Versatile cascade migrating photon avalanches for full-spectrum extremely nonlinear emissions and super-resolution microscopy

Hui Wu; Binxiong Pan; Qi Zhao; Chenyi Wang; Rui Pu; Chang Liu; Zeheng Chen; Zewei Luo; Jing Huang; Wei Wei; Tongsheng Chen; Qiuqiang Zhan

doi:10.1117/1.AP.6.5.056010

Advanced Photonics, Volume. 6, Issue 5, 056010(2024)

Versatile cascade migrating photon avalanches for full-spectrum extremely nonlinear emissions and super-resolution microscopy

Hui Wu^1、†, Binxiong Pan¹, Qi Zhao¹, Chenyi Wang¹, Rui Pu¹, Chang Liu¹, Zeheng Chen¹, Zewei Luo², Jing Huang¹, Wei Wei², Tongsheng Chen², and Qiuqiang Zhan^1,3、*

Author Affiliations

¹South China Normal University, South China Academy of Advanced Optoelectronics, Centre for Optical and Electromagnetic Research, Guangzhou, China

²South China Normal University, College of Biophotonics, MOE Key Laboratory & Guangdong Provincial Key Laboratory of Laser Life Science, Guangzhou, China

³South China Normal University, Guangdong Engineering Research Centre of Optoelectronic Intelligent Information Perception, Guangzhou, China

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Figures & Tables(6)

Fig. 1. Mechanistic diagram and theoretical simulations of cascade migrating photon avalanches (cMPA). (a) Two main kinds of existing PA strategies in the lanthanide-doped nanoparticles: single-type-ion and dual-type-ion. When the excitation intensity $I$ exceeds the PA threshold $I_{th}$ , the population in the metastable state grows rapidly due to cross-relaxation, leading to the occurrence of photon avalanches. (b) The proposed cMPA mechanism. With the synergetic effect of two migrating photon avalanche networks (MPA-I and MPA-II), the $X^{3 +}$ can get avalanched by establishing a cascade photon avalanche migration network for further energy transfer processes from $A^{3 +}$ to $X^{3 +}$ . (c) The simulation results of emission intensity versus excitation intensity curves at 484 nm ( $\Pr^{3 +}$ ), 475 nm ( ${Tm}^{3 +}$ ), and 452 nm ( ${Tm}^{3 +}$ ) in the ${Yb}^{3 +} / \Pr^{3 +} / {Tm}^{3 +}$ -codoped nanoparticles, featuring an $S$ -shaped curve with a clear threshold. (d) The simulation plots of emission intensity versus excitation intensity show the amplified nonlinear response of $X^{3 +}$ through ${Yb}^{3 +}$ and ${Gd}^{3 +}$ cascade avalanching energy migration network.

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Fig. 2. PA effect of ${Yb}^{3 +} / \Pr^{3 +} / {Tm}^{3 +}$ nanoparticles. (a) The energy transfer mechanism of ${Yb}^{3 +} / \Pr^{3 +} / {Tm}^{3 +}$ system. (b) The luminescence spectra of the nanoparticles ${NaYF}_{4} : Yb / \Pr (x / 0.5 %) @ {NaYF}_{4} : Yb / Tm$ $(y / 4 %) @ {NaYF}_{4} : Yb / \Pr (x / 0.5 %) @ {NaYF}_{4}$ ( $x = 15 %, 25 %; y = 3 %, 10 %$ ), respectively, showing different intensities of ${Tm}^{3 +}$ under 452 nm emission while varying the ${Yb}^{3 +}$ concentration. (c) The experimental curves of ${Tm}^{3 +}$ 452 nm emission intensity versus excitation intensity for different nanoparticles with different ${Yb}^{3 +}$ concentrations. The nonlinearity order is derived from a linear fit of the log−log plot. (d) The comparisons of intensity ratio of ${Tm}^{3 +}$ (452 nm) emission intensity to $\Pr^{3 +}$ (484 nm) and nonlinearity order from two samples [sample 1: ${NaYF}_{4} : Yb / \Pr (15 % / 0.5 %) @ {NaYF}_{4} : Yb / Tm (3 % / 4 %) @ {NaYF}_{4} : Yb / \Pr (15 % / 0.5 %) @ {NaYF}_{4}$ and sample 2: ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4} : Yb / Tm (10 % / 4 %) @ {NaYF}_{4} : Yb / \Pr (25 % / 0.5 %)$ @ ${NaYF}_{4}$ ].

