Parameterization of ammonia and water content of atmospheric droplets with fixed number of sulfuric acid molecules

We present a parameterization for numbers of water and ammonia molecules in an equilibrium droplet with fixed number of sulfuric acid molecules at known relative humidity, ammonia mixing ratio and temperature. The radius of the droplet is also parameterized. The parameterizations are based on macroscopic model of solution droplets and up-to-date thermodynamics. The binary parameterizations are valid for temperatures 190–330 K and relative humidities 1–99%. The ternary parameterization can be used at temperatures 240–300 K, relative humidities 5–95%, and ammonia mixing ratios 10^− 4–100 ppt. In both cases the parameterizations are valid for droplets containing up to 10¹¹ sulfuric acid molecules. The droplet composition is always between the limits of pure ammonium bisulfate and pure ammonium sulfate.     

On the reactive uptake of gaseous PAH molecules by micron-sized atmospheric water droplets

A falling droplet reactor was used to study the heterogeneous oxidation of gaseous PAH molecules adsorbed on a 92 μm diameter water droplet by ozone. The dynamic partition constant for the PAH between the droplet and air and the first-order surface rate constant was measured. The increase in uptake with ozone concentration was due to increased mass transfer via surface reaction of co-adsorbed ozone and PAH. The surface rate constant was rationalized through the Langmuir–Hinshelwood mechanism. The rate constant was smaller for phenanthrene than naphthalene. The main reaction products identified in the aqueous phase indicated the peroxidic route for surface reaction of ozone with PAH. The heterogeneous reaction rate of ozone with adsorbed phenanthrene at the air–water interface of a 92-μm droplet was estimated to be 9300 times larger than the homogeneous reaction of ozone with phenanthrene in the gas phase and it was 76 times larger than the homogeneous oxidation by hydroxyl radical in the gas phase. For naphthalene that is more volatile, however, the homogeneous reaction with hydroxyl was more important. Increased organic carbon added to the droplet increased both the partition constant for phenanthrene and surface reaction with ozone. The partition constant for a droplet formed from actual fog water was much larger than for pure distilled water.     

微波遥感海上大气可降水和云液态含水量

根据历史探空资料,对西太平洋海域中有代表性的热带和亚热带地区的云天大气做了l.35cm和8.5mm波段的辐射传输计算,揭示了海上云天辐射传输的某此特征。在此基础上,对原有的一种反演云天大气可降水(Q)及云的垂直积分液态含水量(L)的方法做了相应的改进。 1985年12月至1986年1月用船载双波长微波辐射计取得的西太平洋热带海域中的实际观测结果。着重给出了该海域中Q及L的日变化,对流云Q和L场的水平结构及弱冷锋过境时Q及L的演变等方面的个例。 此外,模式计算及海上观测都表明,8.5mm波长辐射计也可以单独探测海上晴空大气可降水。在此基础上,提出了有可能用两波长辐射计的独立测值进行相互比较来判断视野中是否有云。     

Relevance of ion-induced nucleation of sulfuric acid and water in the lower troposphere over the boreal forest at northern latitudes

The relevance of ion-induced nucleation of sulfuric acid and water (IINSW) in the troposphere over the boreal forest at northern latitudes is investigated by combining two existing and previously published models (MALTE — model to predict new aerosol formation in the lower troposphere; PARNUC — a parameterized steady-state model of neutral and ion-induced nucleation of sulfuric acid and water for atmospheric conditions). Simulations were performed for 4 days with observed new particle formation at ground level by using input data from the SMEAR II station in Hyytiälä, Finland. The selected days were chosen to cover a wide range of values of the parameters most relevant for IINSW. The results showed that ion-induced nucleation of sulfuric acid and water can contribute up to 15% to the total amount of newly formed particles in the size range of 3–10 nm inside the mixed layer at the Hyytiälä site. The importance of IINSW seemed to increase in the free troposphere above the boundary layer, however, lack of measurements in the vertical structure of the input parameters suggest that the model results are burdened with high uncertainties.     

