Relation between Dephasing Time and Energy Gap Fluctuations in Biomolecular Systems.
Relation between Dephasing Time and Energy Gap Fluctuations in Biomolecular Systems.
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DOI：
10.1021/acs.jpclett.6b00134
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发表时间：
2016-03
期刊：
影响因子：
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通讯作者：
M. I. Mallus;Mortaza Aghtar;Suryanarayanan Chandrasekaran;Gesa Lüdemann;M. Elstner;U. Kleinekathöfer
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文献类型：
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作者：
M. I. Mallus;Mortaza Aghtar;Suryanarayanan Chandrasekaran;Gesa Lüdemann;M. Elstner;U. Kleinekathöfer
激发能和电荷转移是生物系统中的基本过程。由于它们的量子性质，退相对这些过程的影响是令人感兴趣的，特别是在试图了解它们的效率时。此外，最近的实验表明，在这样的系统中存在量子相干。作为更好地理解的第一步，我们研究了退相时间与单个分子亚基的能隙涨落之间的关系。为了阐明这种依赖关系，已经进行了一组更大的分子模拟。这一组包括Fenna-Matthews-Olson复合体、PE545聚集体、LH2复合体、DNA、光解酶和隐色素中的细菌-叶绿素。对于这些聚集体的各个分子亚基，已经定量地证实了退相时间与平均能隙能涨落之间存在反比。然而，对于包括各自的分子间偶联在内的整个络合物，这种关系仍然需要验证。
Excitation energy and charge transfer are fundamental processes in biological systems. Because of their quantum nature, the effect of dephasing on these processes is of interest especially when trying to understand their efficiency. Moreover, recent experiments have shown quantum coherences in such systems. As a first step toward a better understanding, we studied the relationship between dephasing time and energy gap fluctuations of the individual molecular subunits. A larger set of molecular simulations has been investigated to shed light on this dependence. This set includes bacterio-chlorophylls in Fenna-Matthews-Olson complexes, the PE545 aggregate, the LH2 complexes, DNA, photolyase, and cryptochromes. For the individual molecular subunits of these aggregates it has been confirmed quantitatively that an inverse proportionality exists between dephasing time and average gap energy fluctuation. However, for entire complexes including the respective intermolecular couplings, such a relation still needs to be verified.