Abstract：
To date, studies on the thermodynamic and kinetic processes that underlie biological function and nanomachine actuation in biological- and biology-inspired molecular constructs have primarily focused on photothermal heating of ensemble systems, highlighting the need for probes that are localized within the molecular construct and capable of resolving single-molecule response. Here we present an experimental demonstration of wavelength-selective, localized heating at the single-molecule level using the surface plasmon resonance of a 15 nm gold nanoparticle (AuNP). Our approach is compatible with force-spectroscopy measurements and can be applied to studies of the single-molecule thermodynamic properties of DNA origami nanomachines as well as biomolecular complexes. We further demonstrate wavelength selectivity and establish the temperature dependence of the reaction coordinate for base-pair disruption in the shear-rupture geometry, demonstrating the utility and flexibility of this approach for both fundamental studies of local (nanometer-scale) temperature gradients and rapid and multiplexed nanomachine actuation.
摘要：
迄今为止,对生物和生物学启发的分子构造中生物功能和纳米机器致动的热力学和动力学过程的研究主要集中在合奏系统的光热加热上，强调了对定位在分子构建体中并能够解决单分子反应的探针的需求。在这里，我们提出了波长选择的实验演示，使用15nm金纳米粒子（AuNP）的表面等离子体共振在单分子水平上进行局部加热。我们的方法与力光谱测量兼容，可用于研究DNA折纸纳米机器以及生物分子复合物的单分子热力学性质。我们进一步证明了波长选择性，并建立了剪切破裂几何形状中碱基对破坏的反应坐标的温度依赖性，证明了这种方法对于局部（纳米级）温度梯度和快速和多路纳米机器驱动的基础研究的实用性和灵活性。
