LDAO对Rhodobacter azotoformans外周捕光复合体LH2构象及其细菌叶绿素解离行为的影响

为探求LDAO与LH2的相互作用关系和规律,深入认识LDAO对LH2结构和功能的影响。采用光谱法系统地研究了LDAO对Rhodobacter azotoformans134K20菌株LH2构象及其在极端环境中细菌叶绿素(BChl)解离行为的影响。结果表明:(1)在室温pH 8.0缓冲溶液中,LDAO导致LH2构象变化,α-螺旋含量提高,Tyr和B850细菌叶绿素特征峰蓝移,能量传递效率提高。(2)在60℃pH 8.0缓冲溶液中,LH2B800和B850细菌叶绿素可解离为游离BChl。LDAO能增加LH2的高温稳定性,延缓并改变B800和B850解离过程和行为。(3)在室温强酸和强碱溶液中,LDAO加剧了B800和B850的解离并分别转化为游离细菌脱镁叶绿素(BPhe)和游离BChl,表现出不同的解离行为。在不含LDAO的强酸溶液中,B850呈现先解离再自组装的过程。LDAO作用于LH2,可使其B800和B850在不同极端环境中的解离行为发生变化。     

紫细菌Rb. Sphaeroides 601外周捕光天线(LH2) B800吸收带的超快动力学研究

利用从紫细菌Rb.sphaeroides 601 所提取出的外周捕光天线LH2以及其不同pH值酸化样品(部分和全部去除B800分子LH2)并采用不同波长下的飞秒单色抽运探测技术详细研究了LH2中B800吸收带内的激发态动力学过程.通过对野生型与部分/完全去B800分子LH2的比较研究,分析了B800吸收带激发后所表现出的丰富变化的动力学过程,研究结果表明激发B800带的动力学过程中包含着B850上激子带的直接激发而产生的对激发态动力学的贡献.     

紫细菌Rb.Sphaeroides 601外周捕光天线(LH2) B800吸收带的超快动力学研究

利用从紫细菌Rb.sphaeroides 601 所提取出的外周捕光天线LH2以及其不同pH值酸化样品(部分和全部去除B800分子LH2)并采用不同波长下的飞秒单色抽运探测技术详细研究了LH2中B800吸收带内的激发态动力学过程.通过对野生型与部分/完全去B800分子LH2的比较研究，分析了B800吸收带激发后所表现出的丰富变化的动力学过程，研究结果表明激发B800带的动力学过程中包含着B850上激子带的直接激发而产生的对激发态动力学的贡献. 关键词： 紫细菌外周捕光天线LH2 部分和全部去除B800分子LH2 激发态动力学的演变 飞秒抽运探测     

紫细菌捕光天线LH2中的超快光物理研究

采用飞秒泵浦探测技术研究了紫细菌外周捕光天线LH2中的超快光动力学过程.从B800蓝侧的激发态动力学中观察到B800到B850的能量传递时间,实验结果与理论计算结果的差别说明激发B800时可能引起B850上激子带的直接激发,或存在由B800到B850上激子态的能量传递通道.在B800红侧激发的动力学过程中,漂白信号前端存在的一个快速光吸收信号主要来源于B850上激子带的直接激发.在天然RS601和突变体GM309的LH2中,800 nm激发时的动力学过程都表现为一个类似的光漂白过程,动力学曲线的衰减时间常量在天然LH2中明显快于突变体中,说明在GM309中B800到B850的激发能传递速率有所降低.而在845 nm激发下两个样品中的快过程类似,但慢过程在GM309中有所增快,激发态中的能量重新分布包括逆向的能量传递也受到类胡萝卜素微结构的影响.     

紫色光合细菌中类胡萝卜素的选择性分布及功能

紫色光合细菌Rhodopseudomonas (Rps.) palustris光合膜中的外周捕光天线(LH2)及核心复合物(LH1-RC)中都含有多种类胡萝卜素分子(Crt)。研究不同种类的Crt在上述色素蛋白复合物中的分布及其生理学功能具有重要意义。采用了高效液相色谱(HPLC)手段分析了中等光强(～4 000 lux)培养条件下所获得的Rps. palustris的LH2及LH1-RC中的Crt组成,发现共轭双键数目(n)为11或12的类胡萝卜素分子(包括lycopene(n=11),Anhydrorhodivibrin(n=12)及Rhodopin(n=12)等,主要集中在LH2复合物中,而n=13的类胡萝卜素分子Spirilloxanthin则优先结合到LH1-RC中。通过将稳态吸收光谱及近红外荧光激发光谱在细菌叶绿素的Qx带处归一化,并比较两者的数值,发现在LH2中Crt从单重态向BChl的传能效率［30.9%(v=0),25.4%(v=1),30.4%(v=2)］明显高于在LH1-RC中的传能效率［10.7%(v=0),7.8%(v=1),11.4%(v=2)］。此外,本文还运用亚微秒时间分辨吸收光谱检测了类胡萝卜素三重态T_n←T₁吸收,发现伴随着532 nm激光脉冲激发,LH1-RC和LH2中Crt三重态的吸收主峰位于571及560 nm左右,它们分别归属于n=13和n=12的类胡萝卜素分子。通过对动力学衰减曲线进行单指数拟合,发现前者的衰减时间常数(1.6 μs)明显短于后者(2.2 μs)。上述研究结果表明,短链Crt易于结合到LH2中承担捕光的功能,而长链Crt优先结合到LH1-RC中发挥光保护功能。     

Energy Transfer in the Light-Harvesting Complexes of Purple Bacteria

In this paper, we use a nonlinear decohering quantum model to study the initial step of photosynthesis which is an ultrafast transfer process of absorption the sunlight by light-harvesting complexes and electronic excitation transfer to the reaction center (RC). In this decohering model, the Hamiltonian of the system commutes with the systemenvironment interaction. We take B850 ring of light-harvesting complex Ⅱ (LH-Ⅱ) in purple bacteria as an example to calculate the efficiency of the energy transfer as a function of time. We find that the environmental noise can make the LH-Ⅱ have stable energy transfer efficiency over a long time. This is to say that the environmental noise which is the decohering source has advantage of the energy transfer in the process of photosynthesis.     

