Continental Clouds Research Articles

Secondary Seeding as a Means of Propagating Seeding Effects in Space and Time

Secondary seeding, whereby unseeded clouds ingest ice particles from clouds that earlier had received direct glaciogenic (e.g., silver iodide) treatment, is hypothesized to be a possible additional mechanism for the propagation of seeding effects in space and for time. The ingested ice particles, after experiencing some growth in the donor cloud, act to glaciate the receptor cloud during its active growth phase and provide it precipitation embryos. These embryos give the new cloud a head-start on precipitation development as they grow further as graupel to precipitation size in the updraft laden with high quantities of supercooled cloud water. This enhancement of precipitation-forming processes is postulated to be strongest in microphysically continental clouds in which natural and seeding-induced primary glaciation and hydrometeor growth are slow. A case study is presented to illustrate these processes.

Aerosol microphysical and radiative effects on continental cloud ensembles

Aerosol–cloud–radiation interactions represent one of the largest uncertainties in the current climate assessment. Much of the complexity arises from the non-monotonic responses of clouds, precipitation and radiative fluxes to aerosol perturbations under various meteorological conditions. In this study, an aerosol-aware WRF model is used to investigate the microphysical and radiative effects of aerosols in three weather systems during the March 2000 Cloud Intensive Observational Period campaign at the US Southern Great Plains. Three simulated cloud ensembles include a low-pressure deep convective cloud system, a collection of less-precipitating stratus and shallow cumulus, and a cold frontal passage. The WRF simulations are evaluated by several ground-based measurements. The microphysical properties of cloud hydrometeors, such as their mass and number concentrations, generally show monotonic trends as a function of cloud condensation nuclei concentrations. Aerosol radiative effects do not influence the trends of cloud microphysics, except for the stratus and shallow cumulus cases where aerosol semi-direct effects are identified. The precipitation changes by aerosols vary with the cloud types and their evolving stages, with a prominent aerosol invigoration effect and associated enhanced precipitation from the convective sources. The simulated aerosol direct effect suppresses precipitation in all three cases but does not overturn the aerosol indirect effect. Cloud fraction exhibits much smaller sensitivity (typically less than 2%) to aerosol perturbations, and the responses vary with aerosol concentrations and cloud regimes. The surface shortwave radiation shows a monotonic decrease by increasing aerosols, while the magnitude of the decrease depends on the cloud type.

Aerosol properties and their impacts on surface CCN at the ARM Southern Great Plains site during the 2011 Midlatitude Continental Convective Clouds Experiment

Aerosol particles are of particular importance because of their impacts on cloud development and precipitation processes over land and ocean. Aerosol properties as well as meteorological observations from the Department of Energy Atmospheric Radiation Measurement (ARM) platform situated in the Southern Great Plains (SGP) are utilized in this study to illustrate the dependence of continental cloud condensation nuclei (CCN) number concentration (NCCN) on aerosol type and transport pathways. ARM-SGP observations from the 2011 Midlatitude Continental Convective Clouds Experiment field campaign are presented in this study and compared with our previous work during the 2009–10 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer field campaign over the current ARM Eastern North Atlantic site. Northerly winds over the SGP reflect clean, continental conditions with aerosol scattering coefficient (σsp) values less than 20 Mm−1 and NCCN values less than 100 cm−3. However, southerly winds over the SGP are responsible for the observed moderate to high correlation (R) among aerosol loading (σsp < 60 Mm−1) and NCCN, carbonaceous chemical species (biomass burning smoke), and precipitable water vapor. This suggests a common transport mechanism for smoke aerosols and moisture via the Gulf of Mexico, indicating a strong dependence on air mass type. NASA MERRA-2 reanalysis aerosol and chemical data are moderately to highly correlated with surface ARM-SGP data, suggesting that this facility can represent surface aerosol conditions in the SGP, especially during strong aerosol loading events that transport via the Gulf of Mexico. Future long-term investigations will help to understand the seasonal influences of air masses on aerosol, CCN, and cloud properties over land in comparison to over ocean.

