Characteristics of cirrus clouds and its radiative properties based on lidar observation over Chung-Li, Taiwan

In this paper, characterization of cirrus clouds are made by using data from ground based polarization lidar and radiosonde measurements over Chung-Li (24.58°N, 121.10°E), Taiwan for a period of 1999–2006. During this period, the occurrence of cirrus clouds is about 37% of the total measurement nights over the lidar site. Analysis of the measurement gives the statistical characteristics about the macrophysical properties such as occurrence height, ambient temperature, and its geometrical thickness while the microphysical properties are interpreted in terms of extinction coefficient, optical depth, effective lidar ratio and depolarization ratio. The effective lidar ratio has been retrieved by using the simulation technique of backscattered lidar signals. The effect of multiple scattering has been taken into the account by a model calculation. Summer (Jun–Aug) shows the maximum appearances of cirrus due to its formation mechanism. It is shown that tropopause cirrus clouds may occur with a probability of about 24%. These clouds are usually optically thin and having laminar in structure with some cases resembling the characteristics similar to that of polar stratospheric clouds (PSCs). The radiative properties of the cirrus clouds are also discussed in detail by the empirical equations with results show a positive feedback on any climate change.     

基于静止卫星红外云图的MCS普查研究进展及标准修订

基于静止卫星红外云图的MCS普查标准不统一不利于各种MCS普查结果的对比分析, 该文在总结MCS普查研究进展的基础上, 依据Orlanski尺度分类标准对MβCS普查的最小尺度标准作了修订, 即修订为TBB≤-32 ℃的连续冷云区直径≥20 km。根据马禹等的MβCS普查标准和该文修订的MβCS普查标准, 利用GOES-9卫星红外云图普查了2003年6月19日—7月22日淮河大水期间的MCS, 结果发现共有10个MαCS和24个MβCS, 并对24个MβCS作了普查标准修订前后的统计结果对比, 发现新的普查标准比根据马禹等的MβCS普查标准获得的结果多7个MβCS, 并且这7个MβCS中有6个都引起强降水, 因此这种对比分析结果表明:新MβCS普查标准对揭示淮河大水和MCS的关系更具合理性。此外, 还分析了3个因MβCS而引起局地强降水的典型个例, 这些MβCS的直径尺度只有几十至一百多公里, 不符合马禹等的MβCS普查标准。对这3个MβCS分析结果表明:该文新MβCS普查标准有助于对产生剧烈天气的MCS的普查研究和预报。     

Breakdown of hydrous ringwoodite to pyroxene and spinelloid at high P and T and oxidizing conditions

To get deeper insight into the phase relations in the end-member system Fe₂SiO₄ and in the system (Fe, Mg)₂SiO₄ experiments were performed in a multi-anvil apparatus at 7 and 13 GPa and 1,000–1,200°C as a function of oxygen fugacity. The oxygen fugacity was varied using the solid oxygen buffer systems Fe/FeO, quartz–fayalite–magnetite, MtW and Ni/NiO. The run products were characterized by electron microprobe, Raman- and FTIR-spectroscopy, X-ray powder diffraction and transmission electron microscopy. At fO₂ corresponding to Ni/NiO Fe-ringwoodite transforms to ferrosilite and spinelloid according to the reaction: 9 Fe₂SiO₄ + O₂ = 6 FeSiO₃ + 5 Fe_2.40Si_0.60O₄. Refinement of site occupancies in combination with stoichiometric Fe³⁺ calculations show that 32% of the total Fe is incorporated as Fe³⁺ according to From the Rietveld refinement we identified spl as spinelloid III (isostructural with wadsleyite) and/or spinelloid V. As we used water in excess in the experiments the run products were also analyzed for structural water incorporation. Adding Mg to the system increases the stability field of ringwoodite to higher oxygen fugacity and the spinel structure seems to accept higher Fe³⁺ but also water concentrations that may be linked. At oxygen fugacity corresponding to MtW conditions similar phase relations in respect to the breakdown reaction in the Fe-end-member system were observed but with a strong fractionation of Fe into spl and Mg into coexisting cpx. Thus, through this strong fractionation it is possible to stabilize very Fe-rich wadsleyite with considerable Fe³⁺ concentrations even at an intermediate Fe–Mg bulk composition: assuming constant K _D independent on composition and a bulk composition of x _Fe = 0.44 this fractionation would stabilize spl with x _Fe = 0.72. Thus, spl could be a potential Fe³⁺ bearing phase at P–T conditions of the transition zone but because of the oxidizing conditions and the Fe-rich bulk composition needed one would expect it more in subduction zone environments than in the transition zone in senso stricto.

