Measurements of natural ice nuclei with a continuous flow diffusion chamber

Measurements of natural ice nuclei were made in winter continental airmasses with a continuous flow thermal gradient diffusion chamber (described in a separate paper). Over the range of temperatures −7°C to −20°C, the concentration of ice nuclei was closely related to ice supersaturation (SS_i) for humidities both below and above water saturation. Measurements below water saturation were interpreted as deposition nuclei with average concentrations (per liter) approximately 0.32 SS_i(%)^0.81. Measurements were made up to 5% above water saturation and activated both deposition and condensation-freezing nuclei. The average concentration of condensation-freezing nuclei was 0.25 e^{−0.15 T(°C)}. Sample residence time in the chamber was probably too small to detect contact nuclei, unless the nucleating aerosols are extremely small. There was large variability in nucleus concentrations, as much as two orders of magnitude at −15°C. Comparisons are made between these ice nuclei measurements and aircraft observations of ice crystal concentrations in winter orographic clouds.     

Aerosol over the Southern Ocean

In a first attempt to assess a proposed climatic change feedback process involving cloud condensation nuclei (CCN) and cloud albedo, CCN concentrations N as a function of supersaturation S were measured on a voyage from latitude 43 to 65°S in October–November 1988. The usual relationship N=CS^k, with k=0.5 and C a constant was a fair apprraximation for S in the range 0.3–0.7% implying that CCN concentrations should largely determine cloud drop concentrations and hence albedo for clouds with S in that range. South of latitude 50°S and at smaller S,k was 1 or larger on average, which would lead to reduced dependence of albedo on CCN for the relevant clouds. N varied very widely for separations of the order of 100 km or 6 hours in time, particularly when the sea was partly ice-covered, suggesting strong local influences. During a large increase in N 60°S, unaccompanied by an increase in condensation nuclei (CN), cloud drops grew more rapidly than usual. In a subsidiary experiment particles were collected and examined by transmission electron microscopy. For particles less than 0.2 μm diameter, 80–90% appeared to consist of ammonium sulfate, the remainder being sea salt or an unknown substance which was more liquid and heat-resistant. Dialysis showed that the sulfate particles contained a few percent of insoluble material. Particles which formed cloud drops in vapours other water, were also studied. Comparison of these and water CCN and the rates of droplet suggested that the water insoluble portion of the particles was ethanol-soluble and surface-active. CN concentrations decreased by a factor of about 2 between 43 and 65°S, a change closely paralleled by ethanol CCN concentrations.     

Statistical analysis of microphysical properties and the parameterization of effective radius of warm clouds in Beijing area

In this paper warm cloud microphysical parameters including cloud droplet number concentration (N_c), liquid water content (q_l) and effective radius (r_e) from 75 flights around the Beijing area during 2005 and 2006 are summarized. Average N_c (cm^− 3) for Cu, Sc, Ac, As and Ns are 376 ± 290, 257 ± 226, 147 ± 112, 60 ± 35 and 60 ± 84, respectively. Many records of high N_c above 1000 cm^− 3 are observed. The large standard deviations indicate a large variation of N_c and q_l in this region. The maxima of q_l reach 1.4 g m^− 3 in Cu and 1.0 g m^− 3 in Sc, respectively. Different parameterizations of effective radius are examined with the in-situ data in this area. There are different ways to obtain the prefactor representing the relationship between effective radius and mean volume radius. Significant systematic errors are found to be at the large sizes when the prefactor is expressed with relative dispersion under the Gamma Distribution. Fixed prefactor of 1, which was widely used, even produces much larger error. A prefactor of 1.22 is found to be better than the former two methods by fitting with the observed data. The effective radius is further parameterized as functions of mean volume radius, liquid water content and cloud droplet number concentration. We suggest that the effective radius can be parameterized as r_e,p ≈ 1.20r_v + 0.22–1.28/r_v², which is a practical and more accurate scheme without too much computation complexity.     

