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Giant nonlinear optical responses from photon-avalanching nanoparticles
Nature ( IF 42.778 ) Pub Date : 2021-01-13 , DOI: 10.1038/s41586-020-03092-9
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. Chan; P. James Schuck

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 lasing4,5,6. 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 methods8,9,10, 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 sensing13,14,15.



中文翻译:

光子束缚纳米粒子的巨大非线性光学响应

雪崩现象使用陡峭的非线性动力学来从小扰动中产生不成比例的大响应,并且在许多事件和材料中都发现1。光子雪崩使诸如光学相位共轭成像2,红外量子计数3和有效的上转换激光4,5,6等技术成为可能。但是,仅在散装材料和聚集体6,7中观察到了这些光学应用背后的光子束缚机制,从而限制了其效用和影响。在这里,我们报告了单个纳米结构(Tm 3+较小)在室温下光子雪崩的实现。掺杂的上转换纳米晶体,并证明了它们在最大生物透明度的近红外光谱窗口中的超分辨率成像中的应用。雪崩纳米颗粒(ANP)可以被连续波激光泵浦,并表现出光子雪崩的所有定义特征,包括清晰的激发功率阈值,在阈值时异常长的上升时间以及大于比基态吸收大一万倍。超过雪崩阈值,由于在每个纳米晶体中引起正光反馈,因此ANP发射与泵浦强度的26次幂成非线性比例关系。这样就可以通过实验实现光子雪崩单束超分辨率成像7仅使用简单的扫描共聚焦显微镜即可实现70纳米以下的空间分辨率,无需任何计算分析。将其陡峭的非线性与现有的超分辨率技术和计算方法8,9,10结合使用,ANP能够以更高的分辨率成像,并且激发强度比其他探头低100倍。ANPs的低光子富集阈值和出色的光稳定性也表明它们在多种应用中的实用性,包括亚波长成像7,11,12以及光学和环境传感13,14,15

更新日期:2021-01-13
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