Quantizing single-molecule surface-enhanced Raman scattering with DNA origami metamolecules

被引:167
作者
Fang, Weina [1 ,2 ,3 ]
Jia, Sisi [3 ]
Chao, Jie [4 ,5 ]
Wang, Liqian [3 ]
Duan, Xiaoyang [6 ,7 ]
Liu, Huajie [3 ,8 ]
Li, Qian [1 ,2 ]
Zuo, Xiaolei [1 ,2 ]
Wang, Lihua [3 ]
Wang, Lianhui [4 ,5 ,9 ]
Liu, Na [6 ,7 ]
Fan, Chunhai [1 ,2 ]
机构
[1] Shanghai Jiao Tong Univ, Sch Med, Renji Hosp, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Med, Renji Hosp, Inst Mol Med, Shanghai 200240, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, CAS Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China
[4] Nanjing Univ Posts & Telecommun, IAM, KLOEID, 9 Wenyuan Rd, Nanjing 210046, Jiangsu, Peoples R China
[5] Nanjing Univ Posts & Telecommun, Sch Mat Sci & Engn, 9 Wenyuan Rd, Nanjing 210046, Jiangsu, Peoples R China
[6] Max Planck Inst Intelligent Syst, Heisenbergstr 3, D-70569 Stuttgart, Germany
[7] Heidelberg Univ, Kirchhoff Inst Phys, Neuenheimer Feld 227, D-69120 Heidelberg, Germany
[8] Tongji Univ, Sch Chem Sci & Engn, Shanghai 200092, Peoples R China
[9] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, 500 Dongchuan Rd, Shanghai 200241, Peoples R China
基金
美国国家科学基金会; 国家重点研发计划;
关键词
NANOPARTICLES; NANOANTENNAS; DIMERS; LIGHT;
D O I
10.1126/sciadv.aau4506
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Tailored metal nanoclusters have been actively developed to manipulate light at the subwavelength scale for nanophotonic applications. Nevertheless, precise arrangement of molecules in a hot spot with fixed numbers and positions remains challenging. Here, we show that DNA origami metamolecules with Fano resonances (DMFR) can precisely localize single dye molecules and produce quantified surface-enhanced Raman scattering (SERS) responses. To enable tailored plasmonic permutations, we develop a general and programmable method for anchoring a set of large gold nanoparticles (L-AuNPs) on prescribed n-tuple docking sites of super-origami DNA frameworks. A tetrameric nanocluster with four spatially organized 80-nm L-AuNPs exhibits peak-and-dip Fano characteristics. The drastic enhancement at the wavelength of the Fano minimum allows the collection of prominent SERS spectrum for even a single dye molecule. We expect that DMFR provides physical insights into single-molecule SERS and opens new opportunities for developing plasmonic nanodevices for ultrasensitive sensing, nanocircuits, and nanophotonic lasers.
引用
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页数:8
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