Microphysical characteristics of convective clouds over ocean and land from aircraft observations

The Cloud Aerosol Interaction and Precipitation Enhancement EXperiment (CAIPEEX) is a field campaign conducted in India with an instrumented research aircraft. On 29 October 2010, a cyclonic circulation over the Bay of Bengal persisted throughout the day. A special mission was conducted over the Bay of Bengal on this day with the objective of characterizing marine and continental clouds on the same day and finding contrasting/similar signatures of their microphysical properties. The research aircraft sampled growing convective clouds over the ocean and over land. High concentrations of aerosol and cloud condensation nuclei (CCN) were observed over land compared to ocean. Over ocean, higher liquid water content (LWC) and lower cloud droplet number concentrations (Nc) were observed, and droplets reached the threshold of precipitation initiation at lower cloud depths. Over land, clouds contained lower LWC and higher Nc, hence droplets did not reach the threshold of precipitation initiation at a warm temperature as in ocean clouds. Over the ocean larger droplets or drizzle were observed at lower cloud depth than over land. The maximum LWC was found to be very similar at higher altitudes. The convective clouds over land were modified by pollution aerosol with contrasting microphysical properties to those over the ocean.

Distinct Impacts of Aerosols on an Evolving Continental Cloud Complex during the RACORO Field Campaign

Abstract A continental cloud complex, consisting of shallow cumuli, a deep convective cloud (DCC), and stratus, is simulated by a cloud-resolving Weather Research and Forecasting Model to investigate the aerosol microphysical effect (AME) and aerosol radiative effect (ARE) on the various cloud regimes and their transitions during the Department of Energy Routine Atmospheric Radiation Measurement Aerial Facility Clouds with Low Optical Water Depths Optical Radiative Observations (RACORO) campaign. Under an elevated aerosol loading with AME only, a reduced cloudiness for the shallow cumuli and stratus resulted from more droplet evaporation competing with suppressed precipitation, but an enhanced cloudiness for the DCC is attributed to more condensation. With the inclusion of ARE, the shallow cumuli are suppressed owing to the thermodynamic effects of light-absorbing aerosols. The responses of DCC and stratus to aerosols are monotonic with AME only but nonmonotonic with both AME and ARE. The DCC is invigorated because of favorable convection and moisture conditions at night induced by daytime ARE, via the so-called aerosol-enhanced conditional instability mechanism. The results reveal that the overall aerosol effects on the cloud complex are distinct from the individual cloud types, highlighting that the aerosol–cloud interactions for diverse cloud regimes and their transitions need to be evaluated to assess the regional and global climatic impacts.

Tryptophan and tryptophan-like substances in cloud water: Occurrence and photochemical fate

This work investigates the occurrence and photochemical behaviour of tryptophan (TRP) in the cloud aqueous phase. The concentrations of tryptophan, TRYptophan LIke Substances (TRYLIS) and HUmic LIke Substances (HULIS) in real cloud water, collected between October 2013 and November 2014 at the top of the puy de Dôme station, were determined using the Excitation-Emission-Matrix (EEM) technique. The amount of free and complexed tryptophan (TRP) up to 10−7 M in cloud aqueous phase was quantified by HPLC-UV-fluorescence analysis, and its photoreactivity under sun-simulated conditions was investigated in synthetic water samples mimicking cloud aqueous phase compositions (oceanic and continental origins). TRP undergoes direct photolysis, and its degradation is enhanced in the presence of naturally occurring species able to photo-generate hydroxyl radicals (HO). The polychromatic quantum yield of TRP (ϕ290−340nmTRP) is estimated to be 8.37 × 10−4 between 290 and 340 nm, corresponding to the degradation rate (RTRPd) of 1.29 × 10−11 M s−1 under our irradiation conditions. The degradation is accelerated up to 3.65 × 10−10 and 8.26 × 10−10 M s−1 in synthetic oceanic and continental cloud water samples doped with 100 μM hydrogen peroxide, respectively.Hydroxyl radical-mediated transformation leads to the generation of different functionalized and oxidized products, as well as small carboxylic acids, such as formate and acetate. Moreover, fluorescent signals of irradiated solutions indicate the formation of HULIS.

