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Spectroscopic evidence for triplet excitation energy transfer among carotenoids in the LH2.complex from photosynthetic bacterium Rhodopseudomonas palustris

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Science China Chemistry 2004年第1期47卷 80-90页

作者： FENG Juan, WANG Qian, ZHANG Xujia, HUANG Youguo, Al Xicheng, ZHANG Xingkang & ZHANG JianpingState Key laboratory for Structural Chemistry of Unstable and Stable Species, institute of Chemistry, {2., beijing 100080, China national laboratory of Biomacromolecules, institute of Biophysics, {2., beijing 100101, China State Key laboratory for Structural Chemistry of Unstable and Stable Species institute of Chemistry Chinese Academy of Sciences Beijing China national laboratory of Biomacromolecules {2. of Biophysics Chinese Academy of Sciences Beijing China

The LH2.complex from Rhodopsudomonas (Rps.) palustris is unique in the heterogeneous carotenoid compositions. The dynamics of triplet excited state Carotenoids (3Car* has been investigated by means of sub-microsecond time-resolved absorption spectroscopy both at physiological temperature (2.5 K) and at cryogenic temperature (77K). Broad and asymmetric T n ←T 1 transient absorption was observed at room temperature following the photo-excitation of Car at 532.nm, which suggests the contribution from various carotenoid compositions having different numbers of conjugated C=C double bonds (Nc=c). The triplet absorption bands of different carotenoids, which superimposed at room temperature, could be clearly distinguished upon decreasing the temperature down to 77 K. At room temperature the shorter-wavelength side of the main Tn04T1 absorption band decayed rapidly to reach a spectral equilibration with a characteristic time constant of ∽1 μs, the same spectral dynamics, however, was not observed at 77 K. The aforementioned spectral dynamics can be explained in terms of the triplet-excitation transfer among heterogeneous carotenoid compositions. Global spectral analysis was applied to the time-resolved spectra at room temperature, which revealed two spectral components peaked at 545 and 565 nm, and assignable to the Tn04 T1 absorption of Cars with Nc=c=11 and Nc=c=13, respectively. Surprisingly, the decay time constant of a shorter-conjugated Car, i.e. 0.72.?s (aerobic) and 1.36 ?s (anaerobic), is smaller than that of a longer-conjugated Car, i.e. 2.12.us (aerobic) and 3.75 ?s (anaerobic), which is contradictory to the general rule of carotenoids and relative polyenes. The results are explained in terms of triplet-excitation transfer among different types of Cars. It is postulated that two Cars with different conjugation lengths coexist in an α, β-subunit in the LH2.complex.

关键词： purple photosynthetic bacteria, carotenoid, excited-state, time-resolved spectroscopy.

Novel gaseous transient species:generation and characterization

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Science China Chemistry 2007年第2期50卷 145-169页

作者： ZENG XiaoQing1,2.& WANG DianXun11 State Key laboratory for Structural Chemistry of Unstable and Stable Species,institute of Chemistry,{2. academy of Sci-ences,beijing 100080,China 2.Graduate School of chinese academy of sciences,beijing 100039,China State Key laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing China Graduate School of chinese academy of sciences Beijing China

Due to special properties of transient species, such as short-lived, unstable, reactive, and even explosive, the generation and subsequent characterization is a great challenge for experimental chemists. In our laboratory, systematic researches have been carried out to investigate novel transient species: reactive halogen species (RHS), short-lived free radicals, and metastable pseudohalogen compounds, based on the successive technical improvements on the Hel Photoelectron spectroscopy (PES). In this review, the topic mainly focuses on innovative methods of generating novel transient species, and subsequent geometric and electronic structure characterizations of these species combined with quantum chemical calculations.

