Tao Li, Chen Kun, Chen Zefeng, Cong Chunxiao, Qiu Caiyu, Chen Jiajie, Wang Ximiao, Chen Huanjun, Yu Ting, Xie Weiguang, Deng Shaozhi, Xu Jian-Bin
Department of Electronic Engineering , The Chinese University of Hong Kong , Shatin, N.T., Hong Kong SAR , China.
State Key Laboratory of Optoelectronic Materials and Technologies, School of Electronics and Information Technology and Guangdong Province Key Laboratory of Display Material , Sun Yat-sen University , Guangzhou 510275 , China.
J Am Chem Soc. 2018 Jul 18;140(28):8696-8704. doi: 10.1021/jacs.8b02972. Epub 2018 Jul 5.
Plasmon-free surface enhanced Raman scattering (SERS) based on the chemical mechanism (CM) is drawing great attention due to its capability for controllable molecular detection. However, in comparison to the conventional noble-metal-based SERS technique driven by plasmonic electromagnetic mechanism (EM), the low sensitivity in the CM-based SERS is the dominant barrier toward its practical applications. Herein, we demonstrate the 1T' transition metal telluride atomic layers (WTe and MoTe) as ultrasensitive platforms for CM-based SERS. The SERS sensitivities of analyte dyes on 1T'-W(Mo)Te reach EM-comparable ones and become even greater when it is integrated with a Bragg reflector. In addition, the dye fluorescence signals are efficiently quenched, making the SERS spectra more distinguishable. As a proof of concept, the SERS signals of analyte Rhodamine 6G (R6G) are detectable even with an ultralow concentration of 40 (400) fM on pristine 1T'-W(Mo)Te, and the corresponding Raman enhancement factor (EF) reaches 1.8 × 10 (1.6 × 10). The limit concentration of detection and the EF of R6G can be further enhanced into 4 (40) fM and 4.4 × 10 (6.2 × 10), respectively, when 1T'-W(Mo)Te is integrated on the Bragg reflector. The strong interaction between the analyte and 1T'-W(Mo)Te and the abundant density of states near the Fermi level of the semimetal 1T'-W(Mo)Te in combination gives rise to the promising SERS effects by promoting the charge transfer resonance in the analyte-telluride complex.
基于化学机制(CM)的无等离子体表面增强拉曼散射(SERS)因其可控分子检测能力而备受关注。然而,与由等离子体电磁机制(EM)驱动的传统基于贵金属的SERS技术相比,基于CM的SERS的低灵敏度是其实际应用的主要障碍。在此,我们展示了1T'过渡金属碲化物原子层(WTe和MoTe)作为基于CM的SERS的超灵敏平台。分析物染料在1T'-W(Mo)Te上的SERS灵敏度达到了与EM相当的水平,并且当它与布拉格反射器集成时甚至更高。此外,染料荧光信号被有效淬灭,使得SERS光谱更易于区分。作为概念验证,即使在原始的1T'-W(Mo)Te上超低浓度为40(400)fM的情况下,分析物罗丹明6G(R6G)的SERS信号也可检测到,并且相应的拉曼增强因子(EF)达到1.8×10(1.6×10)。当1T'-W(Mo)Te集成在布拉格反射器上时,R6G的检测极限浓度和EF可分别进一步提高到4(40)fM和4.4×10(6.2×10)。分析物与1T'-W(Mo)Te之间的强相互作用以及半金属1T'-W(Mo)Te费米能级附近丰富的态密度共同作用,通过促进分析物 - 碲化物复合物中的电荷转移共振产生了有前景的SERS效应。