Filter-based differential hygroscopicity analyzer of aerosol particles

We describe a new differential analyzer implementing a technique for studying the hygroscopic properties of filter-precipitated aerosol particles based on a katharometric measurement of the amount of water vapor absorbed by an aerosol sample. The instrument has been tested on particles of sodium chloride and ammonium sulphate. A comparison of our data with the results of analogous measurements described in literature shows that the suggested technique has several important advantages, i.e., (1) higher sensitivity, which allows the measurement of particles of no more than 0.1 mg in mass; (2) a wide range of relative humidity variations (up to 99% at an accuracy of 0.06% RH at the upper-range value); (3) the absence of intermediate measurement steps connected with the need to account for water absorption by elements of a measurement system; and (4) the absence of restrictions to the size and shape of particles studied. In addition, the measurement technique rules out the possibility of errors caused by the kinetic effects of mass transport in the aerosol-water vapor system.     

Formation of cloud microstructure during hygroscopic seeding

The evolution of cloud microstructure initiated by hygroscopic seeding is studied on the basis of numerical simulation of cloud formation in the initial stage of condensation. The influence of both physicochemical properties of atmospheric aerosol and atmospheric conditions controlling the cloud type on the microstructure of a developing cloud (without hygroscopic seeding) is analyzed. It is shown that cloud seeding with additional particles whose sizes exceed the characteristic size of atmospheric condensation nuclei leads to a decrease in the concentration of cloud droplets and an increase in their sizes. This result of cloud seeding represents a positive effect for stimulation of precipitation from convective clouds. It is shown that this positive effect is achieved if there are some relationships between the parameters characterizing the hygroscopic particles and the atmospheric conditions. In particular, the maximum effect of action can be achieved at some optimal concentration of seeded particles. The decrease in the concentration of cloud droplets because of hygroscopic seeding is compared to the results of numerical simulations performed by other authors with allowance for coagulation processes in clouds. It is shown that this decrease can serve as an estimate for the effectiveness of hygroscopic seeding as a means for artificial intensification of precipitation from convective clouds.     

Study of the possibility of stimulating precipitation from warm convective clouds by hygroscopic particles from numerical simulation

We present the results of numerical simulation of the action of hygroscopic particles on a convective cloud for obtaining additional precipitation. The correspondence of vertical profiles of cloud parameters to those actually observed under natural atmospheric conditions is achieved within a one-dimensional numerical model by parametrization of the process of heat and moisture entrainment into the upward air flow forming the cloud. The model describes in detail microphysical processes in a cloud with the use of the kinetic equation for the size distribution of cloud droplets. The processes of forming precipitation in convective clouds with a vertical thickness of 3–4 km during their natural development and during the introduction of hygroscopic particles are analyzed using numerical calculations. It is shown that it is actually possible to obtain additional precipitation from convective clouds of continental type under the action of hygroscopic particles with sizes of 1–1.5 μm. The results of calculating the intensity and total amount of precipitation as functions of the vertical thickness of a cloud and the parameters of particles introduced into it are presented. The conditions necessary for obtaining the maximum positive effect are elucidated.     

On the Nature of Aerosol Particles in the Atmosphere of Irkutsk

Monitoring data on the ion composition of precipitation and the water-soluble fraction of aerosol have been used to identify two types of aerosol particles in the surface atmosphere of Irkutsk (“metal” and “ammonia” groups). The aerosol acidity is basically governed by the acidity of ammonia particles, and the ion composition depends on air relative humidity (RH). Preliminary estimates are given for the distribution of major cations and anions by aerosol groups.     

青岛近海海域气溶胶干沉降通量模拟研究I-Williams干沉降模型中潮湿粒子增长效应的改进

为了计算青岛近海海域气溶胶粒子的干沉降通量，运用Gerber提出的湿度公式改进了Williams干沉降模型中湿度计算方法，使模型具有更加广泛的使用范围。利用改进后的模型讨论了湿度、风速、水气温差、破碎表面的转移系数和横向转移系数对不同粒径气溶胶粒子干沉降速率的影响。计算了不同粒径粒子的干沉降速率，并与干沉降速率的文献报道进行了比较。结果显示：改进的模型更适合于估算实际区域的气溶胶干沉降通量，可用于青岛近海干沉降通量的研究。     

On the influence of atmospheric chemical reactions on the ion composition of aerosol particles in the Baikal region

