Self-Assembly from a Single-Molecule Perspective
Self-Assembly from a Single-Molecule Perspective
复制标题
从单分子角度看自组装
DOI：
10.1007/978-3-030-24202-2_11
复制
发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Ghosh, P.
中科院分区：
文献类型：
--
作者：
Pilkiewicz, K.R.;Rana, P.;Mayo, M.L.;Ghosh, P.
随着在单分子水平上操纵超分子和纳米级结构的自组装越来越成为常态，必须建立新的理论支架来取代用于描述传统体相活性合成的基于热力学和动力学的模型。像统计力学支持这些后者的理论，我们提出的框架使用状态概率作为其基本对象;但是，与吉布斯范式相反，我们的理论直接建模的初始和最终状态的轨迹之间的转移概率，之前需要假设遍历性。我们利用这些概率的上下文中的分子自组装计算的总体可能性，一个特定的实验条件下，导致一个理想的结构结果。我们展示了这个框架的应用程序，一个简单的玩具模型中，三个相同的分子可以组装在两种方式之一，并得出结论，讨论如何通过近似扩展到更大，更复杂的系统时，可以克服这样一个细粒度的模型的高计算成本。
As manipulating the self-assembly of supramolecular and nanoscale constructs at the single-molecule level increasingly becomes the norm, new theoretical scaffolds must be erected to replace the thermodynamic and kinetics based models used to describe traditional bulk phase active syntheses. Like the statistical mechanics underpinning these latter theories, the framework we propose uses state probabilities as its fundamental objects; but, contrary to the Gibbsian paradigm, our theory directly models the transition probabilities between the initial and final states of a trajectory, foregoing the need to assume ergodicity. We leverage these probabilities in the context of molecular self-assembly to compute the overall likelihood that a specified experimental condition leads to a desired structural outcome. We demonstrate the application of this framework to a simple toy model in which three identical molecules can assemble in one of two ways and conclude with a discussion of how the high computational cost of such a fine-grained model can be overcome through approximation when extending it to larger, more complex systems.
影响因子：
4
作者：
S. Xin;P. Wang;A. Yin;C. Kim;M. Dobrowolska;J. Merz;J. Furdyna
通讯作者：
S. Xin;P. Wang;A. Yin;C. Kim;M. Dobrowolska;J. Merz;J. Furdyna
影响因子：
62.1
作者：
Chakrabarty, Rajesh;Mukherjee, Partha Sarathi;Stang, Peter J.
通讯作者：
Stang, Peter J.