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

Yanyu Xiong, Qinglan Huang, Taylor D. Canady, Priyash Barya, Shengyan Liu, Opeyemi H. Arogundade, Caitlin M. Race, Congnyu Che, Xiaojing Wang, Lifeng Zhou, Xing Wang, Manish Kohli, Andrew M. Smith and Brian T. Cunningham ()
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Yanyu Xiong: University of Illinois at Urbana−Champaign
Qinglan Huang: University of Illinois at Urbana−Champaign
Taylor D. Canady: University of Illinois at Urbana−Champaign
Priyash Barya: University of Illinois at Urbana−Champaign
Shengyan Liu: University of Illinois at Urbana−Champaign
Opeyemi H. Arogundade: University of Illinois at Urbana-Champaign
Caitlin M. Race: University of Illinois at Urbana−Champaign
Congnyu Che: University of Illinois at Urbana−Champaign
Xiaojing Wang: University of Illinois at Urbana−Champaign
Lifeng Zhou: University of Illinois at Urbana−Champaign
Xing Wang: University of Illinois at Urbana−Champaign
Manish Kohli: Huntsman Cancer Institute
Andrew M. Smith: University of Illinois at Urbana−Champaign
Brian T. Cunningham: University of Illinois at Urbana−Champaign

Nature Communications, 2022, vol. 13, issue 1, 1-14

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-32387-w

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