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81.
前寒武纪各种地质记录表明了太古代—元古代早期古全球环境具有显著的陆少洋多和大气富CO2、贫O2的特征。BIFs大气-海洋系统中Fe2+的氧化是导致铁质发生沉淀的一个重要过程,在前寒武纪早期缺O2的环境,生物-无氧氧化和日光-紫外线为主的宇宙射线光致氧化作用产生的直接非生物-无氧氧化过程,在前寒武纪早期缺O2环境对Fe2+的氧化可能起着重要的和主导的作用。BIFs条带状矿石的宏、微观SiO2或Fe2O3/Fe3O4单层厚度非等厚性表征了硅、铁供给非等量性与交替淀积非等时性的韵律堆积。文章提出了一种与地球自转速率有关的日长年际变化(古ELNino事件)-硅铁临界饱和浓度模式,从统一的地球动力学条件和不同类型BIFs的成因联系解析了这种韵律堆积的机制。元古代早—中期大气-海洋系统发生了O2增多和CO2减少的古全球变化,导致了2.2~1.8Ga之间大气圈平流层古臭氧层的形成。古臭氧层大幅度消减日光-紫外线对地球表面的强烈辐射,不仅使全球性由日光-紫外线光致氧化作用直接产生的Fe2+非生物-缺氧氧化过程消失,而且也保证了生命演化的延续和生物进入多样性繁衍。与其伴随的全球性巨厚碳酸盐建造,导致了上壳岩下伏的地球早期富铁?  相似文献   
82.
A high-sensitive technique to detect O(1S) atoms using vacuum ultraviolet laser-induced fluorescence (VUV-LIF) spectroscopy has been applied to study the O(1S) production process from the UV photodissociation of O3, N2O, and H2O2. The quantum yields for O(1S) formation from O3 photolysis at 215 and 220 nm are determined to be (1.4 ± 0.4) × 10−4 and (5 ± 3) × 10−5, respectively. Based on thermochemical considerations, the O(1S) formation from O3 photolysis at 215 and 220 nm is attributed to a spin-forbidden process of O(1S)+O2(X3Σg ). Analysis of the Doppler profile of O(1S) produced from O3 photolysis at 193 nm also indicates that the O(1S) atoms are produced from the spin-forbidden process. In the photolysis of N2O and H2O2 at 193 nm, no discernible signal of O(1S) atoms has been detected. The upper limit values of the quantum yields for O(1S) production from N2O and H2O2 photolysis at 193 nm are estimated to be 8 × 10−5 and 3 × 10−5, respectively. Using the experimental results, the impact of the O(1S) formation from O3 photolysis on the atmospheric OH radical formation through the reaction of O(1S)+H2O has been estimated. The calculated results show that the contribution of the O(1S)+H2O reaction to the OH production rate is ∼2% of that of the O(1D)+H2O reaction at 30 km altitude in mid-latitude. Implications of the present laboratory experimental results for the terrestrial airglow of O(1S) at 557.7 nm have also been discussed.  相似文献   
83.
The theoretical anharmonicity of the inner-OH stretching modes of kaolinite and lizardite is determined using a frozen-phonon approach. The anharmonicity parameter, defined as the difference between half the first overtone frequency and the frequency of the fundamental transition, is −95 and −92 cm−1 for kaolinite and lizardite, respectively. These values are consistent with the experimental measurements. The very good agreement usually observed between harmonic calculations of vibrational frequencies at the density functional theory (DFT) level, using the generalized gradient approximation (GGA), and experimental positions of vibrational bands results from the fortuitous, but almost exact, cancelation of two types of errors. One is related to the GGA approximation and the other to the neglect of anharmonicity.  相似文献   
84.
