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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Optimizing rotary processes in synthetic molecular motors
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Optimizing rotary processes in synthetic molecular motors

机译：优化合成分子电动机的旋转过程

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摘要

We deal with the issue of quantifying and optimizing the rotation dynamics of synthetic molecular motors. For this purpose, the continuous four-stage rotation behavior of a typical light-activated molecular motor was measured in detail. All reaction constants were determined empirically. Next, we developed a Markov model that describes the full motor dynamics mathematically. We derived expressions for a set of characteristic quantities, i.e., the average rate of quarter rotations or "velocity," V, the spread in the average number of quarter rotations, D, and the dimensionless Peclet number, Pe = V/D. Furthermore, we determined the rate of full, four-step rotations (Ω_(eff)), from which we derived another dimensionless quantity, the "rotational excess," r.e. This quantity, defined as the relative difference between total forward (Ω_+) and backward (Ω_-) full rotations, is a good measure of the unidirectionality of the rotation process. Our model provides a pragmatic tool to optimize motor performance. We demonstrate this by calculating V, D, Pe, Ω_(eff), and r.e. for different rates of thermal versus photochemical energy input. We find that for a given light intensity, an optimal temperature range exists in which the motor exhibits excellent efficiency and unidirectional behavior, above or below which motor performance decreases.
机译：我们处理量化和优化合成分子电动机旋转动力学的问题。为此，详细测量了典型的光激活分子马达的连续四阶段旋转行为。所有反应常数均凭经验确定。接下来，我们开发了一个马尔可夫模型，该数学模型描述了完整的电机动力学。我们导出了一组特征量的表达式，即四分之一旋转或“速度”的平均速率V，四分之一旋转的平均数的扩展D和无量纲的Peclet数Pe = V / D。此外，我们确定了完整的四步旋转的速率（Ω_（eff）），由此得出了另一个无量纲的量，即“旋转过量”，即r。该量定义为正向总旋转（Ω_+）与反向总旋转（Ω_-）之间的相对差，可以很好地衡量旋转过程的单向性。我们的模型提供了一种实用的工具来优化电机性能。我们通过计算V，D，Pe，Ω_（eff）和r.e来证明这一点。用于不同的热能和光化学能输入速率。我们发现，对于给定的光强度，存在一个最佳温度范围，在该温度范围内，电动机表现出出色的效率和单向性能，高于或低于该温度范围，电动机性能就会下降。

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  • 作者

    Edzard M. Geertsema; Sense Jan van der Molen; Marco Martens; Ben L. Feringa;

  • 作者单位

    Stratingh Institute for Chemistry, University of Groningen, Nijenborgh 4, 9747 AG, Groningen, The Netherlands University of Edinburgh, School of Chemistry, The King's Buildings, West Mains Road, Edinburgh EH9 3JJ, United Kingdom;

    Kamerlingh Onnes Laboratorium,Leiden University, Niels Bohrweg 2, 2333 CA Leiden, The Netherlands;

    Institute for Mathematical Sciences, State University of New York at Stony Brook,Stony Brook, NY 11794-3651;

    Stratingh Institute for Chemistry, University of Groningen, Nijenborgh 4, 9747 AG, Groningen, The Netherlands;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Markov model; unidirectional rotation;

    机译：马尔可夫模型单向旋转;

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