(Peer-Reviewed) Coulomb attraction driven spontaneous molecule-hotspot paring enables universal, fast, and large-scale uniform single-molecule Raman spectroscopy
	
		Lihong Hong 洪丽红 ¹ ²,  Haiyao Yang 杨海遥 ¹,  Jianzhi Zhang 张简智 ¹,  Zihan Gao 高子涵 ¹,  Zhi-Yuan Li 李志远 ¹ ³
			
				¹ School of Physics and Optoelectronics, South China University of Technology, Guangzhou 510640, China
中国 广州 华南理工大学物理与光电学院
² Institute of Physics, Henan Academy of Sciences, Zhengzhou 450046, China
中国 郑州 河南省科学院物理研究所
³ State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, China
中国 广州 华南理工大学发光材料与器件国家重点实验室
			
			
				Opto-Electronic Advances, 2025-07-17
			
		
		
			
		
		
	 
	
	
	Abstract
Raman spectroscopy offers a great power to detect, analyze and identify molecules, and monitor their temporal dynamics and evolution when combined with single-molecule surface-enhanced Raman scattering (SM-SERS) substrates. Here we present a SM-SERS scheme that involves simultaneously giant chemical enhancement from WS2 2D materials, giant electromagnetic enhancement from plasmonic nanogap hot spot, and inhibition of molecular fluorescence influence under near-infrared laser illumination. 
Remarkably we find Coulomb attraction between analyte and gold nanoparticle can trigger spontaneous formation of molecule-hotspot pairing with high precision, stability and robustness. The scheme has enabled realization of universal, robust, fast, and large-scale uniform SM-SERS detection for three Raman molecules of rhodamine B, rhodamine 6G, and crystal violet with a very low detection limit of 10−16 M and at a very fast spectrum acquisition time of 50 ms.
	
	
	
	
	
	
		    
		    
    			
		    
    			
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