Study of an unexpected convective storm

The occurrence of a severe storm in the Argentine littoral has been analyzed. Although general atmospheric conditions were not favorable to the development of deep convection, this storm produced strong winds and hail of considerable intensity. Its occurrence was associated with the entrance of a pulse of humid air at low levels and could be related to the development of two vorticity centers in the region. Atmospheric conditions existing above a low-level inversion are used to simulate two possible clouds, with base altitudes at 2200 and 3000 m and updraft speeds reaching maximum values of 27 and 29 m s⁻¹ respectively. It is noted that the base temperature of about 13°C, found for the first cloud, can be correlated with the prevalence of frozen drop embryos, observed in an analyzed hailstone sample. Hailstone vertical trajectories are simulated in both modeled clouds, assuming spheroidal and spherical particles and assigning different values to the drag coefficient C_d.     

Influence of drizzle on Z–M relationships in warm clouds

This paper addresses the sensitivity of the relationships between radar reflectivity (Z) and liquid water content (M) for liquid water clouds to microphysical drizzle parameters by means of simulated radar observation at a frequency of 3 GHz of modeled cumulus clouds. A power law relationship for non drizzling clouds with water content as high as 3 gm^− 3: Z_c = 0.026 M_c^1.61 is numerically derived and agreed with previous empirical relationships relative to cumulus and stratocumulus. This relationship is then used to explore the influence of drizzle on the correlation between radar reflectively and water content. Due to their large diameters with respect to cloud droplets, drizzle sized drops dominate radar reflectivity but do not carry the cloud water content so that reflectivity and liquid water content are expected to be not correlated in clouds containing drizzle. It is shown that for congestus or extreme congestus cumuli, microphysical conditions for which the Z_c–M_c relationship can be used with a tolerance of 5 and 10% are provided whereas for humilis or mediocris cumuli, the presence of drizzle breaks down the Z_c–M_c relationship whatever the situations.     

Calculation of cloud modification factors for the horizontal plane eye damaging ultraviolet radiation

This research examines the influence of cloud on the cataract effective UV (UV_Cat) irradiances on a horizontal plane over an extended period of 12months that included the range of cloud conditions, solar zenith angle (SZA) and ozone conditions experienced over that time. The data were collected at five minute intervals. Cloud modification factors were determined from the influence of clouds on the global broadband solar radiation and these were applied to the cloud free cataract effective UV to evaluate the UV_Cat irradiances on a horizontal plane for all cloud conditions. A comparison of the measured and calculated UV_Cat irradiances for the 2004 data set in the range of SZA of 70° or less provided an R² value of 0.85. The data in the first 6months of 2005 for an SZA of 70° or less that were at a different time to that when the technique was developed provided an R² value of 0.83 for the comparison of the measured and calculated UV_Cat irradiances.     

Parameterization of the shortwave radiative properties of water clouds for use in GCMs

Summary The influence of the micro- and macrophysics of water clouds on the scattering and radiative properties of clouds is investigated using versatile cloud drop size distributions (DSDs) and Mie theory for single scattering and the delta-Eddington approximation for multiple scattering. A new parameterization scheme for the shortwave radiative properties of water clouds is presented. As for single- scattering properties, a new parameterization for cloud optical thickness () is proposed. This is based upon the seperation of the dependence of on the total number of DSDs, the cloud thickness, and the liquid water content, combined with equivalent radius. The cloud bulk radiative properties, i.e., the flux reflectance, transmittance, and absorptance, are uniquely fitted by a dimensionless parameter (X) or the optical thickness. The parameterization is compared with other schemes. Finally, the features and potential use of the scheme are discussed.With 5 Figures     