Comparação das Propriedades Microfísicas de Diferentes Tipos de Nuvens em Duas Regiões Tropicais com Ecossistemas Distintos Usando Dados do Satélite CloudSat

The approach used in this work’s methodology looks to represent the average microphysical structure of different types of clouds formed in two different ecosystems. The selected regions were located in the Midwest of Brazil (coordinates: 12-18 ° S and 46-58 ° W) and the South Atlantic Ocean (coordinates: 12-25 ° S and 9-30 ° W). In order to accomplish the proposed goal, data from CloudSat satellite from a period of approximately five years are used (from June 2006 to April 2011). The results show that there is little variation in microphysical structure between continental and maritime clouds in the studied regions. The mean droplet (ice particle) effective radius obtained in all the cloud types analyzed was 12.4 μm (71.9 μm) for maritime clouds and 11.0 μm (72.9 μm) for continental clouds. Particle size distribution (concentration as a function of size) was the most efficient parameter to distinguish cloud types, making it possible to identify particularities of each type. The results showed that even in the period with the highest concentration of aerosols observed in the Central-West region of Brazil (spring), there is a significant difference in the cloud particle size distribution in the regions studied. These results indicate that other external agents (besides the total concentration of aerosol integrated in the atmospheric column) are acting more significantly to modulate the particles distribution within the clouds in the Central-W est region.

Precipitation microstructure in different Madden–Julian Oscillation phases over Sumatra

Intraseasonal variations of precipitation and its microstructure are investigated using measurements of the Equatorial Atmospheric Radar (EAR) facilities at Kototabang, west Sumatra, Indonesia (0.20°S, 100.32°E, 864m above sea level). Raindrop size distribution (DSD) observations are obtained from a 2D-Video Disdrometer (2DVD) with a near continuous record of operation over eight consecutive years (2003–2010). Precipitation types are classified using 1.3-GHz wind profiler observation, and are partitioned according to active and inactive convective phases of Madden–Julian Oscillation (MJO). It is found that precipitation systems during the inactive phase are more continental in nature than those during the active phase. Cloud propagation from brightness temperature data indicates that Sumatra receives the rainfall mainly from maritime clouds during the active phase, while it is mainly from the continental clouds (land-based convection) during the inactive phase. Other remarkable differences between active and inactive phase precipitation systems are also observed from the vertical structure of precipitation. The precipitation during the inactive phase has deeper storms, a higher reflectivity aloft, more lightning activity and less stratiform characteristics, as compared to the active phase. Assessment of cloud effective radius of the Moderate Resolution Imaging Spectroradiometer (MODIS) data also shows a slight difference in the cloud droplet between the active and the inactive MJO phases. Different convective storms in different MJO phases lead to different DSD characteristics and Z–R relationships. The DSD during the inactive phase tends to have a higher concentration of medium and large-size drops than the active counterpart, consistent with the previous study during the first campaign of Coupling Processes in the Equatorial Atmosphere project. Although the DSD parameters and coefficient of Z–R relationships fall within the range of tropical maritime precipitation, mass-weighted mean diameter (Dm) for the deep convective rains during the inactive phase are somewhat larger than that for maritime and closer to the continental cluster. Therefore, continental-like DSDs are somewhat dominant during the inactive phase, consistent with the intraseasonal variation of precipitation structure. The causative processes of the observed difference in the DSD for the two phases have also been discussed with the help of satellite and radar data. Evaporation and updraft associated with the intense convection during the inactive phase seem to eliminate the small-sized drops from the spectra. Finally, radar reflectivity during the inactive phase is larger than that during the active MJO phase, at the same rainfall rate. This condition can limit the accuracy of radar-derived rainfall estimates for the tropics when applying a single Z–R relation to the two MJO phases, particularly for deep convective rains.

High-resolution measurement of cloud microphysics and turbulence at a mountaintop station