Relevance of ion-induced nucleation of sulfuric acid and water in the lower troposphere over the boreal forest at northern latitudes

The relevance of ion-induced nucleation of sulfuric acid and water (IINSW) in the troposphere over the boreal forest at northern latitudes is investigated by combining two existing and previously published models (MALTE — model to predict new aerosol formation in the lower troposphere; PARNUC — a parameterized steady-state model of neutral and ion-induced nucleation of sulfuric acid and water for atmospheric conditions). Simulations were performed for 4 days with observed new particle formation at ground level by using input data from the SMEAR II station in Hyytiälä, Finland. The selected days were chosen to cover a wide range of values of the parameters most relevant for IINSW. The results showed that ion-induced nucleation of sulfuric acid and water can contribute up to 15% to the total amount of newly formed particles in the size range of 3–10 nm inside the mixed layer at the Hyytiälä site. The importance of IINSW seemed to increase in the free troposphere above the boundary layer, however, lack of measurements in the vertical structure of the input parameters suggest that the model results are burdened with high uncertainties.     

On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

We present a theory for the formation of frozen aerosol particles in the Antarctic stratosphere, the coldest region of the Earth's stratosphere. The theory is applied specifically to the formation of polar stratospheric clouds. We suggest that the condensed ices are composed primarily of nitric acid and water with small admixtures of other compounds such as H₂SO₄ and HCl in solid solution. Our assumed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinctions observed in the winter polar stratosphere. Physical chemistry and thermodynamic considerations suggest that at temperatures between about 200 and 185 K, stratospheric particulates are composed primarily of frozen nitric acid solutions with a composition near that of the trihydrate. Available data suggest the particles are amorphous solid solutions and not in the crystalline hydrate form. At lower temperatures (i.e., below the forst point of pure water) cirrus-like ice clouds can form.     

基于NCEP资料的我国大气可降水量的计算及其时空分布

利用1948—2009年的NCEP再分析资料获取多年平均大气可降水量,分析我国大气可降水量的空间分布和季节变化,并选用2001年的资料与同期探空资料进行对比验证.结果表明:我国大气可降水量的空间分布总趋势是低纬大于高纬,平原大于高原,沿海地区大于内陆地区;季节变化明显,冬季大气可降水量较小,夏季较大;NCEP资料与探空资料的计算结果基本一致.     

Seasonal variations of number size distributions and mass concentrations of atmospheric particles in Beijing

Particle number and mass concentrations were measured in Beijing during the winter and summer periods in 2003, together with some other parameters including black carbon (BC) and meteorological conditions. Particle mass concentrations exhibited low seasonality, and the ratio of PM2.5/PM10 in winter was higher than that in summer. Particle number size distribution (PSD) was characterized by four modes and exhibited low seasonality. BC was well correlated with the number and mass concentrations of accumulation and coarse particles, indicating these size particles are related to anthropogenic activities.Particle mass and number concentrations (except ultra-fine and nucleation particles) followed well the trends of 13C concentration for the majority of the day, indicating that most particles were associated with primary emissions. The diurnal number distributions of accumulation and coarse mode particles were characterized by two peaks.     

Growth of homogeneously nucleated water droplets: a quantitative comparison of experiment and theory

