生物学中的量子效应:光合系统中激子运动的主方程研究
Quantum effects in biology: master equation studies of exciton motion in photosynthetic systems
AI总结:
本研究针对光合系统激子长时程量子相干效应无法用传统半经典及微扰主方程解释的问题,总结了自研的非微扰研究方法,并介绍了2D光子回波光谱技术的物理原理。
摘要:
本综述聚焦我们近期针对光合系统中激子运动开展的研究。在光合作用过程中,光子被吸收后会在光合色素的天线复合物中产生一个激子。随后该激子会沿着FMO复合物这类链状生物分子迁移至反应中心,并在那里启动最终生成生物质的化学反应。近期实验观测发现,激子运动本质上具有高度量子力学特性,即涉及长时程(约600飞秒)量子相干效应。Forrester理论等传统半经典理论以及二阶玻恩主方程均不适用。我们阐明了二阶玻恩非马尔可夫主方程及其马尔可夫极限(也称为Redfield主方程)无法解释观测到的长相干性的原因。简言之,原因在于这些方法本质上是微扰性的,而在实际的捕光系统中,各类耦合作用(系统-系统耦合与系统-浴耦合)的量级相近。目前学界正开发多种新方法,以突破上述两种极限理论的局限。本综述并非通常意义上的综述,因为我们仅总结自身提出的方法,仅在提及其他方法时引用相关文献。文末还简要介绍了精密的2D光子回波光谱技术,重点阐述了多维回波光谱学的基础物理原理。
英文摘要:
The present review is devoted to our recent studies on the excitonic motion in photosynthetic systems. In photosynthesis, the light photon is absorbed to create an exciton in the antenna complex of the photosynthetic pigments. This exciton then migrates along the chain-biomolecules, like FMO complex, to the reaction centre where it initiates the chemical reactions leading to biomass generation. Recently, it has been experimentally observed that the exciton motion is highly quantum mechanical in nature i.e., it involve long time ($\sim 600$ femto sec) quantum coherence effects. Traditional semiclassical theories like Forrester's and second Born master equations cannot be applied. We point out why the 2nd Born non-Markovian master equation and its Markovian limit (also called the Redfield master equation) cannot be used to explain the observed long coherences. Briefly, the reason is that these approaches are perturbative in nature and in real light harvesting systems various couplings (system-system and system-bath) are of the similar order of magnitude. Various new approaches are being developed to go beyond the above two limiting theories. The present review is not a review in the usual sense of the word as we summarize our own approaches and only refer to the literature for the other ones. A brief introduction to the sophisticated 2D photon echo spectroscopy is also given at the end with an emphasis on the underlying physics of the multidimensional echo spectroscopies.
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