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Fig. 3. PA effect in ${Tb}^{3 +}$ -doped nanoparticles realized by cMPA mechanism. (a) Schematic of the ${Yb}^{3 +} / \Pr^{3 +} / {Tm}^{3 +} / {Tb}^{3 +}$ multi-layer nanostructure. (b) The energy transfer cMPA mechanism of ${Tb}^{3 +}$ -doped system. Through the ${Gd}^{3 +}$ sublattice network, the avalanching energy can be further transferred from ${Tm}^{3 +}$ to the ${Tb}^{3 +}$ . (c) The luminescence spectra of the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4}$ and ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}$ , indicating the ${Tb}^{3 +}$ characteristic emissions at 544 nm, 586 nm, and 620 nm. (d) The experimental curves of emission intensity versus excitation intensity for the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}$ under an 852 nm CW laser. The obtained optical nonlinearities of $\Pr^{3 +}$ emission at 484 nm, ${Tm}^{3 +}$ emission at 452 nm, and ${Tb}^{3 +}$ emission at 544 nm were 26.4, 38.4, and 42.6 orders, respectively. The nonlinearity order is derived from a linear fit of the log−log plot. (e) The luminescence spectra of ${Tb}^{3 +}$ -doped cMPA nanoparticles under 980 nm excitation. (f) The experimental curve of emission intensity versus excitation intensity at 544 nm ( ${Tb}^{3 +}$ ) under 980 nm excitation. (g) ${Yb}^{3 +}$ -mediated CSU mechanism of ${Tb}^{3 +}$ -doped system. (h) Luminescent spectra of ${Yb}^{3 +} / \Pr^{3 +}$ -codoped PA nanoparticles $[{NaYF}_{4} : Yb / \Pr (25 % / 0.5 %)]$ , ${Tb}^{3 +}$ -doped CSU nanoparticles [ ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4} : Yb (10 %) @ {NaYF}_{4} : Yb / Tb (60 % / 40 %) @ {NaYF}_{4}]$ , and ${Tb}^{3 +}$ -doped cMPA nanoparticles $[{NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}]$ .

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Fig. 4. Full-spectrum extremely nonlinear PA emissions enabled by cMPA mechanism. (a) The cMPA mechanism for ${Eu}^{3 +}$ -doped system. (b) The luminescence spectra of the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4}$ and ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Eu (20 %) @ {NaYF}_{4}$ , respectively. The characteristic emissions of ${Eu}^{3 +}$ exist at 592 nm and 617 nm. (c) The experimental curves of emission intensity versus excitation intensity for the ${Eu}^{3 +}$ -doped nanoparticles under 852 nm excitation. The obtained optical nonlinearities of $\Pr^{3 +}$ emission at 484 nm, ${Tm}^{3 +}$ emission at 452 nm, and ${Eu}^{3 +}$ emission at 592 nm were 25.7, 36.6, and 45.3 orders, respectively. The nonlinearity order is derived from a linear fit of the log−log plot. (d) The cMPA mechanism for ${Dy}^{3 +}$ -doped system. (e) The luminescence spectra of the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4}$ and ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %)$ @ ${NaGdF}_{4} : Dy (5 %) @ {NaYF}_{4}$ , respectively. The characteristic emission of ${Dy}^{3 +}$ exists at 574 nm. (f) The experimental curves of emission intensity versus excitation intensity for the ${Dy}^{3 +}$ -doped nanoparticles under 852 nm excitation. The obtained optical nonlinearities of $\Pr^{3 +}$ emission at 484 nm, ${Tm}^{3 +}$ emission at 452 nm, and ${Dy}^{3 +}$ emission at 574 nm were 24.0, 33.9, and 45.4 orders, respectively. The nonlinearity order is derived from a linear fit of the log−log plot. (g) Emission peaks of lanthanide ions capable of photon avalanche with extremely nonlinear response, showing a full-spectrum PA range through the cMPA mechanism.