关键词： reactive halogen species radicals pseudohalogen compounds Hel Photoelectron Spectroscopy (PES) quantum chemical calculations

Photogeneration of the free radicals and singlet oxygen by chrysophanol from rheum

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Science China Chemistry 2004年第5期47卷 381-387页

作者： RAO Jing1,2. XIE Jie1, ZHAO Jingquan1 & ZHU Teng2.1. Key laboratory of Photochemistry, Center for Molecular Science, institute of Chemistry, The {2., beijing 100080, China 2. University of Science and Technology beijing, beijing 10083, China Key laboratory of Photochemistry Center for Molecular Science Institute of Chemistry The Chinese Academy of Sciences Beijing China University of Science and Technology beijing Beijing China

In the current work, chryosphanol (MHAQ) was isolated and purified from rheum, and the photosensitization activities were studied. In nitrogen-saturated DMSO solution, irradia- tion of chryosphanol (MHAQ) with visible light (>430 nm) produced the semiquinone radical anions (MHAQ??), which was intensified significantly by an electron donor NADH, suggesting electron transfer between the excited and ground state photosensitizer molecules. In an air-saturated DMSO solution, superoxide radical anions (O2.), trapped by DMPO, were detected. ?? It was proved that O2.was not originated from the singlet oxygen (1O2. but dependent on DMPO, ?? chrysophanol, oxygen and the irradiation time. The singlet oxygen and OH could also be pro- ? duced by the photosensitization of the photosensitizer. These suggest that chrysophanol pos- sesses the photosensitization activity via Type I mechanism and Type II mechanism. To evaluate the photosensitization activities of MHAQ, emodin and mixed anthraquinone derivatives ex- tracted from rheum, the relative productivities of O2.were estimated to be 1.8, 1.1 and 1.0 re- ?? spectively and the quantum yields for singlet oxygen to be 0.36, 0.53 and 0.14 respectively. Therefore, these low-cost pigments may be potentially used as phototherapeutic medicine for some kind of vascular diseases or photo-activated pesticides.

关键词： chrysophanol, ESR, semiquinone radical anions, superoxide radical anions, hydroxyl radical, singlet oxygen.

Genesis of ^(2.0)Th excess in basalts from mid-ocean ridges and ocean islands:Constraints from the global U-series isotope database and major and rare earth element geochemistry

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Science China Earth sciences 2010年第10期53卷 1486-1494页

作者： ZHANG GuoLiang1,2.& ZENG ZhiGang1 1 Key laboratory of Marine Geology and Environment,institute of Oceanology,{2.,Qingdao 2.6071,China 2.Graduate University of {2.,beijing 100049,China Key laboratory of Marine Geology and Environment Institute of Oceanology Chinese Academy of Sciences Qingdao China Graduate University of chinese academy of sciences Beijing China

Based on 2.0Th-2.8U disequilibrium and major element data from mid-ocean ridge basalts(MORBs) and ocean island basalts(OIBs),this study calculates mantle melting parameters,and thereby investigates the origin of 2.0Th excess.(2.0Th/2.8U) in global MORBs shows a positive correlation with Fe8,Po,Na8,and Fmelt(Fe8 and Na8 are FeO and Na2. contents respectively after correction for crustal fractionation relative to MgO = 8 wt%,Po=pressure of initial melting and Fmelt=degree of melt),while 2.0Th excess in OIBs has no obvious correlation with either initial mantle melting depth or the average degree of mantle ***,compared with the MORBs,higher(2.0Th/2.8U) in OIBs actually corresponds to a lower melting *** suggests that the 2.0Th excess in MORBs is controlled by mantle melting conditions,while the 2.0Th excess in OIBs is more likely related to the deep garnet *** vast majority of calculated initial melting pressures of MORBs with excess 2.0Th are between 1.0 and 2.5 GPa,which is consistent with the conclusion from experiments in recent years that DU>DTh for Al-clinopyroxene at pressures of >1.0 *** initial melting pressure of OIBs is 2.2.3.5 GPa(around the spinel-garnet transition zone),with their low excess 2.6Ra compared to MORBs also suggesting a deeper mantle ***,excess 2.0Th in MORBs and OIBs may be formed respectively in the spinel and garnet stability *** addition,there is no obvious correlation of K2./TiO2.with(2.0Th/2.8U) and initial melting pressure(Po) of MORBs,so it is proposed that the melting depth producing excess 2.0Th does not tap the spinel-garnet transition *** and MORBs in both(2.0Th/2.8U) vs.K2./TiO2.and(2.0Th/2.8U) *** plots fall in two distinct areas,indicating that the mineral phases which dominate their excess 2.0Th are ***/Yb-Ce curves of fast and slow ridge MORBs are similar,while,in comparison,the Ce/Yb-Ce curve for OIBs shows more influence from *** mechanism