The formation of aerosols proceeds through nucleation, growth and aging stages. The understanding of nucleation and droplet growth is essential for handling the more complex atmospheric condensation processes. To achieve this goal, measurements of the nucleation rate of various systems are performed in an expansion chamber. In this manner nucleation and growth are decoupled by applying a short nucleation pulse of about 1 ms during which the nuclei are formed. The subsequent droplet growth is quantitatively monitored by Mie-scattering. To this end, the Mie-maxima and -minima are detected as a function of time and compared to theoretical Mie-scattering calculations for increasing radii. In this fashion, a wealth of growth curves for pure water depending on supersaturations, number densities of droplets, and temperatures were obtained. Following the approach of Fuchs and Sutugin [Fuchs, N.A., Sutugin, A.G., 1970. Highly Dispersed Aerosols. Ann Arbor Science Publishers, Ann Arbor; Fuchs, N.A., Sutugin, A.G., 1971. In: Hidy, G.M., Brock, J.R. (Eds.), International Reviews in Aerosol Physics and Chemistry: Topics in Current Aerosol Research (Part 2), Pergamon, New York, p. 1], we calculated theoretical growth curves taking into account the depletion of water vapor, the increase of droplet- and system-temperature, temperature-dependent functions of the diffusion coefficient, surface tension, liquid density and latent heat of condensation. The calculated growth curves and experimental data for 230, 240 and 250 K with number densities of droplets between 5×10² and 2×10⁶ droplets/cm³ yield quantitative agreement between theory and experiment. This is remarkable in so far as the theory contains no adjustable parameters and assumes the sticking probability of the vapor molecules to be unity. Using a sticking probability smaller than 0.8 in the calculation leads to growth functions already outside the experimental error.     

Kinetics of ammonia and ammonium ion inhibition of the atmospheric oxidation of aqueous sulfur dioxide by oxygen

This is the first study, which shows both NH₃ and NH₄⁺ to inhibit the autoxidation of aqueous SO₂ in the pH range 7.0–8.5. The rate of the autoxidation, R _aut , in both buffered and unbuffered media at a fixed pH is in conformity with the rate law:

A photoelectric detector for the measurement of photolysis frequencies of ozone and other atmospheric molecules

Photoelectric detectors for the measurement of photolysis frequencies of different trace gases in the atmosphere are described. They exhibit uniform response characteristics over one hemisphere (2 sr) and wavelength characteristics closely matched to those of the photolysis frequencies J _O1D, J _NO2, and J _NO3, respectively. Absolute calibration of the J _O1D detector was performed by chemical actinometry with an accuracy of ±16 percent. Simultaneous measurements of J _NO2 and J _O1D are presented.     

六盘山区夏秋季大气水汽和液态水特征初步分析

六盘山区是中国典型的农牧交错带和生态脆弱带,也是黄土高原重要的水源涵养地、生态保护区及国家级扶贫开发区。利用2017年6-11月隆德气象站地基多通道微波辐射计资料,结合同期平凉探空站及隆德地面降水等观测资料,分析了六盘山区夏秋季大气水汽、液态水变化特征。结果表明：六盘山区夏秋季在降水天气背景下,大气水汽含量和液态水含量均较高,分别为无降水天气背景下的1.4倍和7.0倍;降水天气背景下水汽在5000 m以下有明显的增加,且在此高度范围内的水汽密度随高度的递减率比无降水天气背景下明显偏小;各高度层的液态水相比无降水天气背景下均有明显增大,除6月外,主峰值均出现在0℃层高度层以下。六盘山区夏秋季各月中,6-9月。大气水汽含量高值区均出现在正午到傍晚时段,低值区均出现在日出前后;液态水含量在日出前、午后及傍晚分别出现峰值,最明显的峰值出现在午后。对一次对流性降水天气过程分析后发现,降水发生前40 min大气水汽含量和液态水含量出现两次明显的跃增,水汽向上输送不断加强,2500-7500 m高度的相对湿度明显增大。     

Direct human influence of irrigation on atmospheric water vapour and climate

Human activity increases the atmospheric water vapour content in an indirect way through climate feedbacks. We conclude here that human activity also has a direct influence on the water vapour concentration through irrigation. In idealised simulations we estimate a global mean radiative forcing in the range of 0.03 to +0.1 Wm^–2 due to the increase in water vapour from irrigation. However, because the water cycle is embodied in the climate system, irrigation has a more complex influence on climate. We also simulate a change in the temperature vertical profile and a large surface cooling of up to 0.8 K over irrigated land areas. This is of opposite sign than expected from the radiative forcing alone, and this questions the applicability of the radiative forcing concept for such a climatic perturbation. Further, this study shows stronger links than previously recognised between climate change and freshwater scarcity which are environmental issues of paramount importance for the twenty first century.     

