Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection

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 an...

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Main 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
Other Authors: School of Electrical and Electronic Engineering
Format: Article
Language:English
Published: 2022
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Online Access:https://hdl.handle.net/10356/156856
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Institution: Nanyang Technological University
Language: English
id sg-ntu-dr.10356-156856
record_format dspace
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Electrical and electronic engineering
Fibers
Surface-Enhanced Raman Scattering
spellingShingle Engineering::Electrical and electronic engineering
Fibers
Surface-Enhanced Raman Scattering
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
Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
description 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.
author2 School of Electrical and Electronic Engineering
author_facet School of Electrical and Electronic Engineering
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
format Article
author 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
author_sort Xu, Guoliang
title Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
title_short Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
title_full Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
title_fullStr Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
title_full_unstemmed Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
title_sort selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection
publishDate 2022
url https://hdl.handle.net/10356/156856
_version_ 1734310173915217920
spelling sg-ntu-dr.10356-1568562022-05-09T02:07:35Z Selenium vacancies and synergistic effect of near- and far-fieldenabled ultrasensitive surface-enhanced raman-scattering-active substrates for malaria detection 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 School of Electrical and Electronic Engineering Engineering::Electrical and electronic engineering Fibers Surface-Enhanced Raman Scattering 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. Ministry of Education (MOE) National Research Foundation (NRF) Submitted/Accepted version This work was partially supported by Shenzhen Basic Research Grants JCYJ20200109114801744, JCYJ20180507182431967, and JCYJ20170413153246713, Shenzhen Peacock Technology Innovation Project KQJSCX20170731165602155, and the National Nature Science Foundation of China (11804354, 61774164, 21701185, 61875064). This work was supported in part by the Singapore Ministry of Education Academic Research Fund Tier 2 (MOE2019-T2-2-127), the Singapore Ministry of Education Academic Research Fund Tier 1 (MOE2019-T1-001-103 and MOE2019-T1-001-111) and the Singapore National Research Foundation Competitive Research Program (NRF-CRP18-2017-02). This work was also supported in part by Nanyang Technological University. 2022-05-09T02:07:35Z 2022-05-09T02:07:35Z 2022 Journal Article 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. https://dx.doi.org/10.1021/acs.jpclett.1c03873 1948-7185 https://hdl.handle.net/10356/156856 10.1021/acs.jpclett.1c03873 35129342 2-s2.0-85124799629 6 13 1453 1463 en MOE2019-T2-2-127 MOE2019-T1-001-103 MOE2019-T1-001-111 NRF-CRP18-2017-02 Journal of Physical Chemistry Letters 10.21979/N9/YNDEDL 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 https://doi.org/10.1021/acs.jpclett.1c03873. application/pdf