Monitoring data on the ion composition of aerosols and gas admixtures in the background and polluted atmosphere of the Lake Baikal region are presented. The ion composition and morphology of aerosols are affected by heterogeneous chemical reactions and variations in relative humidity. Two types of aerosol particles are revealed over this region. The fraction of solid particles recorded in most episodes includes primarily carbonates of alkaline and alkaline-earth metals. With increased atmospheric humidity, these particles are engaged in heterogeneous chemical reactions with gas-phase NH₃ and H₂SO₄, proceeding through the phase of watering. As a result, the composition of these aerosols is changed, and a fraction of aqueous H₂O/H₂SO₄/(NH₄)₂SO₄ aerosol particles of a different composition is formed. On the basis of a physical and chemical analysis of monitoring data on the aerosol composition and concentrations of gas admixtures, the average aerosol-size distribution of different types is estimated. For the first time, the mean acidity of aqueous aerosol particles is estimated.     

Brown Carbon and Black Carbon in the Smoky Atmosphere during Boreal Forest Fires

We have investigated the variability of smoke aerosol absorbing ability with variations in the content of brown carbon (BrC) and black carbon (BC). Using monitoring data on radiative characteristics of smoke aerosol at AERONET stations and the spatial distribution of aerosol optical depth (AOD) obtained by the MODIS spectrometer (Terra satellite), we have detected large-scale smokes during boreal forest fires in Russia and Canada (1995–2012). The spatial distribution (50°–70° N, 95°–125° W) and temporal variability (at AERONET station Fort McMurray) of AOD during the smoking of a part of Canada in July 2012 have been analyzed. AOD probability distributions for July 14–18, 2012, and an estimate of aerosol radiative forcing of smoke aerosol at the upper boundary of the atmosphere have been obtained. We have proposed a technique for the diagnostics of BrC and BC in smoke aerosol particles from the spectral dependence of the imaginary part of the refractive index. At a wavelength of 440 nm, the contributions of BrC and BC to the smokeaerosol absorbing abitity can be comparable in magnitude. In many cases, the absorption spectra of smoke aerosol can be adequately approximated by either power or exponential functions. The presence of BrC in smoke-aerosol particles highly extends the variety of observed absorption spectra in a smoky atmosphere and spectral dependences of single scattering albedo. In the spectral range of 440–1020 nm, the radiative characteristics of smoke aerosol are largely contributed by its fine mode.     

The effect of atmospheric circulation on the evolution and radiative forcing of smoke aerosol over European Russia during the summer of 2010

The evolution of smoke plume over European Russia (ER) during the massive forest and peatbog fires of summer 2010 has been studied using observations of aerosol optical depth (AOD) from MODIS instruments (both Aqua and Terra platforms), objective analysis of meteorological fields performed at the Russian Hydrometeorological Research Center, NCEP/NCAR reanalysis, as well as upper air data. A relation between the structure inhomogeneities of the AOD field and regional atmospheric circulation has been found. It is shown that, on August 5–9, 2010, the maximum of smoke pollution did complete turn around Moscow, while remaining at a distance of 200 to 650 km from the megacity. Both regionally averaged shortwave aerosol radiative forcings (ARFs) at the top and the bottom of the atmosphere are estimated for the period of extreme smoke pollution over ER. The spatial distributions of ARF values over the territory of the region and the estimates of the local and spatially distributed thermal effects of smoke aerosol are given. It is shown that, on August 5–9, 2010, the spatial distribution of AOD and the calculated thermal effects of smoke aerosol were in agreement with the spatial distributions of air-temperature anomalies observed in the lower 1.5-km layer of the atmosphere. MODIS’s AOD data obtained during the wildfires were validated by AOD observations from the CIMEL sun photometer operated at the AERONET station Zvenigorod.     