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Fig. 5. Extremely nonlinear cMPA super-resolution microscopic imaging. (a) The cMPA nanoscopy system with a low-power, single-CW beam is compatible with the standard multiphoton/confocal laser scanning microscope. OL, 100× NA = 1.45 oil-immersed objective lens; PMT, photomultiplier tube; DM, 690 nm short-pass dichroic mirror; F1, $850 / 10 nm$ band-pass filter; F2, 694 nm short-pass filter; F3, 665 nm short-pass filter; PBS, polarizing beam splitter; HWP, half-wave plate. (b-i), (c-i) Single-nanoparticle of ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4} : Yb / Tm (10 % / 4 %) @ {NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaYF}_{4}$ imaged at 605 nm of $\Pr^{3 +}$ (red) and at 452 nm of ${Tm}^{3 +}$ (blue) emission peak, excited by an 852 nm Gaussian beam with $1403 kW {cm}^{- 2}$ . (b-iii), (c-iii) Super-resolution imaging of panels (b-i) and (c-i), excited near the PA threshold ( $320 kW {cm}^{- 2}$ ). (b-ii), (b-iv) Line profile analyses of single nanoparticles indicated by white arrows in panels (b-i) and (b-iii), showing a PSF FWHM of 230 nm and 81 nm, respectively. (c-ii), (c-iv) Line profile analyses of single nanoparticles indicated by the white arrow in panels (c-i) and (c-iii), showing a PSF FWHM of 225 nm and 48 nm, respectively. (b-v) Line profile analysis (black) of a line cut from (b-i), compared with another line cut through a super-resolution image (red) in panel (b-iii). (c-v) As in panel (b-v), but for the image of ${Tm}^{3 +}$ (452 nm) emission peak. (d-i), (e-i) Single-nanoparticle of ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}$ imaged at 484 nm of $\Pr^{3 +}$ (blue) and at 545 nm of ${Tb}^{3 +}$ (green) emission peak, excited by an 852 nm Gaussian beam with $1029 kW {cm}^{- 2}$ . (d-iii), (e-iii) Super-resolution imaging of panels (d-i) and (e-i), excited near the PA threshold ( $196 kW {cm}^{- 2}$ ). (d-ii), (d-iv) Line profile analyses of single nanoparticles indicated by a white arrow in panels (d-i) and (d-iii), showing a PSF FWHM of 231 nm and 96 nm, respectively. (e-ii), (e-iv) Line profile analyses of single nanoparticles indicated by white arrow in panels (e-i) and (e-iii), showing a PSF FWHM of 238 nm and 80 nm, respectively. (d-v) Line profile analysis (black) of a line cut from (d-i), compared with another line cut through a super-resolution image (blue) in panel (d-iii). (e-v) As in panel (d-v), but for the image of ${Tb}^{3 +}$ (545 nm) emission peak. Scale bars are 100 nm, and the pixel dwell time is $100 μ s$ .

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Fig. 6. Single-beam multi-color cMPA super-resolution microscopy. (a) The schematic diagram of the cMPA nanoscopy system. OL, 100× NA = 1.45 oil-immersed objective lens; DM1, 690 nm short-pass dichroic mirror; DM2, 593 nm short-pass dichroic mirror; DM3, 458 nm short-pass dichroic mirror; F1, $605 / 30 nm$ band-pass filter; F2, $550 / 20 nm$ band-pass filter; F3, $440 / 40 nm$ band-pass filter. (b) Channel 1: 605 nm band for the nanoparticles ${NaYF}_{4} : Yb / \Pr (15 % / 0.5 %) @ {NaYF}_{4}$ . The line profile showed $\Pr^{3 +}$ with a resolution of 107 nm at $157 kW {cm}^{- 2}$ excitation. (c) Channel 2: 452 nm band for the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}$ . The line profile showed ${Tm}^{3 +}$ with a resolution of 120 nm at $377 kW {cm}^{- 2}$ excitation. (d) Channel 3: 544 nm band for the nanoparticles ${NaYF}_{4} : Yb / \Pr (25 % / 0.5 %) @ {NaGdF}_{4} : Yb / Tm (10 % / 4 %) @ {NaGdF}_{4} : Tb (20 %) @ {NaYF}_{4}$ . The line profile showed ${Tb}^{3 +}$ with a resolution of 108 nm at $377 kW {cm}^{- 2}$ excitation. (e) Dual-color super-resolution imaging of red and green luminescence from the above two nanoprobes. (f) Dual-color super-resolution imaging of red and blue luminescence from the above two nanoprobes. Scale bars are 300 nm, and the pixel dwell time is $100 μ s$ .

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Hui Wu, Binxiong Pan, Qi Zhao, Chenyi Wang, Rui Pu, Chang Liu, Zeheng Chen, Zewei Luo, Jing Huang, Wei Wei, Tongsheng Chen, Qiuqiang Zhan, "Versatile cascade migrating photon avalanches for full-spectrum extremely nonlinear emissions and super-resolution microscopy," Adv. Photon. 6, 056010 (2024)

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Paper Information

Category: Research Articles

Received: Feb. 8, 2024

Accepted: Aug. 15, 2024

Published Online: Sep. 20, 2024

The Author Email: Qiuqiang Zhan (zhanqiuqiang@m.scnu.edu.cn)

DOI:10.1117/1.AP.6.5.056010

CSTR:32187.14.1.AP.6.5.056010

Topics

laser devices and laser physics

Lasers and Laser Optics

Laser physics

laser manufacturing

Instrumentation, Measurement and Metrology