关键词： excess 2.0Th clinopyroxene garnet spinel-lherzolite mid-ocean ridge ocean island

Collision dynamics of He@C_(60)+He@C_(60) at low energies

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Science China(physics,Mechanics & Astronomy) 2008年第7期51卷 765-772页

作者： ZHAO Qiang1,2. ZHANG FengShou1,2.3 & ZHOU HongYu1,2.1 Key laboratory of Beam Technology and Material Modification of Ministry of Education, institute of Low Energy Nuclear {2., beijing Normal University, beijing 100875, China 2.beijing Radiation Center, beijing 100875, China 3 Center of Theoretical Nuclear {2., national laboratory of Heavy Ion Accelerator of Lanzhou, Lanzhou 730000, China Key laboratory of Beam Technology and Material Modification of Ministry of Education Institute of Low Energy Nuclear Physics Beijing Normal University Beijing China beijing Radiation Center Beijing China Center of Theoretical Nuclear physics National Laboratory of Heavy Ion Accelerator of Lanzhou Lanzhou China

A semi-empirical molecular dynamics model is developed. The central collisions of C60+C60 and He@C60+He@C60 at different incident energies are investigated based on this model. It is found that the dimer structures have been produced at proper incident energies and these fullerene dimers could be formed by a self-assembly of C60 fullerene and He@C60. The He atom has a significant effect at higher incident energy and this embedded He atom can enhance the stability of the dimer structure.

关键词： C60 He@C60 collision molecular dynamics

A brief account on the study of the insulin crystal structure In retrospect:Forty years after the determination of insulin’s crystal structure by chinese scientists

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Science China(Life sciences) 2010年第1期53卷 13-15页

作者： WANG Da-Cheng1 & GU XiaoCheng2.1 national laboratory of Macromolecules,{2. of Biophysics,chinese academy of sciences,beijing 100101,China 2.College of Life sciences,Peking University,beijing 100871,China national laboratory of Macromolecules Institute of Biophysics Chinese Academy of Sciences Beijing China College of Life sciences Peking University Beijing China

"Standards there as high as achieved elsewhere";news delivered to the world by Science in China Approximately forty years ago when China was undergoing a period of great difficulty, Science in China,

关键词： A brief account on the study of the insulin crystal structure In retrospect

Investigation of fine and complex vortex circulation structures

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Science China Earth sciences 2010年第10期53卷 1552-1558页

作者： LUO ZheXian1,MA GeLan1 & PING Fan2.1 Remote Sensing College,Nanjing University of Information Science and Technology,Nanjing 2.0044,China 2.laboratory of Cloud-Precipitation physics and Severe Storms(LACS),{2. of Atmospheric physics,chinese academy of sciences,beijing 10002.,China Remote Sensing College Nanjing University of Information Science and Technology Nanjing China laboratory of Cloud-Precipitation physics and Severe Storms (LACS) Institute of Atmospheric Physics Chinese Academy of Sciences Beijing China

The formation and evolution of fine and complicated vortex circulation structures were investigated using a two-dimensional quasi-geostrophic barotropic model *** find that the highly localized asymmetric and complex configuration of energy transfer flux between large-and small-scale components is caused by the nonlinear interaction between a large-scale vortex with an initial axi-symmetric flow and four beta meso-scale *** complex structure is characterized by a fine pattern,which contains seven closed systems with spatial scales of less than 100 km,embedded in a positive flux wave train and a negative wave train,*** average wind speed decreased with time in the positive flux region,but was nearly unchanged in the negative flux *** pattern reveals the evolutionary asymmetry and localization of wind speed of the major *** track of the major vortex center has a trend toward the center of the negative flux center,indicating that there is a certain relation between the complex structure of the energy transfer flux and the motion of the major vortex *** results imply that the formation and evolution of the fine and complex structure should be attributed to the nonlinear interaction between the vortices at different spatial scales.

