Millimetre wave absorption by aqueous aerosol clusters

It is shown that laboratory measurements of the anomalous millimetre wave absorption of water vapour can be interpreted as due to aqueous aerosol (Aitken) clusters. A phenomenological theory is presented which accounts for the vapour pressure and temperature dependence of existing experimental results. The relevance of the aerosol theory to the widely reported anomalous absorption in the atmosphere is discussed.     

超光谱红外卫星资料同步反演不同地表类型的大气廓线、地表温度和地表发射率

大气温度、水汽、地表温度和地表发射率是大气和地表的本征信息量。利用卫星红外资料精确反演大气温湿廓线有利于准确预报天气和研究气候变化,同时地表温度和地表发射率光谱的反演为研究植物生长与作物产量、地表水分蒸发与循环、能量平衡、地表成分及物理性质、气候变迁与全球环境提供重要参数指标。把大气和地面作为一个整体系统来考虑,建立一种能同步反演大气温度廓线、大气水汽廓线、地表温度和地表发射率的反演方法,利用超光谱红外卫星资料(atmospheric infrared sounder, AIRS),针对我国新疆地区沙漠和雪地两种典型发射率地表同步反演大气温度廓线、水汽廓线、地表温度和地表发射率。反演方法首先线性化地球-大气系统红外辐射传输方程, 提出通过经验正交函数构建大气廓线和地表发射率光谱,有效减少反演变量数,建立同步物理反演模式,然后以美国国家环境预报中心(National Centers for Environmental Prediction,NCEP)的预报结果(初始大气温度、水汽廓线以及地表参数)作为初始值,最后通过牛顿迭代得到最优化解。反演观测区域覆盖我国新疆塔克拉玛干沙漠和准噶尔盆地,分别选择位于塔克拉玛干沙漠腹地的塔中探测站(纬度38.98°, 经度83.64°)和准噶尔盆地的阜康荒漠生态系统国家野外科学观测研究站(纬度44.2°, 经度87.9° )为反演地面验证点。反演结果表明,塔克拉玛干沙漠地表温度明显高于准噶尔盆地地表温度,与实际情况相一致;根据反演的8.6和13.4 μm处的地表发射率分布情况,可以看出在8.6 μm处沙漠地表发射率明显低于雪地发射率,在6～15 μm范围内,反演的沙漠地区(塔中站)地表发射率和雪地地区(阜康站)地表发射率与美国喷气推进实验室测量的沙漠发射率光谱和雪地发射率光谱相一致。研究表明,把大气和地面作为一个整体系统来考虑,把地表发射率加入到反演中,通过比较和分析沙漠地区(塔中)和雪地地区(阜康)的大气廓线反演结果与当地气象探空值和传统反演方法反演值,改进了大气温度廓线和水汽廓线反演精度,特别是边界层温度和水汽改进尤为明显;同时分析表明在发射率光谱变化较大的沙漠地区, 大气廓线反演精度的改进比雪地要高,这是由于地表发射率光谱在沙漠、戈壁地区变化较大,而雪地的发射率光谱变化不大。用该方法针对地表发射率光谱变化较大的地区(沙漠)同步反演大气廓线、地表温度和地表发射率,可以更有效的提高大气温度廓线、水汽廓线的反演精度。该研究结果可以为数值天气预报和我国未来超光谱红外卫星应用提供服务和有力支持, 具有十分重要的意义。     

Characterization of ?ngstr?m''s turbidity parameters in the Po Valley area for summer conditions of the atmosphere