Emissions of ammonia from weeping wall stores and earth-banked lagoons determined using passive sampling and atmospheric dispersion modelling

Ammonia emissions from stored farm manures form a small but significant proportion (∼10%) of the total emitted annually from UK sources. These emissions are regulated by factors including: the surface area of the store; the storage method; the physical form of the stored manure and the source of manure. A method was developed to estimate in situ emissions from a range of store types (weeping wall and earth-banked lagoon) that are currently under-represented in UK emissions estimates. Passive diffusion samplers (Willems Badges) were used to determine vertical concentration profiles to a height of 4.5 m at a number of locations around each slurry store. An atmospheric dispersion model was applied to estimate the contribution from emissions from other on-farm ammonia sources to the measured data and also to determine the emission rates from the stored manure. A procedure was applied whereby the emission rates from each source were allowed to vary and a numerical equation solver was applied to backfit the modelled data set to the field measurements. Measurements were collected at four farms on a monthly basis throughout the year, with each dataset being collected over 24 h. The uncertainties in the estimates of emissions from the slurry stores during individual measurement periods typically ranged between 20–40% though higher uncertainties occurred when emission fluxes from the stores were below 0.25 g NH₃–N m⁻² day⁻¹ and were entrained in the wakes, and mixed with the emissions, of adjacent buildings. The average emission from the farms was 0.6 g NH₃–N m⁻² day⁻¹ which agrees with other recent data on ammonia emissions from crusted slurry stores and, though it is within the range of data considered in the UK emissions inventory, suggests that emissions from weeping wall stores and earth-banked lagoons may be currently overestimated in national predictions.     

Homogeneous freezing of single sulfuric and nitric acid solution drops levitated in an acoustic trap

The freezing temperatures of single supercooled drops of binary and ternary sulfuric and nitric acid solutions were measured while varying the acid concentration. An acoustic levitator was used which allows to freely suspend single solution drops in air without electrical charges thereby avoiding any electrical influences which may affect the freezing process. The drops of typically 500 µm in radius were monitored by a video camera during cooling cycles down to − 85 °C to simulate the upper tropospheric and stratospheric temperature range. The present data confirm that liquid solution droplets can be supercooled far below the equilibrium melting point by approximately 35 °C. They follow the general trend of the expected freezing temperatures for homogeneous ice nucleation.     

Determination of water vapor and liquid water content by an iterative method

Summary A simple method of retrieving water vapor and liquid water content is presented and validated by applying the Special Sensor Microwave/Imager data using ground truth data from Japan. The method is based on an iterative technique which uses model functions of relating two geophysical parameters to brightness temperature. Water vapor is found by a model function of relating water vapor content to brightness temperature at 22.235 GHz. Liquid water content is found by two model functions. One function defines a level of clear sky condition, and the other gives a ratio of liquid water content to brightness temperature increased from clear sky conditions. The retrieved water vaporcontent is compared with upper air observations at Chichijima Island. The rms of errors is estimated at 3.3 Kg m^–2. The retrieved liquid water content is related to monthly precipitation observed at Chichijima Island, and a correlation coefficient of 0.68 is obtained.With 7 Figures     

水面粗糙度可变时的定常中性大气边界层数值模式

本文将Blackadar的中性大气边界层数值模式推广到水面上的大气边界层,其中粗糙度是摩擦速度的函数.解得的若干边界层特征参数满意地符合实测结果和理论考虑,因此,本模式可用来计算水面边界层中不同高度的风速,只要知道地转风和地理纬度即可.最后,将模式推广到空气动力学光滑流的情况.     

邢台市大气水汽及云水变化的降水前兆分析

利用MWP967KV型地基微波辐射计及红外观测仪探测数据,对邢台市2016年发生降水前的水汽含量(IWV)、液态水含量(ILW)和云底高度变化特征进行了分析.结果表明,云底高度的持续明显下降提前约1h于IWV的明显升高,IWV的明显增加提前约1h于ILW的明显升高;IWV呈持续增加时间≥3h且IWV≥4.00cm,IL...