Chen Tianhong, Wang Xiao, Alizadeh Mohammad Hossein, Reinhard Björn M
Department of Chemistry and The Photonics Center, Boston University, 590 Commonwealth Avenue, Boston, MA 02215, USA.
Microsyst Nanoeng. 2017;3. doi: 10.1038/micronano.2016.86. Epub 2017 Apr 10.
The encapsulation of individual pairs of plasmonic nanoparticles (NPs) in liposomes is introduced as a new strategy for utilizing plasmon coupling to monitor interactions between co-confined NPs in a nanoconfinement that ensures high local NP concentrations. We apply the approach to monitor transient binding contacts between noncovalently tethered 55 nm diameter gold NPs, which were functionalized with cytosine (C)-rich DNAs, in acidic and mildly basic buffer conditions. At pH = 8, a rich spectral dynamics indicates DNA-mediated transient binding and unbinding of co-confined NPs due to weak attractive interparticle interactions. A decrease in pH from 8 to 4 is observed to favor the associated state for some co-confined NPs, presumably due to a stabilization of the bound dimer configuration through noncanonical C-C bonds between the DNA-functionalized NPs. Plasmonic nanoemitters whose spectral response switches in response to chemical cues (in this work pH) represent optical transducers with a rich application space in chemical sensing, cell analysis and nanophotonics.
将单个等离激元纳米颗粒(NP)对封装在脂质体中,作为一种利用等离激元耦合来监测纳米限域中共定位NP之间相互作用的新策略,该纳米限域可确保高局部NP浓度。我们应用该方法监测在酸性和弱碱性缓冲条件下,用富含胞嘧啶(C)的DNA功能化的直径55 nm的非共价连接金NP之间的瞬态结合接触。在pH = 8时,丰富的光谱动力学表明,由于颗粒间弱吸引相互作用,共定位NP之间存在DNA介导的瞬态结合和解离。观察到pH从8降至4有利于一些共定位NP的缔合状态,这可能是由于DNA功能化NP之间通过非经典C-C键稳定了结合二聚体构型。光谱响应随化学信号(在本工作中为pH)切换的等离激元纳米发射器代表了在化学传感、细胞分析和纳米光子学中具有丰富应用空间的光学传感器。