单分子配分函数的可视化与热力学编码
Visualization and thermodynamic encoding of single-molecule partition functions
摘要：
分子态的包络平均是实验测定热力学量的基础。一个特殊的情况下发生的单分子的调查平衡条件下，自由能，熵和焓在有限的温度是具有挑战性的，以确定与整体平均单独。在这里，我们提供了一种方法来访问单分子热力学，通过将单个分子限制在二维金属有机纳米网的纳米级孔中，在那里我们使用温度控制的扫描隧道显微镜直接记录有限温度时间平均统计权重。所得到的图案代表一个真正的空间平衡概率分布。我们将此分布与配分函数投影相关联，以通过计算建模来评估空间分辨的热力学量。所提出的基于分子动力学的玻尔兹曼加权模型能够高精度地再现实验观察到的分子状态。通过计算机定制的能量景观，我们证明了不同的概率分布可以在不同的温度下加密。这种调制提供了将信息编码和解码到位置-温度空间或实现纳米级热探针的手段。
英文摘要：
Ensemble averaging of molecular states is fundamental for the experimental determination of thermodynamic quantities. A special case occurs for single-molecule investigations under equilibrium conditions, for which free energy, entropy and enthalpy at finite-temperatures are challenging to determine with ensemble-averaging alone. Here, we provide a method to access single-molecule thermodynamics, by confining an individual molecule to a nanoscopic pore of a two-dimensional metal-organic nanomesh, where we directly record finite-temperature time-averaged statistical weights using temperature-controlled scanning tunneling microscopy. The obtained patterns represent a real space equilibrium probability distribution. We associate this distribution with a partition function projection to assess spatially resolved thermodynamic quantities, by means of computational modeling. The presented molecular dynamics based Boltzmann weighting model is able to reproduce experimentally observed molecular states with high accuracy. By an in-silico customized energy landscape we demonstrate that distinct probability distributions can be encrypted at different temperatures. Such modulation provides means to encode and decode information into position-temperature space or to realize nanoscopic thermal probes.
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