辉石中结构羟基变温行为的红外光谱初步研究   总被引:2,自引:1,他引:2  
运用显微傅立叶变换红外光谱(Micro-FTIR)技术观察了辉石(单斜辉石和斜方辉石)中结构OH在原位连续加热、降温和阶段加热过程中的行为,从而更清楚地了解了缺陷氢在晶体结构中的位置及其结合机制。样品为安徽女山新生代玄武岩中的普通辉石巨晶和橄榄岩包体中的斜方辉石。温度从室温升到500℃,间隔100℃。实验结果表明,单斜辉石和斜方辉石的红外谱图随温度变化的趋势相同,即:OH的伸缩振动峰位都是随温度升高而向低波数移动,而且这种变化是可逆的;峰位的移动主要受H所取代的阳离子的位置或晶格空隙的热膨胀的影响。  相似文献   
85.
We report here a single-crystal polarized-light study of stoppaniite, ideally (Fe,Al,Mg)4(Be6Si12O36)(H2O)2(Na,□), from Capranica (Viterbo). Polarized-light FTIR spectra were collected on an oriented (hk0) section, doubly polished to 15 μm. The spectrum shows two main bands at 3,660 and 3,595 cm−1; the former is strongly polarized for E c, while the latter is polarized for E //c. A sharp and very intense band at 1,620 cm−1, plus minor features at 4,000 and 3,228 cm−1 are also polarized for E //c. On the basis of literature data and considering the pleochroic behavior of the absorptions, the 3,660 cm−1 band is assigned to the ν3 stretching mode and the 1,620 cm−1 (associated with an overtone 2*ν2 at 3,230 cm−1) band to the ν2 bending mode of “type II” water molecules within the structural channels of the studied beryl. The sharp band at 3,595 cm−1 is not associated with a corresponding ν2 bending mode; thus it is assigned to the stretching vibration of O–H groups in the sample. The minor 4,000 cm−1 feature can be assigned to the combination of the O–H bond parallel to c with a low-frequency metal-oxygen mode such as the Na–O stretching mode. The present results suggest that the interpretation of the FTIR spectrum of Na-rich beryl needs to be carefully reconsidered.  相似文献   
86.
The IR spectrum of an alpine, hydrothermally formed diopside containing 17 wt ppm H2O consists of three main OH absorption bands centred at 3647, 3464 and 3359 cm−1. Jadeite from a Californian vein occurrence is characterised by bands at 3616 and 3557 cm−1 and contains about 197 wt ppm H2O. Based on the pleochroic scheme of the OH absorption bands in diopside, OH defect incorporation models are derived on the basis of fully occupied cation sites and under the assumption of M1 and M2 site vacancies; OH defects replacing O2 oxygen atoms are most common. The less pronounced OH pleochroism and the broad band absorption pattern of jadeite indicate a high degree of OH defect disordering. The pleochroic scheme of the main absorption bands at 3616 and 3557 cm−1 implies partial replacement of O2 oxygen atoms by OH dipoles pointing to vacant Si sites. Under the assumption of M1 and M2 site vacancies, O1–H and O2–H defects are also derivable. OH incorporation modes assuming Si-vacancies should be considered for jadeite-rich clinopyroxenes formed in deep crust and upper mantle regions.  相似文献   
87.
本文探讨了OH Meinel夜气辉辐射的光化学模式,给出OH(ν≤9)分子数密度分布的计算通式,重点研究了化学反应HO\-2+O→OH(ν≤6)+O2对ν≤6各振动能级上OH分子数密度分布以及(ν′—ν″)(ν′≤6)振动带气辉辐射的影响.结果表明,该反应对数密度的贡献随振动能级的减小而增大,对(ν′—ν″)振动带辐射的贡献随着较高振动能级ν′的减小而增大,以春分时为例,它可使第1振动能级上的OH分子最大数密度和(1—0)带的最大辐射率增加约33%,第6振动能级上的最大数密度和(6—ν″)带的最大辐射率增加约7%,(1—0)带的辐射强度增加约30%,(6—ν″)带的强度增加约11%.该反应使各振动能级上分子数密度的高度分布剖面以及各振动带体辐射率的高度分布剖面变宽,最大数密度、最大发射率所处的高度下降1 km左右.此外,该反应的影响程度随着原子氧密度的降低而增大,随着温度的升高而增大,并且在夏至时最大,在冬至时最小.  相似文献   
88.
