高等植物外周捕光天线LHCⅡ中的超快光动力学过程

利用飞秒抽运探测技术及时间分辨荧光(TRPL)等光谱技术对高等植物LHCⅡ中的超快光动力学过程进行了研究。在其时间分辨荧光光谱中表现出了明显的各向异性特性。实验上观察了LHCⅡ中色素间的能量传递过程,由飞秒动力学发现,单体内Chlb到邻近的Chla之间的能量传递在200～300fs的时间尺度,Chla激子带间的能量弛豫发生在几百飞秒,不同单体Chla分子间能量分布过程在几个皮秒。而时间分辨荧光和飞秒动力学过程中上百皮秒的慢过程归属于不同聚集体间的能量平衡过程或分子构象变化。     

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. 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     

假根羽藻外周天线LHCⅡ寡聚体的瞬态吸收光谱(英文)

采用时间分辨瞬态吸收光谱技术研究了假根羽藻外周天线寡聚体的光保护机制.分别以667nm飞秒激光脉冲和白光脉冲作为泵浦光和探测光,探测光与泵浦光之间的延时范围和准确度分别为340ps和134fs.实验结果表明在泵浦光激发之后外周天线对探测光的吸收是动态变化的.对瞬态吸收光谱进行多指数拟合,并结合外周天线的荧光发射谱和激发谱进行分析,结果表明:500~600nm的瞬态吸收谱主要来源于类胡萝卜素分子,外周天线寡聚体至少包含四种具有光保护作用的类胡萝卜素分子,对应的S0→Sn跃迁光谱为511nm和554nm,522nm和541nm,530nm和563nm(对应管藻黄素),536nm和575nm;类胡萝卜素分子以两种方式参与到光保护过程中:一种是直接方式,在几皮秒范围内猝灭叶绿素三重态;另一种是间接方式,在几百皮秒范围内猝灭从叶绿素分子获得能量的单线态氧.     

捕光天线色素分子到反应中心光能传递机理研究

利用皮秒和飞秒时间分辨光谱技术研究了PSⅡ捕光天线β-car分子和Chla分子传递光能到反应中心的机理，β-car分子接收到514.5nm光能之后，将能量主要以Dexter电子交换机理传递给相邻ε-car分子或Chla分子以后，再以Forster共振传能机理通过Chla分子向相邻Chal分子单步传递，最终以250ps的时间传递到反应中心，理论计算值为267ps。捕光天线中的Chla分子接收到光能后，以随机转移激子跃迁方式用了25ps时间将光能传递到反应中心，理论计算值为29.7ps。实验还得到了捕光天线LHCⅡ三聚体中Chal分子接收-400nm光能后，将能量为520fs的时间常数传递给相邻Chla分子，Chlb分子接收-400nm光能后，将能量以210fs的时间常数传递给相邻Chla分子，理论研究与实验结果基本符合。     

光学相关论题 生物光学

Q63 2005010795 高等植物外周捕光天线LHCⅡ中的超快光动力学过程= Ultrafast dynamics in peripheral light-harvesting complex LHCⅡ from high plant[刊,中]／郭立俊(河南大学物理与信息光电子学院．河南,开封(475001)),郭俊华…／／发光学报．-2004．25(3)．-242-246 利用飞秒抽运-探测技术及时间分辨荧光(TRPL)等光谱技术对高等植物LHCⅡ中的超快光动力学过程进行了研究。在其时间分辨荧光光谱中表现出了明显的各向异性特性。实验上观察了LHCⅡ中色素间的能量传递过     

PSII高效传能超快微观机理研究

在飞秒、皮秒时间分辨泵浦探测光谱学、荧光动力学、能量传递动力学研究基础上，确立了PSⅡ各功能单元激发能传递途径，由主外周天线LHCIIb吸收太阳能，通过次外周天线CP29，CP26，CP24，经内周天线CP43和CP47分别传递到反应中心D1－D2－Cytb559。利用四能带理论解析研究了PSII激发能传递机理和规律，利用四能级理论解析研究了天线复合物内部激发能传递过程。最后理论计算了PSII核心天线CP43及CP47中β－Car到Chla分子间激发能传递效率，分别为47．5％和66．5％。     

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.     