Laser depolarization studies of simulated crystallized H2O/H2SO4 clouds

Laboratory experiments were carried out to investigate the linear depolarization ratios (LDRs) of crystallized H₂O/H₂SO₄ acid clouds at angles of 45°, 135° and 157° to the forward direction. LDR is the ratio of the returned energies in the planes of polarization perpendicular and parallel to that of the source (Sassen, 1974). Experiments were carried out for different concentrations of aqueous solution of sulfuric acid. A cloud of supercooled droplets is formed inside an experimental chamber kept in a walk-in cold room by heating an aqueous solution of sulfuric acid, and the ice crystal formation is initiated by momentarily introducing a rod dipped in liquid nitrogen into the cloud. A 2-mW polarized He:Ne laser beam is directed through the cloud and a photomultiplier tube measures the scattered intensity. It is found that the scattered energy is higher in the direction of 157° and 135° than that at 45°. Microscopic examination of the crystals formed from acid concentrations above 50% shows dark fuzzy spots on the surface of the ice crystals suggesting that this could be a film of acid drops. This film also alters the shape of the crystals, and the crystal boundaries are no longer sharp and well defined like that observed for pure water clouds and this is found to influence the LDR.     

Observational Diagnosis of Cloud Phase in the Winter Antarctic Atmosphere for Parameterizations in Climate Models

The cloud phase composition of cold clouds in the Antarctic atmosphere is explored using data from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instruments for the period 2000--2006. We used the averaged fraction of liquid-phase clouds out of the total cloud amount at the cloud tops since the value is comparable in the two measurements. MODIS data for the winter months (June, July, and August) reveal liquid cloud fraction out of the total cloud amount significantly decreases with decreasing cloud-top temperature below 0oC. In addition, the CALIOP vertical profiles show that below the ice clouds, low-lying liquid clouds are distributed over ～20% of the area. With increasing latitude, the liquid cloud fraction decreases as a function of the local temperature. The MODIS-observed relation between the cloud-top liquid fraction and cloud-top temperature is then applied to evaluate the cloud phase parameterization in climate models, in which condensed cloud water is repartitioned between liquid water and ice on the basis of the grid point temperature. It is found that models assuming overly high cut-offs (》-40oC) for the separation of ice clouds from mixed-phase clouds may significantly underestimate the liquid cloud fraction in the winter Antarctic atmosphere. Correction of the bias in the liquid cloud fraction would serve to reduce the large uncertainty in cloud radiative effects.     

Condensed water in tropical cyclone “Oliver”, 8 February 1993

On February 8, 1993, the NASA DC-8 aircraft profiled from 10,000 to 37,000 feet (3.1–11.3 km) pressure altitude in a stratified section of tropical cyclone “Oliver” over the Coral Sea northeast of Australia. Size, shape and phase of cloud and precipitation particles were measured with a 2-D Greyscale probe. Cloud/ precipitation particles changed from liquid to ice as soon as the freezing level was reached near 17,000 feet (5.2 km) pressure altitude. The cloud was completely glaciated at −5°C. There was no correlation between ice particle habit and ambient temperature. In the liquid phase, the precipitation-cloud drop concentration was 4.0 × 10³ m⁻³, the geometric mean diameter D_g=0.5−0.7 mm, and the liquid water content 0.7−1.9 g m⁻³. The largest particles anywhere in the cloud, dominated by fused dendrites at concentrations similar to that of raindrops (2.5 × 10³ m⁻³) but a higher condensed water content (5.4 g m⁻³ estimated) were found in the mixed phase; condensed water is removed very effectively from the mixed layer due to high settling velocities of the large mixed particles. The highest number concentration (4.9 × 10⁴ m⁻³), smallest size (D_g=0.3−0.4 mm), largest surface area (up to 2.6 × 10² cm² m⁻³ at 0.4−1.0 g m⁻³ of condensate) existed in the ice phase at the coldest temperature (−40°C) at 35,000 feet (10.7 km). Each cloud contained aerosol (haze particles) in addition to cloud particles. The aerosol total surface area exceeded that of the cirrus particles at the coldest temperature. Thus, aerosols must play a significant role in the upscattering of solar radiation. Light extinction (6.2 km⁻¹) and backscatter (0.8 sr⁻¹ km⁻¹) was highest in the coldest portion of the cirrus cloud at the highest altitude.     