Sensitivity of large-scale atmospheric analyses to humidity observations and its impact on the global water cycle and tropical and extratropical weather systems in ERA40

Reanalysis data obtained from data assimilation are increasingly used for diagnostic studies of the general circulation of the atmosphere, for the validation of modelling experiments and for estimating energy and water fluxes between the Earth surface and the atmosphere. Because fluxes are not specifically observed, but determined by the data assimilation system, they are not only influenced by the utilized observations but also by model physics and dynamics and by the assimilation method. In order to better understand the relative importance of humidity observations for the determination of the hydrological cycle, in this paper we describe an assimilation experiment using the ERA40 reanalysis system where all humidity data have been excluded from the observational data base. The surprising result is that the model, driven by the time evolution of wind, temperature and surface pressure, is able to almost completely reconstitute the large-scale hydrological cycle of the control assimilation without the use of any humidity data. In addition, analysis of the individual weather systems in the extratropics and tropics using an objective feature tracking analysis indicates that the humidity data have very little impact on these systems. We include a discussion of these results and possible consequences for the way moisture information is assimilated, as well as the potential consequences for the design of observing systems for climate monitoring. It is further suggested, with support from a simple assimilation study with another model, that model physics and dynamics play a decisive role for the hydrological cycle, stressing the need to better understand these aspects of model parametrization.     

Retrieval of integral parameters of tropospheric aerosol from two-wavelength lidar sounding

A scheme of interpreting the data of two-wavelength lidar sounding is proposed. The scheme is based on functional relationships between the lidar ratios and between some integral characteristics of aerosol and the ratio of the backscattering coefficients at the sounding wavelengths. The AERONET data, results of contact aerosol measurements and multiwavelength lidar sounding, and the OPAC aerosol model are used to find these functional relationships, which are statistical in character. Analysis of data is made separately for continental, dust, oceanic, and smoke aerosols. Backscattering for mineral aerosol fractions are calculated for a model of randomly oriented spheroids. A numerical experiment shows that the errors in determining a number of integral parameters of aerosol (extinction coefficient, characteristic radius of particles, volume concentrations) that are due to the statistical straggling of lidar ratios and other specified integral characteristics are no greater than 32% if the optical thickness of the sounding layer is no greater than 1.     

Humidity of the tropical lower stratosphere: Observations and analysis

The results of measurements of water-vapor vertical profiles in the upper troposphere and stratosphere on board a meteorological balloon with a FLASH-B optical fluorescent hygrometer (Russia) are presented. These data were obtained during two international field campaigns in West Africa (August 2006) and Central America (August 2007). Eleven high-resolution water-vapor vertical profiles measured in the course of these works make it possible to characterize the processes controlling humidity in the tropical tropopause region. Layers with increased humidity are detected in the lower stratosphere over West Africa to the level of the potential temperature 450 K. An analysis of satellite maps of the brightness temperature, balloon ozone measurements, and aerosol scattering, as well as trajectory modeling, display the relation between the observed layers with increased humidity and the phenomena of convective overshooting of the tropopause, as a result of which cold and ozone-depleted air penetrates into the lower stratosphere together with ice particles, which, rapidly sublimating, locally increase the water-vapor concentration. A comparison of the humidity data obtained in West Africa in 2006 and in Central America in 2007 reveals substantial distinctions in values and vertical structures of water vapor, both in the tropopause region and in the middle stratosphere.     

On the effect of the coastal zone wind regime on the optical characteristics of haze

Based on an experimental study of directed dissipation coefficients and aerosol microstructure in the coastal area the problem of wind regime manifestation is considered. It is shown that the main changes of parameters of dissipation indicatrix form near angles =15°–165°, which are conditioned by submicron fractions of aerosol particles, take place without regard for wind regime. Usually they are defined by effect of relative air humidity. It is found that specific manifestations of wind regime are observed close to small dissipation angles and are conditioned by the effect of coarse-dispersed aerosol fractions.UDK 551.593     

Radiative and Thermal Impacts of Smoke Aerosol Longwave Absorption during Fires in the Moscow Region in Summer 2010

The aerosol longwave radiative forcing of the atmosphere and heating rate of the near-surface aerosol layer are estimated for the extreme smoke conditions in the Moscow region in summer 2010. Thermal radiation fluxes in the atmosphere are determined using the integral transmission function and semiempirical aerosol model developed on the basis of standard aerosol models and measurements at the Zvenigorod Scientific Station, Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences. The aerosol radiative forcing reached 33 W/m² at the lower atmospheric boundary and ranged between–1.0 and 1.0 W/m² at the upper atmospheric boundary. The heating rate of the 10-m atmospheric layer near surface was up to 0.2 K/h during the maximum smoke conditions on August 7–9. The sensitivity of the aerosol longwave radiative forcing to the changes in the aerosol absorption coefficient and aerosol optical thickness are estimated.     