Abstract. Mountain research stations are advantageous not only for long-term sampling of cloud properties but also for measurements that are prohibitively difficult to perform on airborne platforms due to the large true air speed or adverse factors such as weight and complexity of the equipment necessary. Some cloud–turbulence measurements, especially Lagrangian in nature, fall into this category. We report results from simultaneous, high-resolution and collocated measurements of cloud microphysical and turbulence properties during several warm cloud events at the Umweltforschungsstation Schneefernerhaus (UFS) on Zugspitze in the German Alps. The data gathered were found to be representative of observations made with similar instrumentation in free clouds. The observed turbulence shared all features known for high-Reynolds-number flows: it exhibited approximately Gaussian fluctuations for all three velocity components, a clearly defined inertial subrange following Kolmogorov scaling (power spectrum, and second- and third-order Eulerian structure functions), and highly intermittent velocity gradients, as well as approximately lognormal kinetic energy dissipation rates. The clouds were observed to have liquid water contents on the order of 1 g m−3 and size distributions typical of continental clouds, sometimes exhibiting long positive tails indicative of large drop production through turbulent mixing or coalescence growth. Dimensionless parameters relevant to cloud–turbulence interactions, the Stokes number and settling parameter are in the range typically observed in atmospheric clouds. Observed fluctuations in droplet number concentration and diameter suggest a preference for inhomogeneous mixing. Finally, enhanced variance in liquid water content fluctuations is observed at high frequencies, and the scale break occurs at a value consistent with the independently estimated phase relaxation time from microphysical measurements.

Frequency of occurrence of rain from liquid‐, mixed‐, and ice‐phase clouds derived from A‐Train satellite retrievals

AbstractA climatology of thermodynamic phase of precipitating cloud is presented derived from global—land and ocean—, retrievals from Cloudsat, CALIPSO, and Moderate Resolution Imaging Spectroradiometer. Like precipitation rate, precipitation frequency is dominated by warm rain, defined as rain produced via the liquid phase only, over the tropical oceans outside the Intertropical Convergence Zone and by cold rain, produced via the ice phase, over the midlatitude oceans and continents. Warm rain is very infrequent over the continents, with significant warm rain found only in onshore flow in the tropics, and over India, China, and Indochina. Comparison of the properties of precipitating and nonprecipitating warm clouds shows that the scarcity of warm rain over land can be explained by smaller effective radii in continental clouds that delay the onset of precipitation. The results highlight the importance of ice‐phase processes for the global hydrological cycle and may lead to an improved parameterization of precipitation in general circulation models.

Study of longwave radiative transfer in stratocumulus clouds by using bin optical properties and bin microphysics scheme

Infrared radiative cooling at the cloud top is the major driving force for stratocumulus-topped boundary layer turbulence and the major source of buoyancy within a convective mixed layer. However, there is still large uncertainty about the rate of longwave cooling at the cloud top in recent numerical models. Radiative transfer calculations within stratocumulus clouds can be further improved by using bin scheme in the calculation of longwave extinction coefficients.A method to calculate bin optical properties was developed and was implemented in the RRTM LW radiative transfer model. This bin-type radiation scheme allows us more accurate calculation of the optical properties of clouds, because it does not need any arbitrary assumption for the size distribution of the hydrometeors. The number concentrations and mixing ratios in 36 size-bins provided by bin microphysical scheme are used for calculation of the extinction coefficient. In this paper results of this new scheme were compared to that of one-moment and two-moment bulk radiation schemes where the size distributions were supposed to follow a gamma-function. It was found that the application of the two-moment bulk scheme had no advantage against the one-moment bulk scheme in simulation of radiation profiles, if radiation feedback on cloud processes was not taken into account. Although the gamma function used by bulk schemes fitted relatively well to the size distribution of the water drops calculated by the bin scheme, the longwave radiation fluxes calculated by the two schemes (bulk vs. bin) were significantly different. The bin radiation scheme gave at least 50% larger warming rates both at the cloud base and at the cloud top than the bulk schemes did. The cooling/warming occurred in a thinner vertical layer in the case of the bin scheme than in the case of bulk schemes. The shape of the net radiation profile strongly depended on the CCN concentration. Continental clouds were found to have horizontally less varying value and vertically thinner region of cloud top cooling than maritime clouds.Compared with the observations the bulk radiation schemes failed to simulate the cloud base warming, while the bin radiation scheme reproduced well the observed cloud base warming. Considering the cloud top cooling the bin scheme overestimated the observed values, but agreed well with the results of other detailed radiation models. This difference might be explained by uncertainties about the vertical extent of the layer where divergence of the net radiation profile was large.