Microphysical and optical features of polluted cooling tower clouds

In November 1993 an airborne field study was performed in order to investigate the microphysical and radiative properties of cooling tower water clouds initiated by water vapour emissions and polluted by the exhaust from coal-fired power plants. The number-median diameter of the droplet size distributions of these artificial clouds was in the range of 13 μm. The concentration of smaller droplets (diameters d_D < 10 μm) increased with height and horizontal distance from the cooling towers. Close to the cooling towers, bimodal spectra were found with a second mode at 19 μm. The liquid water content (LWC) ranged between 2 and 5 g/m³ and effective droplet radii (R_e) between 6 and 9 μm were measured. LWC and R_e decreased with altitude, whereas the droplet concentration (N_D) remained approximately constant (about 2000 cm⁻³ ). An enrichment of interstitial aerosol particles with particle diameters (d_p) smaller 0.2 μm compared to the power plant plume in the vicinity of the clouds was observed. Particle activation for d_m > 0.3 μm. was evident, especially in cooling tower clouds further apart and separated from their sources. Furthermore, radiation measurements were performed, which revealed differences in the vertical profiles of downwelling solar and UV radiation flux densities inside the clouds.The effective droplet radius R_e was parameterized in terms of LWC and N_D using equations known from literature. The close agreement between measured and parameterized Re indicates a similar coupling of R_e, LWC and N_D as in natural clouds.By means of Mie calculations, volume scattering coefficients and asymmetry factors are derived for both the cloud droplets and the aerosol particles. For the cloud droplets, the optical parameters were described by parameterizations from the literature. The results show, that the link between radiative and microphysical properties of natural clouds is not changed by the extreme pollution of the artificial clouds.     

Radiative energy partition and cloud radiative forcing at a Po valley site

Values of downward and upward flux densities of solar and terrestrial radiation were continuously recorded between 1 December 2001 and 30 November 2002 using a four-components radiometer at S. Pietro Capofiume (SPC) in northern Italy (44°39′N, 11°37′E, alt. 11 m a.m.s.l.), which is characterized by a weakly-reflective surface. The aim of the study was to investigate the effects of clouds on surface radiation balance (SRB); the cloud fraction (N) has been retrieved through the inverted form of the parameterization proposed by Kasten and Czeplak [Solar Energy 24 (1980) 177] and cloud types estimated following the methodology of Duchon and O'Malley [J. Appl. Meteorol. 38 (1999) 132]. The cloud radiative forcing (CRF) was evaluated through the Bintanja and Van den Broeke [Int. J. Climatol. 16 (1996) 1281] formula and then associated with cloud type. Experimental results showed that during the measuring period the net shortwave (Sw) balance always decreased with increasing N, whereas the net longwave (Lw) balance increased in all seasons. The net radiation available at the surface decreased with increasing N in all seasons except in winter, where no significant dependency was detected.The analysis of the cloud radiative forcing indicates that all seasons were characterized by a net cooling of the surface except winter, where clouds seem to have no effects on the surface warming or cooling. Taking into account the dependence on solar radiation cycle, an intercomparison between the retrieved cloud types seems to indicate that the effect of stratus was a slight cooling whereas that of cumulus clouds was a stronger cooling of the surface. On the contrary, cirrus clouds seem to have slight warming effect on the surface.The annual trends of mean monthly values of shortwave and longwave radiation balances confirmed that the measurement site is characterized by a temperate climate. Moreover, in spite of the cooling effect of clouds, a monthly radiative energy surplus is available all year long for surface–atmosphere energy exchanges. The analysis is also instrumental for the detection of SRB variations.     