During the EASE/OXICOA campaign of the NERC ACSOE programme, trichloroethylene and a wide range of man-made halocarbons and radiatively-active trace gases were monitored with high precision and high frequency throughout July 1996 at Mace Head on the Atlantic Ocean coast of Ireland. Trichloroethylene concentrations in concert with many other trace gases became elevated as regionally-polluted and photochemically-aged air masses reached Mace Head. However, as the anticyclonic air masses retreated during 19 and 20 July, trace gas concentrations remained elevated for a significant period. During this 2–4 day period, trichloroethylene concentrations decayed significantly, though the concentrations of the other more chemically-inert trace gases did not. A detailed interpretation of this behaviour using a Lagrangian dispersion model has allowed the estimation of average and peak OH radical concentrations of 3 and 9×106 molecule cm-3, respectively, during the travel from the source areas in the U.K. and the low countries out to Mace Head. Using a simple box model, the available Mace Head measurements, when combined into a detailed chemical mechanism, generated OH radical concentrations which peaked at 7×106 molecule cm-3, in close agreement with the estimates based on trichloroethylene decay.  相似文献   
89.
A two-dimensional global chemistry model is developed to study the distribution and long-term trends of methane. The model contains 34 species and 104 chemical and photochemical reactions. Using the model, the long-term trends of CH4, CO and OH in atmosphere are simulated, comparison between the model and observations shows that the simulation is successful. Experiments are done to investigate the causes of dramatic decrease in the growth rate of CH4 in 1992 such as OH increase due to stratospheric ozone depletion, decrease of temperature in the troposphere due to Mount Pinatubo eruption and descendent of CH4 sources fluxes. A new explanation is proposed and verified by this model that the decrease of CO emission plays an important role for the abnormal growth rate of CH4 in 1992. We find that the decreases of CH4 and CO emissions are the main reasons for the sudden decrease of growth rate of CH4 in 1992, which account for 73% and 27% respectively.  相似文献   
90.
渐近巨星分支恒星 (AGB星 )是一种晚期演化恒星 ,它是恒星作为以核反应释能为发光能源的天体的最后演化阶段。AGB星阶段的恒星具有许多有趣的性质 ,如很大的质量损失率 (因此形成很厚的拱星尘埃气体包层 ) ,光变 ,热脉动 (或He闪耀 ) ,强的红外超量发射 ,分子脉泽发射等 ,弄清AGB星的演化规律是研究恒星演化理论的重要任务。目前人们所知道的AGB星的演化图景是 ,恒星经过漫长的主序演化之后 ,将经过红巨星 (RGB)阶段 ,然后才进入AGB阶段 ,在其演化过程中AGB星的光度和质量损失率要逐渐增大 ,它的光变周期也逐渐变长 ,在其中心星经历了一系列的由He核反应不稳定性引起的热脉动之后 ,它的质量损失很快停止 ,恒星开始向行星状星云 (PN)演化 ,最后行星状星云将会变成一个白矮星 ,这将是许多初始质量不很大的恒星的最终结局。OH/IR星阶段是AGB星演化的一个阶段 ,OH/IR星是那些质量稍大的恒星在AGB阶段后期演化而成的天体。现阶段人们对OH/IR星的具体演化过程还知道得很少。我们利用了球对称包层中的尘埃辐射转移模型来研究OH/IR星的演化性质 ,并且收集了尽量多的具有可靠距离的OH/IR星来研究他们的光度和质量损失率的演化性质。在本文的研究工作中 ,我们主要讨论了OH/IR星在远红外双色图中的分布规律 ,还发现  相似文献   
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