Satellite‐based climatology of low‐level continental clouds in southern West Africa during the summer monsoon season

AbstractSynoptic observations and various satellite products have been utilized for computing climatologies of low‐level stratus over southern West Africa for the wet monsoon seasons July–September of 2006–2011. Previous studies found inconsistencies between satellite cloud products; climate models often fail to reproduce the extensive stratus decks. Therefore, a better observational reference and an understanding of its limitations are urgently needed to better validate models. Most detailed information of the spatiotemporal characteristics of low‐level clouds was obtained from two Meteosat Second Generation (MSG) satellite‐based data sets. However, CALIPSO and CloudSat cross sections of cloud occurrence frequency suggest that both MSG products underestimate the low‐level cloudiness over Nigeria due to shielding by abundant upper level and midlevel clouds and reveal that the stratus is lower over the continent than over the ocean. The Terra Multiangle Imaging Spectroradiometer product appears to overestimate the morning extent of low‐level clouds. The climatology presented here shows that the zone of abundant low‐level stratiform clouds is at its diurnal minimum south of 6–7°N around sunset (~1800 UTC). Thereafter, it starts to spread inland and reaches its maximum northward extent of 10–11°N between 0900 and 1000 UTC. The maximum affected area is approximately 800,000 km2. After about 1000 UTC, the northern boundary gets fragmented due to the breakup of stratus decks into fair‐weather cumuli. The stratus is most frequent around Cape Palmas, over Ivory Coast, and at the windward sides of the Mampong Range (Ghana) and Oshogbo Hills (Nigeria).

Simulations of Stratus Clouds over Eastern China in CAM5: Sensitivity to Horizontal Resolution

Abstract This paper evaluates the simulations of stratus clouds over eastern China (EC) in the Community Atmosphere Model, version 5 (CAM5), with an emphasis on the impact of changing horizontal resolutions on the performance. CAM5 in all experiments generally satisfactorily simulates the cloud radiative features over EC, including the spatial distributions of the continental shortwave cloud radiative forcing (SWCF) and stratus regimes, the responses of SWCF to the dynamic and thermodynamic ambient environment, and several relations in the environmental fields that are favorable to the stratus formation. Meanwhile, all experiments suffer from similar biases. Models tend to underestimate the stratus amount because of a corresponding underestimate of stratus occurrence frequency, while the stratus amount when present (AWP) is generally higher than that in the observation. Models also simulate similar errors in the environmental fields. The differences between low- and high-resolution experiments are distinct. An increase of resolution enhances the SWCF in southern China, but the skill deteriorates in the Sichuan basin. Correspondingly, the stratus amount increases in southern China from low- to high-resolution experiments, mainly because of more stratus occurrences, which are found to be related to the better represented environmental fields in the high-resolution experiments, especially the dynamic component. Several relations in the ambient environment are also slightly improved in the high-resolution experiments. Meanwhile, the reason for the decrease of stratus AWP within the Sichuan basin, which is mainly responsible for the decreased stratus amounts and weaker SWCF from low- to high-resolution experiments, is also discussed.

The interdependence of continental warm cloud properties derived from unexploited solar background signals in ground-based lidar measurements

Abstract. We have extensively analysed the interdependence between cloud optical depth, droplet effective radius, liquid water path (LWP) and geometric thickness for stratiform warm clouds using ground-based observations. In particular, this analysis uses cloud optical depths retrieved from untapped solar background signals that are previously unwanted and need to be removed in most lidar applications. Combining these new optical depth retrievals with radar and microwave observations at the Atmospheric Radiation Measurement (ARM) Climate Research Facility in Oklahoma during 2005–2007, we have found that LWP and geometric thickness increase and follow a power-law relationship with cloud optical depth regardless of the presence of drizzle; LWP and geometric thickness in drizzling clouds can be generally 20–40% and at least 10% higher than those in non-drizzling clouds, respectively. In contrast, droplet effective radius shows a negative correlation with optical depth in drizzling clouds and a positive correlation in non-drizzling clouds, where, for large optical depths, it asymptotes to 10 μm. This asymptotic behaviour in non-drizzling clouds is found in both the droplet effective radius and optical depth, making it possible to use simple thresholds of optical depth, droplet size, or a combination of these two variables for drizzle delineation. This paper demonstrates a new way to enhance ground-based cloud observations and drizzle delineations using existing lidar networks.