Fenna-Matthews-Olson捕光复合物中的冗余结构（英文）

研究了绿色硫细菌中捕光天线复合物Fenna-Matthews-Olson的一个子单元和反应中心的能量传递.通过细菌叶绿素分子的能量和耦合强度,构建了包含反应中心的哈密顿量及约化模型.通过级联运动方程研究了不同分子间和反应中心的激子布居演化.计算了Fenna-Matthews-Olson及其约化模型的二维三阶光子回波谱,获得能量传输过程中不同激子态间的相干性.结果表明在能量捕获过程中,Fenna-Matthews-Olson复合物存在冗余结构.     

Fenna-Matthews-Olson捕光复合物中的冗余结构

研究了绿色硫细菌中捕光天线复合物Fenna-Matthews-Olson的一个子单元和反应中心的能量传递.通过细菌叶绿素分子的能量和耦合强度,构建了包含反应中心的哈密顿量及约化模型.通过级联运动方程研究了不同分子间和反应中心的激子布居演化.计算了Fenna-Matthews-Olson及其约化模型的二维三阶光子回波谱,获得能量传榆过程中不同激子态间的相干性.结果表明在能量捕获过程中,Fenna-Matthews-Olson复合物存在冗余结构.     

The study of photo-induced ultrafast dynamics in light-harvesting complex LH2 of purple bacteria

In this paper, we introduce the photo-induced ultrafast dynamics taking place in the peripheral light harvesting antenna LH2 from purple bacteria Rhodobacter sphaeroides by using absorption, fluorescence emission and ultrafast spectroscopic techniques. Three kinds of LH2 samples, pH treated LH2 (complete removal of B800 pigments), carotenoid mutated LH2 (GM 309) and electrochemical oxidation treated LH2 were used in comparison with native LH2 to investigate the mechanism of photo-induced ultrafast energy transfer within the LH2 complex.     

Impacting materials by light and seeing their structural dynamics

The emergence of the field of photo-induced transformation triggered by intense and ultra-short light pulse in a material has opened a new route to acting on matter. It combines many of today’s issues such as far away from equilibrium phenomena, coherence and quantum control, complex correlations and non linear responsiveness, inter-conversion of energy and information. The advent of ultrafast structural dynamics motivated developing new tools to directly watch how matter works, by probing the time- and length-scales on which photo-induced processes take place. Different points will be briefly overviewed: (i) the development of laser pump and X-ray probe for watching ultrafast structural dynamics, (ii) the physical features resulting from this way of impacting materials by light, (iii) the presentation of some examples investigated by time-resolved X-ray diffraction and diffuse scattering experiments to illustrate the complex structural dynamics of a photo-induced transformation.     

Ultrafast blue light emission from SiC nanowires

Cubic silicon carbide (SiC) nanowires are synthesized in a catalyst-assisted process. The nanowires with diameter of ～ 40 nm exhibit strong blue light emission at room temperature under ultraviolet (UV) femtosecond laser excitation. The photon energy of peak emission is higher than the energy bandgap of cubic SiC which shows involvement of quantum confinement effect. The ultrafast fluorescence is deconvoluted by Monte-Carlo method. The results show two ultrafast decay processes whose lifetimes are about 26 and 567 ps respectively. The mechanisms of such ultrafast processes are discussed.     

Influence of the absorbed optical quanta energy on GHz ultrasound generation in GaAs

Experimental results of the investigation of the optoacoustic processes taetang place in GaAs semiconductor at ultrashort time scales are reported. Femtosecond laser has been used both for the generation (through the deformation potential mechanism by the interband absorption of laser radiation) and detection of GHz ultrasound waves. First experimental observation of an abrupt change in the phase of the photoexcited GHz ultrasound, when with increase of the energy of optical quanta direct generation of the electron-hole pairs in the side-valleys of GaAs becomes allowed by the energy and momentum conservation laws, is reported. We relate this observation, at least partially, to abrupt change in the ultrafast dynamics of photogenerated electron-hole plasma, in particular to deceleration of plasma diffusion when heavy carriers in the high energy side valley are photogenerated instead of light carriers in the lowest energy valley.     

