Quantum coherence in single biomolecules measured by multidimensional optical micro-spectroscopy

生命是建立在多种生物分子之间错综复杂的相互作用的基础上的，包括脂质、蛋白质和DNA。它们本质上是动态的，并维持着生命的非平衡状态。为了了解生命的机制，分子之间的相互作用作为长期进化的结果进行了微调。虽然许多机制可以用利用浓度空间梯度的局域平衡的非平衡热力学来描述，但也有一些例子表明了分子络合物上激发态的量子相干的重要性[10.1098/rsif.2018.0640]。具体地说，在感觉(嗅觉、视觉)和光合作用的功能中，长距离相干耦合(例如通过偶极-偶极相互作用)和局部振动耦合之间的相互作用是一个正在研究的有趣机制[10.1126/Science.1235820]。在导师实验室开发先进激光显微光谱技术的开创性工作的基础上，本项目将研究单个生物分子功能单元的相干量子动力学。您将从半导体纳米结构的研究[10.1038/nComms2764，0.1038/nPhoon.2016.2]向这一雄心勃勃的目标转化为我们实验室开发和获得的二维相干显微光谱技术“外差光谱干涉法”。捕光复合体中相干的演化将从预期长寿命相干的低温(5K)一直到室温，在室温下，热激发缩短相干时间，生物分子处于其工作范围内。这将使您能够确定消相干的机制，并验证大自然是否在相关生物(如藻类和硫磺/紫色细菌)的生存条件下调节了最佳平衡。利用这一洞察力，我们计划研究人工采光结构中的这些相干性[10.1126/Science.1249771]，以了解和优化它们的性能。

Life is based on the intricate interactions between a multitude of biomolecules, including lipids, proteins, and DNA. They are dynamical in nature and maintain the non-equilibrium state of life. To understand the machinery of life, the interactions between the molecules are finely tuned as a result of long-term evolution. While many mechanisms can be described by non-equilibrium thermodynamics making use of local equilibrium with spatial gradients of concentrations, some examples have been highlighted which show the importance of quantum coherence of excitations over molecular complexes [10.1098/rsif.2018.0640]. Specifically in the functions of sensing (smell, vision) and photosynthesis, the interplay between long range coherent coupling, e.g. via dipole-dipole interaction, and coupling to local vibrations, is an intriguing mechanism being investigated [10.1126/science.1235820]. Building on the pioneering work of the supervisor's laboratory in developing advanced laser micro-spectroscopy techniques, this project will investigate the coherent quantum dynamics of single biomolecule functional units.You will translate the two-dimensional coherent micro-spectroscopy technique "Heterodyne Spectral Interferometry", developed and available in our laboratory, from the investigations of semiconductor nanostructures [10.1038/ncomms2764, 0.1038/nphoton.2016.2], towards this ambitious goal. The evolution of the coherence in light-harvesting complexes will be studied from low temperatures (5K), where long lived coherence is expected, up to room temperature, where the thermal excitations reduce the coherence time and the biomolecules are in their operating range. This will allow you to identify the mechanisms of decoherence and verify if nature has tuned the balance optimally at living conditions of the related organisms, such as algae, and sulphur/purple bacteria. Using this insight, we plan to study these coherences in artificial light-harvesting structures [10.1126/science.1249771], which are being developed as a green energy source, in order to understand and optimize their performance.