title: Sequence-Modulated Interactions between Single Multivalent DNA-Conjugated Gold Nanoparticles.
abstract: DNA-conjugated gold nanoparticle (AuNP) is an attractive building block to construct elegant plasmonic nanomaterials by self-assembly but the complicated interaction between multivalent nanoconjugates governing the assembly process and the properties of assembled structures remains poorly understood. Herein, with an in situ kinetic single-particle imaging method, we report the dynamic interaction between single multivalent DNA-conjugated AuNPs quantitatively depends on the nucleic acid sequence in nanoconjugates. From the binding dynamics analysis, it was found that the binding of nanoconjugates with DNA length longer than nine bases is kinetically irreversible and the binding rate is dependent on both the sequence length and GC content, enabling us to predict the rational modulation of binding rates of individual building blocks for stepwise assembly. Moreover, the reversibility for the multivalent interaction between single nanoconjugates at constant temperature can be reinstated by adopting the DNA sequence with single-nucleotide mismatch and the lifetime for nanoconjugates at bound state can be tailored by changing the mismatch positions in DNA strands, providing new opportunity to create active nanostructures with controlled dynamic properties. All these findings provide new insights for understanding the multivalent interaction during the assembly process at the single-nanoconjugate level and predicting the programmable self-assembly of engineered nanoconjugates for the fabrication of dynamic nanomaterials.
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Chunyan
authors.initials: C
authors.lastname: Qiao
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Jia
authors.initials: J
authors.lastname: Wu
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Zhenrong
authors.initials: Z
authors.lastname: Huang
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Xuan
authors.initials: X
authors.lastname: Cao
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Jiayu
authors.initials: J
authors.lastname: Liu
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.
authors.forename: Bin
authors.initials: B
authors.lastname: Xiong
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.|Department of Chemistry, Tsinghua University , Beijing, 100084, P. R. China.
authors.forename: Yan
authors.identifier: 0000-0001-7133-0558
authors.initials: Y
authors.lastname: He
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, P. R. China.|Department of Chemistry, Iowa State University , Ames, Iowa 50011, United States.
authors.forename: Edward S
authors.initials: ES
authors.lastname: Yeung
mesh_terms: D020137:Base Pair Mismatch; D001483:Base Sequence; D004247:DNA / Q000737:chemistry*; D006046:Gold / Q000737:chemistry*; D007700:Kinetics; D053768:Metal Nanoparticles / Q000737:chemistry*; D008853:Microscopy; D008962:Models, Theoretical
chemical_list: D006046:Gold; D004247:DNA