苯乙炔分子电子激发态超快动力学研究

采用飞秒时间分辨质谱技术结合飞秒时间分辨光电子影像技术研究了苯乙炔分子电子激发态超快非绝热弛豫动力学.用235 nm光作为泵浦光,将苯乙炔分子激发到第二激发态S2,用400 nm光探测激发态的演化过程.时间分辨的母体离子的变化曲线用指数和高斯函数卷积得到不同的两个组分,一个是超快衰减组分,时间常数为116 fs,一个是慢速组分,时间常数为106 ps.通过分析时间分辨的光电子影像得到光电子动能分布,结合时间分辨光电子能谱数据发现,时间常数为116 fs的快速组分反映了S2态向S1态的内转换过程.实验还表明S1态通过内转换被布局后向T1态的系间窜跃过程为重要的衰减通道.本工作为苯乙炔分子S2态非绝热弛豫动力学提供了较清晰的物理图像.     

Ultrafast all-optical modulation by near-infrared intersubband transition in n-doped InGaAs/AlAsSb quantum wells

We demonstrate the ultrafast modulation of interband (IB)-resonant light (1.0–1.1 μm) by near-infrared intersubband (ISB)-resonant light (1.55–1.9 μm) in n-doped InGaAs/AlAsSb multiple quantum wells (QWs) using non-degenerate pump–probe spectroscopy. A modulation with an absorption recovery time of 1.0–2.0 ps has been observed in a planer-type modulation device due to ultrafast ISB relaxation of the carriers. The IB carrier relaxation process in the absence of an ISB-resonant light has also been investigated by time-resolved photoluminescence (PL) measurement. The modulation speed is determined by the inter- and intra-subband relaxation of the carriers in the conduction subband. The modulation speed at 1.1 μm due to an ISB-resonant pump light at 1.95 μm has been observed to be 1.4 ps at excitation energy of 500 fJ/μm².     

石墨烯超快动态光学性质

通过建立石墨烯的光学布洛赫方程, 研究了弱光场下的单层石墨烯超快动态光学性质. 理论研究表明在太赫兹辐射光场下由于泡利不相容和能量守恒原理使得石墨烯系统建立动态非平衡载流子并达到饱和的时间是20–200 fs, 能够在1 ps之内迅速产生光电流. 研究发现√2ev_F E₀ t<0 和ω 分别对应入射光的强度和频率, t为时间, v_F是石墨烯狄拉克点附近电子的费米速度. 研究发现光子能量?ω越大, 电极化强度以及光电流越强. 我们的理论研究结果与已有的众多实验结果一致, 表明石墨烯在超快动态光学领域尤其是太赫兹领域拥有重要的研究和应用价值.     

Ultrabroadband phase-matched optical parametric generation in the ultraviolet by use of guided waves

We present what is believed to be the first experimental demonstration of guided-wave phase-matched frequency mixing and harmonic conversion in gases. Broad-bandwidth ultrafast pulses, tunable around 270 nm, were generated from an ultrafast Ti:sapphire amplifier system using 2? + 2? - ? parametric wave mixing in a capillary waveguide. We achieved nonresonant phase matching by coupling both the fundamental and the second-harmonic light into the lowest-order mode. The output 3? pulses have an energy of >4muJ at a 1-kHz repetition rate. Simple extensions of this method can generate higher-energy 10-20-fs pulses tunable throughout the vacuum ultraviolet.     

Measurement of x-ray pulse widths by intensity interferometry

The pulse width of hard undulator radiation (32 ps width, energy 14 keV) was determined by intensity interferometry. The method, in combination with various x-ray monochromators, enables measurements to be taken over a wide range of time frames, from ns to fs. The applicable target includes measurements of ultrafast x-ray pulse widths from fourth generation synchrotron light sources.