Numerical simulation of the relationship between electrification and microphysics in the prelightning stage of thunderstorms

To further investigate the influence of cloud base temperature, updraft velocity and precipitation particle constitution on cloud electrification, five thunderstorms in various regions of China were simulated by using the three-dimensional compressible hailstorm numerical model including inductive and non-inductive charging mechanisms. The results indicate that changes of cloud base temperature have an influence on the initial electrification. Comparison of the above cases shows that in the case of warm cloud base and moderate updraft velocity (< 20 m s^{−  1}), active electrification occurred below the − 10 °C level before moving upward to the − 20 °C level. In contrast, when cloud base is cold and updraft velocity is intensive, the main charging region is at the − 20 °C or even higher level. In that case, the vertical extent of the main negative charge region becomes larger with the increase of cloud base temperature. Apart from the main dipolar or tripolar charge structure, some smaller charge regions with relatively high values of charge density may also appear. Frozen drops, originating mainly from supercooled raindrops, mainly get electrified through charging interactions with snow at or below the − 20 °C level. They are responsible for the negative charge region near the melting level at the initial stage of precipitation if there is a large supercooled raindrop content. Non-inductive charging during hail-snow collisions is rather weak, resulting in the charge density on hail of no more than − 0.01 nC m^− 3.     

Nearly steady convection and the boundary-layer budgets of water vapor and sensible heat

The budgets of water vapor and sensible heat in the convective atmospheric boundary (mixed) layer are analyzed by means of a simple slab approach adapted to steady large-scale advective conditions with radiation and cloud activity. The entrainment flux for sensible heat is assumed to be a linear function of the surface flux. The flux of water vapor at the top of the mixed layer is parameterized by extending the first-order Betts-Deardorff approach, i.e., by adopting linear changes for both the specific humidity and the flux across the mixed layer and across the inversion layer of finite thickness. In this way the dissimilarity of sensible heat and water vapor transport in the mixed layer can be taken into account. The experimental data were obtained from the Air Mass Transformation Experiment (AMTEX). The entrainment constant for sensible heat at the top of the mixed layer was found to have values similar to those observed in other weakly convective situations, i.e., around 0.4 to 0.6. This appears to indicate that the effect of mechanical turbulence was not negligible; however, the inclusion of this effect in the formulation did not improve the correlation. In contrast to the first-order approach, the zero-order approach, i. e., the jump equation commonly used for the flux of a scalar at the inversion, (ovwc ) _h = w_e c (where w _e is the entrainment velocity and c the concentration jump across the inversion), was found to be invalid and incapable of describing the data.     

Ice crystal shape effects on solar radiative properties of Arctic mixed-phase clouds—Dependence on microphysical properties

Based on 1-year cloud measurements with radar and microwave radiometer broadband solar radiative transfer simulations were performed to quantify the impact of different ice crystal shapes of Arctic mixed-phase clouds on their radiative properties (reflectance, transmittance and absorptance). The ice crystal shape effects were investigated as a function of microphysical cloud properties (ice volume fraction f_i, ice and liquid water content IWC and LWC, mean particle diameter D_m^I and D_m^W of ice/water particle number size distributions, NSDs).The required NSDs were statistically derived from radar data. The NSD was composed of a liquid and a solid mode defined by LWC, D_m^W (water mode) and IWC, D_m^I (ice mode). It was found that the ratio of D_m^I and D_m^W determines the magnitude of the shape effect. For mixed-phase clouds with D_m^I ≤ 27 μm a significant shape effect was obtained. The shape effect was almost insensitive with regard to the solar zenith angle, but highly sensitive to the ice volume fraction of the mixed-phase cloud. For mixed-phase clouds containing small ice crystals (D_m^I ≤ 27 μm) and high ice volume fractions (f_i > 0.5) crystal shape is crucial. The largest shape effects were observed assuming aggregates and columns. If the IWC was conserved the shape effect reaches values up to 0.23 in cloud reflectance and transmittance. If the ice mode NSD was kept constant only a small shape effect was quantified (≤ 0.04).     

