Photonic crystal enhanced fluorescence emission and blinking suppression for single quantum dot digital resolution biosensing.

Photonic crystal enhanced fluorescence emission and blinking suppression for single quantum dot digital resolution biosensing.
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DOI:
10.1038/s41467-022-32387-w
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发表时间:
2022-08-08
影响因子:
16.6
通讯作者:
Cunningham, Brian T.
Cunningham, Brian T.
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Xiong, Yanyu;Huang, Qinglan;Canady, Taylor D.;Barya, Priyash;Liu, Shengyan;Arogundade, Opeyemi H.;Race, Caitlin M.;Che, Congnyu;Wang, Xiaojing;Zhou, Lifeng;Wang, Xing;Kohli, Manish;Smith, Andrew M.;Cunningham, Brian T.

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While nanoscale quantum emitters are effective tags for measuring biomolecular interactions, their utilities for applications that demand single-unit observations are limited by the requirements for large numerical aperture (NA) objectives, fluorescence intermittency, and poor photon collection efficiency resulted from omnidirectional emission. Here, we report a nearly 3000-fold signal enhancement achieved through multiplicative effects of enhanced excitation, highly directional extraction, quantum efficiency improvement, and blinking suppression through a photonic crystal (PC) surface. The approach achieves single quantum dot (QD) sensitivity with high signal-to-noise ratio, even when using a low-NA lens and an inexpensive optical setup. The blinking suppression capability of the PC improves the QDs on-time from 15% to 85% ameliorating signal intermittency. We developed an assay for cancer-associated miRNA biomarkers with single-molecule resolution, single-base mutation selectivity, and 10-attomolar detection limit. Additionally, we observed differential surface motion trajectories of QDs when their surface attachment stringency is altered by changing a single base in a cancer-specific miRNA sequence. Nanoscale emitters are useful for measuring biomolecular interactions, but are limited by weak signals. Here, the authors use a photonic crystal surface for 3000-fold signal enhancement, achieving single emitter sensitivity with extended on-time, and demonstrate its application in miRNA biomarker sensing.
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