Electrization of aerosol wetted in bipolarly ionized air

We studied the influence of the characteristics of the atmospheric ionization and physical-chemical state of condensation nuclei on the electric state of convective cells. Based on the results of experiments in an adiabatic chamber with a volume of 3200 m³, we found that, with increase in relative air humidity H from 40 to 95% with an equivalent ascent rate of 100–400 cm/s, excessive charges in amounts of about 10³ or more elementary charges per cm3 may be accumulated on the nuclei. The sign of the charge depends on the chemical composition of the hygroscopic nuclei. For instance, media with insoluble nuclei (porous silica, etc.) typically have prevailing negative charges; those with soluble nuclei (sodium chloride, etc.) are dominated by positive charges. At H = 60−90%, the electrization of soluble nuclei can be interpreted in the diffusion-kinetic models of the ion charging of aerosols. Considerable negative volume charges, which appear on insoluble hygroscopic nuclei during a rise in humidity from 40 to 70%, are explained by the structuring of surface water films, which exhibit a resemblance to negative lightweight ions. At high values (H > 90%), it is necessary to take into account the resemblance of the wetted surfaces to positive lightweight ions. We showed for the first time that, at ion formation rates of 3 and 1010 ion pairs/(cm³ s), the differences in the volume charge and wetting rate of condensation nuclei are insignificant. It is concluded that, in many meteorological situations, the first stage of electrization of the convection-derived cloud media is the ion charging of the condensation nuclei.     

Modeling radiative forcing by background aerosol on the basis of measurement data

The solar radiation flux incident on the land surface and aerosol radiative forcing are calculated from measurements carried out under clear skies during the summers of 2004 and 2005 at the Zvenigorod Scientific Station (ZSS) of the A.M. Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences. In these calculations, the following five models of aerosol optical parameters are used: a standard model of continental aerosol, a semiempirical model based on measurement data, and three models obtained from calculations on the basis of the Mie scattering theory for the mean size distribution of aerosol particles (which is retrieved from aureole measurements). A study of the sensitivity of the flux and forcing to the choice of aerosol model has shown that the relative error related to the model choice is not large (<5%) for the incident radiation flux and reaches 120% for aerosol forcing at the atmospheric upper boundary. The aerosol radiative forcing at the atmospheric upper boundary is also estimated and, according to our calculations, varies from −15 to −2 W/m². The use (in calculations) of the values of the albedo of single-scattering and the factor of scattering-indicatrix asymmetry at a wavelength of 550 nm, which were obtained for each of the observation periods, has made it possible to significantly refine the value of aerosol radiative forcing (compared to that calculated for the means of these parameters over all the periods). An even more accurate determination of aerosol radiative forcing is possible only when data on the size-distribution of aerosol particles and their chemical composition for a certain situation under analysis are available. As a result of this study, two models of the optical parameters of background aerosol have been proposed for use in radiation calculations: a semiempirical model and a mean model obtained from the calculations based on the theory of scattering. Both models use the values of the albedo of single scattering and the factor of asymmetry (at a wavelength of 550 nm) retrieved from the measurements for each of the observation periods.     

On the use of poorly soluble hygroscopic substances for modification of warm clouds and fogs

From analysis of the relationships between the equilibrium state of condensation nuclei and the relative humidity, a conclusion is made concerning the preferred use of poorly soluble substances for the generation of artificial condensation nuclei (ACN) designed for modification of warm clouds and fogs with the purpose of their dissipation and precipitation formation. The advantage of poorly soluble substances over commonly used soluble salts is that the finely dispersed part of the spectrum of the poorly soluble ACN does not deliquesce and so is not involved in the formation of cloud droplets. For experimental testing of the conclusions, preference was given to cement, whose main soluble substance is calcium oxide with a solubility of about 1 g/l. The spectrum of dispersed cement particles was measured and compared with the spectra of pyrotechnic flares widely used for modification at present. The process of formation of the cloud droplet spectra was simulated in the aerosol chamber of the Institute of Experimental Meteorology by decreasing the preliminarily generated excess pressure. It was found in these experiments that, compared to the spectra of particles formed on background condensation nuclei, the introduction of dispersed cement leads to the broadening of spectra and to a decrease in the concentration of droplets. Even at the early stage of condensation, droplets with radii of ∼20 μm appear. In this case, no “overseeding” phenomenon is observed, which, for soluble substances, manifests itself in an increase in the concentration of cloud droplets with a large ACN concentration. These effects indicate that, according to the existing concepts about the mechanism of warm-cloud modification with hygroscopic substances, the introduction of poorly soluble ACN (in particular, dispersed cement) below the base of cumulus clouds should stimulate coagulation processes and accelerate rain-formation processes. Considerations are given that the introduction of poorly soluble ACN into the already existing cumulus or stratocumulus clouds or fogs should also result in the acceleration of precipitation-formation processes or cloud dispersal. Comparison of cement powder with the well-known means of warm-cloud and fog modification is carried out. Original Russian Text ? N.P. Romanov, A.S. Drofa, N.S. Kim, A.V. Savchenko, G.F. Yaskevich, 2006, published in Izvestiya AN. Fizika Atmosfery i Okeana, 2006, Vol. 42, No. 1, pp. 80–91.     