Carbon dioxide segregation in 1:4 and 1:9 CO2:H2O ices

The mid-infrared spectra of mixed vapor deposited ices of CO₂ and H₂O were studied as a function of both deposition temperature and warming from 15 to 100 K. The spectra of ices deposited at 15 K show marked changes on warming beginning at 60 K. These changes are consistent with CO₂ segregating within the ice matrix into pure CO₂ domains. Ices deposited at 60 and 70 K show a greater degree of segregation, as high as 90% for 1:4 CO₂:H₂O ice mixtures deposited at 70 K. As the ice is warmed above 80 K, preferential sublimation of the segregated CO₂ is observed. The kinetics of the segregation process is also examined. The segregation of the CO₂ as the ice is warmed corresponds to temperatures at which the structure of the water ice matrix changes from the high density amorphous phase to the low density amorphous phase. We show how these microstructural changes in the ice have a profound effect on the photochemistry induced by ultraviolet irradiation. These experimental results provide a framework in which observations of CO₂ on the icy bodies of the outer Solar System can be considered.     

The coating hypothesis for ammonia ice particles in Jupiter: Laboratory experiments and optical modeling

We report laboratory experiments and modeling calculations investigating the effect of a hydrocarbon coating on ammonia ice spectral signatures. Observational evidence and thermochemical models indicate an abundance of ammonia ice clouds in Jupiter's atmosphere. However, spectrally identifiable ammonia ice clouds are found covering less than 1% of Jupiter's atmosphere, notably in areas of strong vertical transport, indicating a short lifetime for the signature of ammonia absorption on condensed ammonia particles [Baines, K.H., Carlson, R.W., Kamp, L.W., 2002. Icarus 159, 74-94]. Current literature has suggested coating of ammonia ice particles by a hydrocarbon haze as a possible explanation for this paradox. The work presented here supports the inference of a coating effect that can alter or suppress ammonia absorption features. In the experiments, thin films of ammonia ices are deposited in a cryogenic apparatus, coated with hydrocarbons, and characterized by reflection-absorption infrared spectroscopy. We have observed the effects on the ammonia ice absorption features near 3 and 9 μm with coverage by thin layers of hydrocarbons. Modeling calculations of these multilayer thin films assist in the interpretation of the experimental results and reveal the important role of optical interference in altering the aforementioned ammonia spectral features. Mie and T-matrix scattering calculations demonstrate analogous effects for ammonia ice particles and investigate the relative effects of ammonia ice particle size, shape, and coating layer thickness on the ice particle spectral signatures.     

Optical constants of amorphous and crystalline H2O-ice in the near infrared from 1.1 to 2.6 μm

Using new laboratory spectra, we have calculated the real and imaginary parts of the index of refraction of amorphous and crystalline H₂O-ice from 20 to 150 K in the frequency range 9000-3800 cm⁻¹ (1.1-2.6 μm) at a spectral resolution of 1 cm⁻¹. These optical constants can be used to create model spectra for comparison to spectra from Solar System objects. We also analyzed the differences between the amorphous and crystalline H₂O-ice spectra, including weakening of bands and shifting of bands to shorter wavelength in amorphous H₂O-ice spectra. We have also observed two spectrally distinct phases of amorphous H₂O-ice.     

Trapping and adsorption of CO2 in amorphous ice: A FTIR study

The interaction of carbon dioxide and amorphous water ice at 95 K is studied using transmission infrared spectroscopy. Samples are prepared in two ways: co-deposition of the gases admitted simultaneously or sequential deposition, in which amorphous water ice (ASW) is grown first and CO₂ vapor is added subsequently. In either case, a fraction of the CO₂ molecules is found to interact with water in a way that gives rise to shifts and splittings in the infrared bands with respect to those of a pure CO₂ solid. In co-deposition experiments, a larger amount of carbon dioxide is trapped within the amorphous water than in sequential deposition samples, where a substantial proportion of molecules appears to be trapped in macropores of the ASW. The specific surface area of sequential samples is evaluated and compared to previous literature results. When the sequential samples are heated to 140 K, beyond the onset temperature at which water ice undergoes a phase transition, the CO₂ molecules at the pores relocate inside the bulk in a structure similar to that found in co-deposited samples, as deduced by changes in the shape of the CO₂ infrared bands.     

