zhao & Xiaogang Liu, 2022. "Super-resolution microscopy enabled by high-efficiency surface-migration emission depletion," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    3. Zhao Jiang & Liangrui He & Zhiwen Yang & Huibin Qiu & Xiaoyuan Chen & Xujiang Yu & Wanwan Li, 2023. "Ultra-wideband-responsive photon conversion through co-sensitization in lanthanide nanocrystals," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Long Yan & Jinshu Huang & Zhengce An & Qinyuan Zhang & Bo Zhou, 2024. "Spatiotemporal control of photochromic upconversion through interfacial energy transfer," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    5. Ahmed Sule & Zulkarnain Abdul Latiff & Mohd Azman Abas & Ibham Veza & Manzoore Elahi M. Soudagar & Irianto Harny & Vorathin Epin, 2023. "Dual Effects of N-Butanol and Magnetite Nanoparticle to Biodiesel-Diesel Fuel Blends as Additives on Emission Pattern and Performance of a Diesel Engine with ANN Validation," Sustainability, MDPI, vol. 15(2), pages 1-22, January.
    6. Xiang-Dong Chen & En-Hui Wang & Long-Kun Shan & Shao-Chun Zhang & Ce Feng & Yu Zheng & Yang Dong & Guang-Can Guo & Fang-Wen Sun, 2023. "Quantum enhanced radio detection and ranging with solid spins," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    7. Guowei Li & Shihui Jiang & Aijun Liu & Lixiang Ye & Jianxi Ke & Caiping Liu & Lian Chen & Yongsheng Liu & Maochun Hong, 2023. "Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H+ doping," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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