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DNA模板化银纳米簇的光致发光机制:表面等离子体与发光体之间的耦合及溶菌酶传感

Photoluminescence Mechanism of DNA-Templated Silver Nanoclusters: Coupling between Surface Plasmon and Emitter and Sensing of Lysozyme.

作者信息

Liu Xiaorong, Hu Ruoxin, Gao Zhidan, Shao Na

机构信息

College of Chemistry, Beijing Normal University, Beijing 100875, PR China.

出版信息

Langmuir. 2015 Jun 2;31(21):5859-67. doi: 10.1021/acs.langmuir.5b00589. Epub 2015 May 18.

Abstract

DNA-templated silver nanoclusters (DNA-AgNCs) have now been thrust into the limelight with their superior optical properties and potential biological applications. However, the origin of photoluminescence from DNA-AgNCs still remains unclear. In this work, DNA-AgNCs were synthesized and the photoluminescence properties as well as the biosensing applications of the designed DNA-AgNCs were investigated. The photoluminescence properties of the DNA-AgNCs were studied under three regions of excitation wavelength based on the UV-visible absorption spectra. It was deemed that the photoluminescence originated from coupling between the surface plasmon and the emitter in AgNCs when they were excited by visible light above 500 nm, and thus the emission wavelength varied with changing the excitation wavelength. The photoluminescence of the red-emitting-only AgNCs was the intrinsic fluorescence when excited from 200 to 400 nm, which was only related to the emitter; but for two components of blue- and red-emitting AgNCs, the emission wavelength varied with the excitation wavelength ranging from 300 to 360 nm, and the photoluminescence was a coupling between the surface plasmon and the emitter. The photoluminescence was only related to the surface plasmon when the AgNCs were excited from 400 to 500 nm. Four DNA probes were designed and each contained two parts: one part was the template used to synthesize AgNCs and it was same to all, and the other part was the lysozyme binding DNA (LBD) used to bind lysozyme and two kinds of LBD were studied. It was deemed that the difference in DNA bases, sequence, and secondary structure caused the synthesized DNA-AgNCs to be different in photoluminescence properties and sensing ability to lysozyme, and the sensing mechanism based on photoluminescence enhancement was also presented. This work explored the origin of photoluminescence and the sensing ability of DNA-AgNCs, and is hoped to make a better understanding of this kind of photoluminescence probe.

摘要

DNA模板化银纳米簇(DNA-AgNCs)凭借其卓越的光学性质和潜在的生物应用,如今已备受瞩目。然而,DNA-AgNCs光致发光的起源仍不明确。在这项工作中,合成了DNA-AgNCs,并研究了所设计的DNA-AgNCs的光致发光性质及其生物传感应用。基于紫外可见吸收光谱,在三个激发波长区域研究了DNA-AgNCs的光致发光性质。人们认为,当DNA-AgNCs被500nm以上的可见光激发时,其光致发光源于表面等离子体与银纳米簇中发射体之间的耦合,因此发射波长会随激发波长的变化而变化。仅发射红光的AgNCs在200至400nm激发时,其光致发光为固有荧光,仅与发射体有关;但对于发射蓝光和红光的AgNCs的两个组分,发射波长在300至360nm的激发波长范围内变化,且光致发光是表面等离子体与发射体之间的耦合。当AgNCs在400至500nm激发时,光致发光仅与表面等离子体有关。设计了四种DNA探针,每种探针包含两部分:一部分是用于合成AgNCs的模板,所有探针的这部分相同;另一部分是用于结合溶菌酶的溶菌酶结合DNA(LBD),研究了两种LBD。人们认为,DNA碱基、序列和二级结构的差异导致合成的DNA-AgNCs在光致发光性质和对溶菌酶的传感能力方面存在差异,还提出了基于光致发光增强的传感机制。这项工作探索了DNA-AgNCs的光致发光起源及其传感能力,希望能更好地理解这种光致发光探针。

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