Summary Measurements of direct solar irradiance were taken at the San Pietro Capofiume station in the centre of the Po Valley using two examples of the multispectral sun photometer, model UVISIR, on several clear-sky days of late spring and early summer in the years 1989 and 1990. Realistic evaluations of aerosol optical thickness at several sun-photometric wavelengths were obtained from these measurements by i) using values of the calibration constants carefully found by following both the Langley plot method and the spectral-correction procedure, which had previously been applied with satisfactory results to the sun-photometric measurements carried out in Antarctica and ii) taking into account the extinction effects produced by Rayleigh scattering and absorption due to ozone, water vapour and nitrogen dioxide on the solar radiation passing through the atmosphere. By examining a wide set of spectral series of the aerosol optical thickness in terms of the well-known Ångstr?m formula, a large number of pairs of atmospheric-turbidity parameters α and β was obtained, presenting a range of the mean daily values of α from 1.0 to 1.7 (with the median of 1.48) and a range of the mean daily values of β from 0.10 to 0.30 (with the median of 0.15). Using the particulate extinction models CR (for continental particles) and TR (for small tropospheric particles and large rural particles), the aerosol mass loading of the atmosphere calculated for these values of α and β was estimated to vary between 0.09 and 0.31 g m⁻² (with the median of 0.21 g m⁻²) during the measurement period of 1989 and between 0.09 and 0.41 g m⁻² (with the median of 0.13 g m⁻² for model CR and of 0.21 g m⁻² for model TR) during June and July 1990. Paper presented at the IX Congresso del Gruppo Nazionale per la Fisica dell'Atmosfera e dell'Oceano, June 8–10, 1992, Rome.     

Fluorescence spectroscopy of naphthalene at high temperatures and pressures: implications for fuel-concentration measurements

Fluorescence of the S ₁→S ₀ transition of naphthalene vapour after laser excitation at 266 nm was studied in a heated cell. Experiments were carried out for temperature in the range 350–900 K, at pressure between 0.1 and 3.0 MPa and for oxygen molar fraction from 0 to 21%. The absorption cross section of naphthalene showed a non-monotonic dependence upon temperature, which may be attributed to the spectral structures present in the absorption spectrum of naphthalene. Under nitrogen atmosphere, naphthalene fluorescence bi-exponentially decreased by an order of magnitude as temperature increased, whereas it increased by about 10% with pressure. Strong influence of quenching by O₂ on naphthalene fluorescence was observed and Stern–Volmer plots were found to be linear for temperatures between 450 and 750 K. The dependence of naphthalene fluorescence on oxygen concentration suggests one to use this molecule for fuel-concentration measurements in turbulent flows.     

Application of 940 nm high-power DFB lasers for line-broadening measurements at normal pressure using a robust and compact setup

High-power distributed-feedback (DFB) lasers for the wavelength range near 940 nm (i.e. about 10,600 cm⁻¹) were used for line-broadening measurements of individual rotational-vibrational absorption lines of water vapour at atmospheric pressure using a minimalist set-up. The laser has a maximum output power larger than 500 mW. Over the whole power range from threshold to maximum power, it operates in single mode operation with a tuning range of 4.7 nm, i.e. 50 cm⁻¹, at 20°C. With an emission line-width ≤2 MHz (0.66×10⁻⁴ cm⁻¹), the device is well suited for high-resolution spectroscopy.     

Atmospheric pressure chemical vapour synthesis of silicon–carbon nanoceramics from hexamethyldisilane in high temperature aerosol reactor

Silicon–carbon nanoceramics have been synthesised from hexamethyldisilane (HMDS) by the atmospheric pressure chemical vapour synthesis (APCVS). Direct aerosol phase synthesis enables continuous production of high purity materials in one-stage process. The particle formation is based on the decomposition of the precursor in a high temperature reactor. Reaction of the gas phase species leads to homogeneous nucleation and formation of the nanoparticles with a narrow size distribution (geometric mean diameter range of particle number size distribution 160–200 nm with 1.5–1.6 geometric standard deviation at reaction temperatures 800–1200 °C). A systematic investigation of the influence of the process temperature on the powder characteristics, including the particle size, crystallinity, chemical structure, surface and bulk composition and surface morphology, was carried out. At the reactor temperature of 800 °C, the synthesised nanoparticles were amorphous preceramics containing mostly SiC₄, Si–CH₂–Si and Si–H units. The composition of the powder turned towards nanocrystalline 3C–SiC (crystal size under 2 nm) when the reaction temperature was increased to 1200 °C. The reaction temperature appeared to be a key parameter controlling the structure and properties of the synthesised powders.     