关键词： vortex complex structure non-linear interaction energy cascade

Debating about the climate warming

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Progress in Natural Science:Materials International 2006年第1期16卷 1-6页

作者： WANG Shaowu1, LUO Yong2. ZHAO Zongci2. DONG Wenje2.and YANG Bao3 (1.Department of Atmospheric sciences, School of physics, Peking University, {2. 100871, China 2. laboratory for Climate Studies, China Meteorological Administration, {2. 100081, China 3. institute of Cold and Arid Regions Environmental and Engineering, chinese academy of sciences, Lanzhou 730000, China) Department of Atmospheric sciences School of Physics Peking University Beijing 100871 China laboratory for Climate Studies China Meteorological Administration Beijing 100081 China institute of Cold and Arid Regions Environmental and Engineering Chinese Academy of Sciences Lanzhou 730000 China

Debating about the climate warming is reviewed. Discussions have focused on the validity of the temperature reconstruction for the last millennium made by Mann et al. Arguments against and for the reconstruction are introduced. Temperature reconstructions by other authors are examined, including the one carried out by Wang et al. in 1996. It is concluded that: (1) Ability of reproducing temperature variability of time scale less than 10 a is limited, so no sufficient evidence proves that the 1990s was the warmest decade, and 1998 was the warmest year over the last millennium. (2. All of the temperature reconstructions by different authors demonstrate the occurrence of the MWP (Medieval Warm Period) and LIA (Little Ice Age) in low frequency band of temperature variations, though the peak in the MWP and trough in LIA varies from one reconstruction to the others. Therefore, terms of MWP and LIA can be used in studies of climate change. (3) The warming from 1975 to 2.00 was significant, but we do not know if it was the strongest for the last millennium, which needs to be proved by more evidence.

关键词： climate warming MWP LIA the 2.th century.

Threading dislocation density comparison between GaN grown on the patterned and conventional sapphire substrate by high resolution X-ray diffraction

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Science China(physics,Mechanics & Astronomy) 2010年第3期53卷 465-468页

作者： ZHANG YuChao1, XING ZhiGang2. MA ZiGuang2. CHEN Yao2. DING GuoJian2. XU PeiQiang2. DONG ChenMing3, CHEN Hong2.& LE XiaoYun1 1 School of physics and Nuclear Energy Engineering, Beihang University, beijing 100190, China 2.Renewable Energy {2., institute of physics, chinese academy of sciences, beijing 100190, China 3 School of Information and Communication, Tianjin Polytechnic University, Tianjin 300160, China School of physics and Nuclear Energy Engineering Beihang University Beijing China Renewable Energy laboratory Institute of Physics Chinese Academy of Sciences Beijing China School of Information and Communication Tianjin Polytechnic University Tianjin China

GaN epifilms are grown on the patterned sapphire substrates (PSS) (0001) and the conventional sapphire substrates (CSS) (0001) by metal-organic chemical vapor deposition (MOCVD) using a novel two-step growth. High resolution X-ray diffraction (HR-XRD) is used to investigate the threading dislocation (TD) density of the GaN epifilms. The TD density is calculated from the ω-scans full width at half maximum (FWHM) results of HR-XRD. The edge dislocation destiny of GaN grown on the PSS is 2.7×108 cm-2. which is less than on the CSS. This is confirmed by the results of atomic force microscopy (AFM) measurement. The lower TD destiny indicates that the crystalline quality of the GaN epifilms grown on the PSS is improved compared to GaN epifilms grown on the CSS. The residual strains of GaN grown on the PSS and CSS are compared by Raman Scattering spectra. It is clearly seen that the residual strain in the GaN grown on PSS is lower than on the CSS.

关键词： GaN patterned sapphire substrate threading dislocation XRD