Structure and optical properties of soot aerosol in a moist atmosphere: 1. Structural changes of soot particles in the process of condensation

A laboratory setup and a procedure for measuring the volume coefficients and mean cross sections of extinction, scattering, and absorption of soot particles in the medium of saturated water vapor are described. A method for hydrophilization of the surface of soot particles, which makes it possible to obtain model objects with specified hygroscopic properties, is presented. The processes of transformation of soot particles are analyzed with the use of data of electron-microscopic investigations on the basis of the fractal approach. The structural parameters of hydrophobic soot are shown to depend on the conditions of moistening, whereas hydrophilic particles are subject to substantial structural changes indicative of their watering. Investigation of the coagulation of soot particles with drops shows that hydrophobic particles form a weakly bound system; they coagulate on the surface of drops and cause no changes in the structure of soot aggregates. During the coagulation, hydrophilic soot particles penetrate inside a drop and irreversibly form a mixed system.     

Investigation of the action of hygroscopic particles on a warm convective cloud from the results of numerical simulation

The results of a numerical simulation of the action of hygroscopic particles on a warm convective cloud with the purpose of obtaining additional precipitation are presented. The one-dimensional numerical model considered in this work describes the evolution of the cloud medium in the central part of an axisymmetric convective cloud at the specified height-variable velocity of the upward air flow which forms the cloud. Our model comprehensively describes microphysical processes in the cloud medium with the use of the kinetic equation for the size distribution of cloud droplets. This model makes it possible to obtain the spatiotemporal pattern of the cloud formation and development and to analyze regular features in the cloud evolution under the action of hygroscopic reagents. The cloud characteristics calculated with the use of this model correspond to the cloud parameters observed in natural conditions of the atmosphere. The process of precipitation stimulation by hygroscopic particles in convective clouds with vertical thicknesses of 2.5–4.5 km was analyzed on the basis of the results of numerical calculations. The results of calculations of the dependence of the intensity and total amount of precipitation on the vertical cloud thickness and parameters of particles introduced into the cloud are presented. It is shown that hygroscopic particles with root-mean-cube radii of 1–1.5 μm are the most effective for acting on warm convective clouds with the purpose of obtaining additional precipitation. In this case, the required reagent expenditure is 100–200 kg/km². The conditions necessary for obtaining the maximal positive effect of the action are elucidated.     

珠江三角洲及珠江口海区的空气微生物含量

１９９４年６，７月，调查了广州、深圳、珠海及珠江口海区的空气微生物粒子沉降量状况。发现空气微生物粒子总量、真菌粒子量、真菌粒子数／总菌粒子数百分比在三市中不一致。这三种数据一般是陆上的高于海上。随着距陆的增加，都市影响的减弱和海面的开阔，空气微生物含量呈减少之势，显示出海洋新鲜空气对陆上污染空气的调节、净化作用。文中还分析了空气微生物有关参数与气温、风力或相对湿度间的相关关系。     

The effect that coarse particles have on estimates of both optical and radiation characteristics of dust aerosol

Based on mathematical simulation, quantitative estimates of the effect that coarse dust particles have on the accuracy of retrieving the optical characteristics of aerosol have been obtained from the results of ground-based measurements of the spectral fluxes of both direct and scattered solar radiations. The results of verifying a retrieval algorithm (used at the AERONET ground-based network) based on special test models showed that the aerosol characteristics retrieved with this algorithm are unsuitable for calculating integral solar fluxes and for simulating space spectrometric IR measurements when the concentration of dust particles in the atmosphere exceeds their concentration in the well-known CONT model of continental aerosol by a factor of two or more.