Energy Transfer in the Light-Harvesting Complexes of Purple Bacteria

In this paper, we use a nonlinear decohering quantum model to study the initial step of photosynthesis which is an ultrafast transfer process of absorption the sunlight by light-harvesting complexes and electronic excitation transfer to the reaction center(RC). In this decohering model, the Hamiltonian of the system commutes with the systemenvironment interaction. We take B850 ring of light-harvesting complex II(LH-II) in purple bacteria as an example to calculate the efficiency of the energy transfer as a function of time. We find that the environmental noise can make the LH-II have stable energy transfer efficiency over a long time. This is to say that the environmental noise which is the decohering source has advantage of the energy transfer in the process of photosynthesis.     

Excitonic level structures of LH1 and LH2 of purple photosynthetic bacteria using an analytical approach

The excitonic level structure of a ring-like chain of dimers is discussed analytically in order to aid the understanding of the possible spectral properties of LH1 and LH2 of purple photosynthetic bacteria. Under the approximation of dipole－dipole interaction between Bchls, the excitonic levels, bandwidths and energy gap between two Davydov subbands are expressed analytically in terms of interaction energies and configurational parameters of dipoles. Our model includes all the interactions between pigment molecules in the system. The oscillator strengths and circular dichroism (CD) for the excitonic states are also presented analytically. The simulated absorption and CD spectra of LH1 and LH2 complexes reproduce the main features of the measured results.     

Quantum Dynamics of Entanglement and Single Excitation Transfer in LH1-RC-Type Trimer

In this paper, we study quantum dynamics of entanglement and single excitation transfer (SET) in an LH1-RC-type trimer which can describe a basic unit cell in the LH1-RC complex in the photosynthetic process. It is shown that there exists a sudden change of entanglement at the critic point of quantum phase transition (QPT) of the system at low temperatures, the entanglement sudden change caused by the QPT is suppressed at higher temperatures. We investigate the influence of environment on entanglement and SET. We show the generation of the dephasing-assisted entanglement between a donor and an acceptor and the existence of the steady-state entanglement, and demonstrate the entanglement transfer from donor-donor entanglement to donor-acceptor entanglement in the dynamic evolution. We reveal the close relation between the SET probability and donor-acceptor entanglement. Especially, we find that the SET probability is proportional to the amount of donor-acceptor entanglement under certain conditions.     

碳量子点/罗丹明B分子复合体系中的能量和电子转移过程研究

本文采用荧光光谱结合稳态和瞬态吸收光谱技术,研究了碳量子点(CQDs)/罗丹明B(RhB)分子复合体系o-CQDs/RhB和m-CQDs/RhB中的能量转移和电子转移过程以及它们之间的关系. 研究发现在能量转移效率为73.2%的o-CQDs/RhB体系中,电子转移过程可以忽略;而在能量转移效率低于33.5%的m-CQDs/RhB体系中,电子转移过程则较为显著. 在这个由碳量子点和染料分子组成的典型复合体系中所揭示的能量转移与电子转移过程之间的内联关系,将为与激子猝灭相关的应用提供有用的视角.     

碳量子点-VB2荧光共振能量转移法测定VB2

用微波法合成了具有发光特性的CDs,以发射波长为447nm的CDs为供体,维生素B2 (VB2)为受体,建立了一种以十六烷基三甲基溴化铵(CTAB)为介质的荧光共振能量体系检测VB2含量的方法.结果表明:在pH=7.1时,VB2的浓度与Fa/Fd值在1.8×10-8-3.0×10-7mol/L范围内呈线性关系,其线性方程为Fa/Fd=0.0766C(×10-8mol/L)+0.5658,相关系数为0.9996,检出限为8.3×10-9 mol/L.     

激发态Cs2和H2的电子-振转能级的碰撞转移

利用相干反斯托克斯拉曼光谱(CARS)探测技术, 研究了激发态Cs2与H2间的电子-振转能级的碰撞转移。用波长为532 nm和中心波长为716 nm的两束激光同时聚焦到样品池中, 扫描CARS谱确认了H2分子的S支(△v =1, △J=2)仅在v=1, J=4,5及v=2, J=3,4能级上有布居, 用n1、n2、n3、n4分别表示(2,4)、(2,3)、(1,4)及(1,5)上的粒子数密度。从CARS线的峰值得到n2/n1、n3/n1、n4/n1分别为6.34±1.27、3.66±0.73和1.45±0.29。转移能配置到振动、转动和平动的比例分别为0.44、0.06和0.50, 能量主要分配在振动和平动上。在T=523 K和PH2=2.5×103 Pa条件下, 通过求解速率方程组和对时间分辨CARS线轮廓的分析, 得到碰撞转移速率系数k1=(6.0±1.2)×10-14 cm-3s-1和k2=(4.0±0.8)×10-13cm-3 s-1。