Markina Anastasia, Muratov Alexander, Petrovskyy Vladislav, Avetisov Vladik
N. N. Semenov Federal Research Center for Chemical Physics Russian Academy of Sciences, Kosygina 4, 119991 Moscow, Russia.
Nanomaterials (Basel). 2020 Dec 15;10(12):2519. doi: 10.3390/nano10122519.
Ultra-sensitive elements for nanoscale devices capable of detecting single molecules are in demand for many important applications. It is generally accepted that the inevitable stochastic disturbance of a sensing element by its surroundings will limit detection at the molecular level. However, a phenomenon exists (stochastic resonance) in which the environmental noise acts abnormally: it amplifies, rather than distorts, a weak signal. Stochastic resonance is inherent in non-linear bistable systems with criticality at which the bistability emerges. Our computer simulations have shown that the large-scale conformational dynamics of a short oligomeric fragment of thermosrespective polymer, poly--isopropylmethacrylamid, resemble the mechanical movement of nonlinear bistable systems. The oligomers we have studied demonstrate spontaneous vibrations and stochastic resonance activated by conventional thermal noise. We have observed reasonable shifts of the spontaneous vibrations and stochastic resonance modes when attaching an analyte molecule to the oligomer. Our simulations have shown that spontaneous vibrations and stochastic resonance of the bistable thermoresponsive oligomers are sensitive to both the analyte molecular mass and the binding affinity. All these effects indicate that the oligomers with mechanic-like bistability may be utilized as ultrasensitive operational units capable of detecting single molecules.
许多重要应用都需要能够检测单分子的纳米级器件的超灵敏元件。人们普遍认为,传感元件不可避免地会受到周围环境的随机干扰,这将限制在分子水平上的检测。然而,存在一种现象(随机共振),其中环境噪声的作用异常:它放大而不是扭曲微弱信号。随机共振存在于具有双稳态出现临界性的非线性双稳态系统中。我们的计算机模拟表明,热响应性聚合物聚甲基丙烯酸异丙酯的短寡聚片段的大规模构象动力学类似于非线性双稳态系统的机械运动。我们研究的寡聚物表现出由传统热噪声激活的自发振动和随机共振。当将分析物分子连接到寡聚物上时,我们观察到自发振动和随机共振模式有合理的偏移。我们的模拟表明,双稳态热响应性寡聚物的自发振动和随机共振对分析物分子质量和结合亲和力都很敏感。所有这些效应表明,具有类似机械双稳态的寡聚物可作为能够检测单分子的超灵敏操作单元。