Examining the aerosol indirect effect over China using an SO2 emission inventory

The relationship between SO₂ emissions and the effective particle radius of low-level water clouds (r_e) over China was investigated to determine anthropogenic effects on clouds. Sulfur dioxide emission values were obtained from a statistical inventory, and r_e origins were retrieved by satellite remote sensing on a 0.5° grid. Comparisons between annual mean SO₂ emissions and r_e showed generally decreasing r_e values, explained by the Twomey effect. The existence of the Twomey effect is supported by comparisons with simulated aerosol optical depths. Results further suggest that clouds over land show sensitivity to the Twomey effect as well as clouds over the ocean.     

Remote sensing of cloud liquid water

Summary A method is presented to infer cloud liquid water path (LWP in kg/m²) over the ocean from passive microwave measurements of SSM/I. The algorithm to retrieve LWP is based on simulated satellite observations. They are calculated with a radiative transfer model applied to about 3000 radiosonde ascents over the Atlantic Ocean. Since radiosonde observations do not contain direct information about cloud water and ice, these parameters are parameterized based on relative humidity and temperature using modified adiabatic liquid water density profiles. A multiple linear regression is applied to the simulated radiances and the calculated LWP to derive the algorithm. The retrieval accuracy based on the regression analysis including instrumental noise is 0.03 kg/m². Validation of the LWP-algorithm was pursued through a comparison with measurements of a ground-based 33 GHzmicrowave radiometer on board of R.V. Poseidon during the International Cirrus Experiment 1989 at the North Sea (ICE'89). The LWP values agree within the range of uncertainty caused by the different sampling characteristics of the observing systems. The retrieval accuracy for clear-sky cases determined using colocated METEOSAT data over the North Sea is 0.037 kg/m² and confirms the accuracy estimated from regression analysis for the low liquid water cases.The algorithm was used to derive maps of monthly mean LWP over the Atlantic Ocean. As an example the Octobers of the 5 years 1987–1991 were selected to demonstrate the interannual variability of LWP. The results were compared with the cloud water content produced by the climate model ECHAM-T2 from the Max-Planck-Institut Hamburg.Observations during ICE'89 were used to check the accuracy of the applied radiative transfer model. Brightness temperatures were calculated from radiosonde ascents launched during the overpass of DMSP-F8 in cloud-free situations. The channel-dependent differences range from about –2 to 3 K.The possibility to identify different cloud types using microwave and infrared observations was examined. The main conclusion is that simultaneous microwave and infrared measurements enable the separation of dense cirrus and cirrus with underlying water clouds. A classification of clouds with respect to their top heights and LWP was carried out using a combination of SSM/I derived LWP and simultaneously recorded Meteosat IR-data during ICE'89.With 11 Figures     

Correlations between microphysical properties of large-scale semi-transparent cirrus and the state of the atmosphere

By making use of TOVS Path-B satellite retrievals and ECMWF reanalyses, correlations between bulk microphysical properties of large-scale semi-transparent cirrus (visible optical thickness between 0.7 and 3.8) and thermodynamic and dynamic properties of the surrounding atmosphere have been studied on a global scale. These clouds constitute about half of all high clouds. The global averages (from 60°N to 60°S) of mean ice crystal diameter, D_e, and ice water path (IWP) of these clouds are 55 μm and 30 g m⁻², respectively. IWP of these cirrus is slightly increasing with cloud-top temperature, whereas D_e of cold cirrus does not depend on this parameter. Correlations between D_e and IWp of large-scale cirrus seem to be different in the midlatitudes and in the tropics. However, we observe in general stronger correlations between D_e and IWP and atmospheric humidity and winds deduced from the ECMWF reanalyses: D_e and IWP increase both with increasing atmospheric water vapour. There is also a good distinction between different dynamical situations: In humid situations, IWP is on average about 10 gm⁻² larger in regions with strong large-scale vertical updraft only that in regions with strong large-scale horizontal winds only, whereas the mean D_e of cold large-scale cirrus decreases by about 10 μm if both strong large-scale updraft and horizontal winds are present.