Two-wavelength mid-IR diagnostic for temperature and n-dodecane concentration in an aerosol shock tube

A two-wavelength, mid-IR optical absorption diagnostic is developed for simultaneous temperature and n-dodecane vapor concentration measurements in an aerosol-laden shock tube. FTIR absorption spectra for the temperature range 323 to 773 K are used to select the two wavelengths (3409.0 and 3432.4 nm). Shock-heated mixtures of n-dodecane vapor in argon are then used to extend absorption cross section data at these wavelengths to 1322 K. The sensor is used to validate a model of the post-evaporation temperature and pressure of shock-heated fuel aerosol, which can ultimately be used for the study of the chemistry of low-vapor-pressure compounds and fuel blends. The signal-to-noise ratio of the temperature and concentration are ～20 and ～30, respectively, illustrating the sensitivity of this diagnostic. The good agreement between model and measurement provide confidence in the use of this aerosol shock tube to provide well-known thermodynamic conditions. At high temperatures, pseudo-first-order decomposition rates are extracted from time-resolved concentration measurements, and data from vapor and aerosol shocks are found to be in good agreement. Notably, the n-dodecane concentration measurements exhibit slower decomposition than predicted by models using two published reaction mechanisms, illustrating the need for further kinetic studies of this hydrocarbon. These results demonstrate the potential of multi-wavelength mid-IR laser sensors for hydrocarbon measurements in environments with time-varying temperature and concentration.     

The impact of Martian aerosols on the retrieval of temperature profiles from PFS measurements

Our purpose was a qualitative assessment of the impact of dust and water ice aerosols on the retrieved temperature profiles and the retrieval process itself in the Martian atmosphere. It aims to quantify the related uncertainties in the atmospheric temperature profiles derived from radiance measurements of the Planetary Fourier Spectrometer (PFS), currently operating on the Mars Express orbiter. In this study the effects of aerosol opacities on simulated data and retrieved temperature profiles were also investigated.From the analysis of the model atmosphere including dust and water ice with different size distributions it results that the dust component affects weighting functions and brightness temperatures less than water ice. A similar situation is also observed when different vertical distributions are considered. Unlike dust, water ice with different sizes of crystals evidently influences weighting functions and brightness temperatures. The impact of the considered water ice vertical distributions on brightness temperatures is noticeable only near 840 cm⁻¹.Considering different dust opacities, the largest differences—5 K maximum—between retrieved temperature profiles were observed close to the surface, regardless assumptions on a size distribution or the refractive indices. Contrary to dust, the different sizes of water ice particles assumed during retrieval stronger affected the retrieved temperature profiles than water ice opacities. Moreover, the differences in the retrieved temperature profiles were amplified while wrong optical properties for dust as well as for water ice aerosol were assumed instead of the nominal case. This means that the wrong assumption can induce an additional source of the retrieval error and lead to unreasonable temperature profiles. In the cases of expected heavily loads water ice crystals, their size distribution in the Martian atmosphere should be known from other observations before the retrieval of the temperature profile is attempted.For the analyzed examples of real PFS measurements the impact of different dust vertical distributions on the retrieval of temperature profile is prominent only in layers close to the surface. However, these differences remain comparable with retrieval errors. All influences of dust on weighting functions, brightness temperatures and during retrieval can be neglected if the noise equivalent radiance (NER) of PFS is taken into account.     

Satellite measurements of atmospheric ozone profiles,including tropospheric ozone,from ultraviolet/visible measurements in the nadir geometry: a potential method to retrieve tropospheric ozone

Numerical studies of a new method for the retrieval of ozone profile information from nadir-observing satellite measurements in the ultraviolet and visible are presented. The method combines information from back scattered radiation in the Hartley band down to the O₃ concentration peak, lower atmospheric information from the temperature structure of the Huggins bands, and a constraint on the total column from the Chappuis bands. The Huggins bands' temperature structure provides altitude information on the ozone distribution that includes clear distinction between stratospheric and tropospheric ozone. Studies presented here include dependence of the retrieved O₃ profiles on surface albedo, tropospheric aerosol, and tropospheric O₃ content for a range of atmospheric conditions.     

Sea surface temperature from AVHRR-2 data

Summary From the measurements in two channels of the 10 to 13 μm window region, the correction for the atmospheric absorption, useful to retrieve the sea surface temperature from satellite data, can be obtained. By using radiative-transfer model simulations, an up-to-date algorithm was developed, to retrieve the sea surface temperature from the AVHRR (advanced very high resolution radiometer) data. This algorithm has been compared with the algorithms found in the literature. A map of surface temperature in the Northern Adriatic Sea has been processed as an example of application of the algorithm developed. Visiting Scientist at the Joint Research Centre, Commission of the European Communities, 21020 ISPRA.