Dehydration experiments on natural omphacites: qualitative and quantitative characterization by various spectroscopic methods

A series of natural omphacites from a wide range of P, T occurrences were investigated by electron microprobe (EMP), infrared (IR)-, Mössbauer (MS)- and optical spectroscopy in the UV/VIS spectral range (UV/VIS), secondary ion mass spectrometry (SIMS) and single crystal structure refinement by X-ray diffraction (XRD) to study the influence of hydrogen loss on valence state and site occupancies of iron. In accordance with literature data we found Fe²⁺ at M1 as well as at M2, and in a first approach assigned Fe³⁺ to M1, as indicated by MS and XRD results. Hydrogen content of three of our omphacite samples were measured by SIMS. In combination with IR spectroscopy we determined an absorption coefficient: ε _i,tot = 65,000 ± 3,000 lmol_H2O ^?1 cm^?2. Using this new ε _i,tot value, we obtained water concentrations ranging from 60 to 700 ppm H₂O (by weight). Hydrogen loss was simulated by stepwise heating the most water rich samples in air up to 800°C. After heat treatment the samples were analyzed again by IR, MS, UV/VIS, and XRD. Depending on the type of the OH defect, the grade of dehydration with increasing temperature is significantly different. In samples relatively poor in Fe³⁺ (<0.1 Fe³⁺ pfu), hydrogen associated with vacancies at M2 (OH bands around 3,450 cm^?1) starts to leave the structure at about 550°C and is completely gone at 780°C. Hydrogen associated with Al³⁺ at the tetrahedral site (OH bands around 3,525 cm^?1, Koch-Müller et al., Am Mineral, 89:921–931, 2004) remains completely unaffected by heat treatment up to 700°C. But all hydrogen vanished at about 775°C. However, this is different for a more Fe³⁺-rich sample (0.2 Fe³⁺ pfu). Its IR spectrum is characterized by a very intense OH band at 3,515 cm^?1 plus shoulder at 3,450 cm^?1. We assign this intense high-energy band to vibrations of an OH dipole associated with Fe³⁺ at M1 and a vacancy either at M1 or M2. OH release during heating is positively correlated with decrease in Fe²⁺ and combined with increase in Fe³⁺. That dehydration is correlated with oxidation of Fe²⁺ is indirectly confirmed by annealing of one sample in a gas mixing furnace at 700°C under reducing conditions keeping almost constant OH^? content and giving no indication of Fe²⁺-oxidation. Obtained data indicate that in samples with a relatively high concentration of Fe²⁺ at M2 and low-water concentrations, i.e., at a ratio of Fe^{2+ M2}/H > 10 dehydration occurs by iron oxidation of Fe²⁺ exclusively at the M2 site following the reaction: \( {\left[ {{\text{Fe}}^{{{\text{2 + [ M2]}}}}{\text{OH}}^{ - } } \right]} = {\left[ {{\text{Fe}}^{{{\text{3 + [ M2]}}}} {\text{O}}^{{{\text{2}} - }} } \right]} + {\text{1/2}}\;{\text{H}}_{{\text{2}}} \uparrow . \) In samples having relatively low concentration of Fe²⁺ at M2 but high-water concentrations, i.e., ratio of Fe^{2+ M2}/H < 5.0 dehydration occurs through oxidation of Fe²⁺ at M1.     

垂直气柱中大气微量成分总含量的反演

提出了一种利用地面中等光谱分辨率的太阳红外光谱反演整层大气中某几种微量成分总含量的方法,用逐线积分（ Ｌ Ｂ Ｌ） 法计算整层大气分子吸收,采用差分吸收法测量太阳红外光谱得到实际大气中微量成分的吸收,用最大似然法反演出微量成分的总量。详细分析了这种方法的可行性和反演精度,数值模拟分析和实际测量表明该方法有较高的精度,已把该方法用于监测实际大气中甲烷和水汽总含量的变化。     

Spectroscopic Characterization of Organic Structures and Organic‐Inorganic Interactions in Paper Mill Sludge

The organic composition and organic‐inorganic interaction in paper mill sludge (PS) solvent extracts (hexane, ethyl acetate, acetone and ethanol) and humic fractions, humic acid (HA) and humin (HU) were studied by electron paramagnetic resonance spectroscopy (EPR), proton and carbon‐13 nuclear magnetic resonance spectroscopy (¹H NMR; ¹³C NMR), Fourier‐transformed infrared spectroscopy (FTIR), and ultraviolet‐visible spectroscopy (UV‐vis). The strategy of fractionating the PS, sequentially, with organic solvents of increasing polarity is a reliable analytical procedure for humic substance sample separation because it results in more purified fractions. FTIR, ¹H NMR and ¹³C NMR results showed that hexane extract consisted mainly of aliphatic hydrocarbon structures. Their contents in the extracts decreased as the polarity of the extracting solvent increased and the content of oxygen functional groups increased. Carboxylic and carboxylate functional groups were found in the acetone extract, and ester and ether functions were predominantly found in the ethanol extract. EPR spectra revealed some Fe³⁺ complexes with rhombic structure (g₁ = 4.3; g₂ = 9.0) in the humic fractions and in all solvent extracts, except hexane. Quasi‐octahedral Fe³⁺ complexes (g = 2.3; ΔH_pp ≤ 400 G) were found in the HU fraction and in the acetone extract. The organic free radical content in the HA fraction was higher than the non‐fractionated PS sample and HU fraction.