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Title: Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
Authors: Xu, Guoliang
Dong, Ruiling
Gu, Dayong
Tian, Huili
Xiong, Lei
Wang, Zhixun
Wang, Wei
Shao, Yan
Li, Wenjie
Li, Guangyuan
Zheng, Xue
Yu, Yang
Feng, Ye
Dong, Yuming
Zhong, Guohua
Zhang, Baoping
Li, Weimin
Wei, Lei
Yang, Chunlei
Chen, Ming
Keywords: Engineering::Electrical and electronic engineering
Issue Date: 2022
Source: Xu, G., Dong, R., Gu, D., Tian, H., Xiong, L., Wang, Z., Wang, W., Shao, Y., Li, W., Li, G., Zheng, X., Yu, Y., Feng, Y., Dong, Y., Zhong, G., Zhang, B., Li, W., Wei, L., Yang, C. & Chen, M. (2022). Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection. Journal of Physical Chemistry Letters, 13(6), 1453-1463.
Project: MOE2019-T2-2-127
Journal: Journal of Physical Chemistry Letters
Abstract: Defect engineering with the active control of defect states brings remarkable enhancement on surface-enhanced Raman scattering (SERS) by magnifying semiconductor-molecule interaction. Such light-trapping architectures can increase the light path length, which promotes photon-analytes interactions and further improves the SERS sensitivity. However, by far the reported semiconductor SERS-active substrates based on these strategies are often nonuniform and commonly in the form of isolated laminates or random clusters, which limit their reliability and stability for practical applications. Herein, we develop self-grown single-crystalline "V-shape" SnSe2-x (SnSe1.5, SnSe1.75, SnSe2) nanoflake arrays (SnSe2-x NFAs) with controlled selenium vacancies over large-area (10 cm × 10 cm) for ultrahigh-sensitivity SERS. First-principles density functional theory (DFT) is used to calculate the band gap and the electronic density of states (DOS). Based on the Herzberg-Teller theory regarding the vibronic coupling, the results of theoretical calculation reveal that the downshift of band edge and high DOS of SnSe1.75 can effectively enhance the vibronic coupling within the SnSe1.75-R6G system, which in turn enhances the photoinduced charge transfer resonance and contributes to the SERS activity with a remarkable enhancement factor of 1.68 × 107. Furthermore, we propose and demonstrate ultrasensitive (10-15 M for R6G), uniform, and reliable SERS substrates by forming SnSe1.75 NFAs/Au heterostructures via a facile Au evaporation process. We attribute the superior performance of our SnSe1.75 NFAs/Au heterostructures to the following reasons: (1) selenium vacancies and (2) synergistic effect of the near and far fields. In addition, we successfully build a detection platform to achieve rapid (∼15 min for the whole process), antibody-free, in situ, and reliable early malaria detection (100% detection rate for 10 samples with 160 points) in whole blood, and molecular hemozoin (<100/mL) can be detected. Our approach not only provides an efficient technique to obtain large-area, uniform, and reliable SERS-active substrates but also offers a substantial impact on addressing practical issues in many application scenarios such as the detection of insect-borne infectious diseases.
ISSN: 1948-7185
DOI: 10.1021/acs.jpclett.1c03873
DOI (Related Dataset): 10.21979/N9/YNDEDL
Schools: School of Electrical and Electronic Engineering 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
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