에어로솔의 대륙 층운형 구름 연직발달(Invigoration)에 미치는 영향 분석

This study examines the effect of aerosols on the vertical invigoration of continental stratiform clouds, using a dataset of Atmospheric Radiation Measurement (ARM) Intensive Operational Period (IOP, March 2000) at the Southern Great Plains (SGP) site. To provide further support to our observation-based findings, the weather research and forecasting (WRF) sensitivity simulations with changing cloud condensation nuclei (CCN) concentrations have been carried out for the golden episode over SGP. First, cross correlation between observed aerosol scattering coefficient and cloud liquid water path (LWP) with a 160-minutes lag is the highest of r = 0.83 for the selected episode, which may be attributable to cloud vertical invigoration induced by an increase in aerosol loading. Modeled cloud fractions in a control run are well matched with the observation in the perspective of cloud morphology and lasting period. It is also found through a simple sensitivity with a change in CCN that aerosol invigoration (AIV) effect on stratiform cloud organization is attributable to a change in the cloud microphysics as well as dynamics such as the corresponding modification of cloud number concentrations, drop size, and latent heating rate, etc. This study suggests a possible cloud vertical invigoration even in the continental stratiform clouds due to aerosol enhancement in spite of a limited analysis based on a few observed continental cloud cases.

How well do climate models simulate cloud vertical structure? A comparison between CALIPSO‐GOCCP satellite observations and CMIP5 models

The Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite provides robust and global direct measurements of the cloud vertical structure. The GCM‐Oriented CALIPSO Cloud Product is used to evaluate the simulated clouds in five climate models using a lidar simulator. The total cloud cover is underestimated in all models (51% to 62% vs. 64% in observations) except in the Arctic. Continental cloud covers (at low, mid, high altitudes) are highly variable depending on the model. In the tropics, the top of deep convective clouds varies between 14 and 18 km in the models versus 16 km in the observations, and all models underestimate the low cloud amount (16% to 25%) compared to observations (29%). In the Arctic, the modeled low cloud amounts (37% to 57%) are slightly biased compared to observations (44%), and the models do not reproduce the observed seasonal variation.

High lightning activity in maritime clouds near Mexico

Abstract. Lightning activity detected by the World Wide Lightning Location Network (WWLLN) over oceanic regions adjacent to Mexico is often as high as that observed over the continent. In order to explore the possible causes of the observed high flash density over those regions, the relationships between lightning, rainfall, vertical hydrometeor profiles, latent heating, wind variability and aerosol optical depth are analyzed. The characteristics of lightning and precipitation over four oceanic zones adjacent to Mexican coastlines are contrasted against those over the continent. The number of flashes per rainfall over some coastal maritime regions is found to be higher than over the continent. The largest number of flashes per rainfall is observed during the biomass burning season. In addition, we compare two smaller areas of the Tropical Pacific Ocean: one located within the Inter-Tropical Convergence Zone and characterized by high rainfall and weak lightning activity and the other one influenced by a continental wind jet and characterized by high rainfall and strong lightning activity. During the rainy season, the monthly distribution of lightning within the region influenced by the continental wind jet is contrary to that of rainfall. Moreover, the monthly variability of lightning is very similar to the variability of the meridional wind component and it is also related to the variability of aerosol optical depth. The analysis suggests that the high lightning activity observed over coastal Pacific region is linked to the continental cloud condensation nuclei advected over the ocean. Analysis of daily observations indicates that the greatest lightning density is observed for moderate values of the aerosol optical depth, between 0.2 and 0.35.

Development and testing of the Active Temperature, Ozone and Moisture Microwave Spectrometer (ATOMMS) cm and mm wavelength occultation instrument

Abstract. We present initial results from testing a new remote sensing system called the Active Temperature, Ozone and Moisture Microwave Spectrometer (ATOMMS). ATOMMS is designed as a satellite-to-satellite occultation system for monitoring climate. We are developing the prototype instrument for an aircraft to aircraft occultation demonstration. Here we focus on field testing of the ATOMMS instrument, in particular the remote sensing of water by measuring the attenuation caused by the 22 GHz and 183 GHz water absorption lines. Our measurements of the 183 GHz line spectrum along an 820 m path revealed that the AM 6.2 spectroscopic model provdes a much better match to the observed spectrum than the MPM93 model. These comparisons also indicate that errors in the ATOMMS amplitude measurements are about 0.3%. Pressure sensitivity bodes well for ATOMMS as a climate instrument. Comparisons with a hygrometer revealed consistency at the 0.05 mb level, which is about 1% of the absolute humidity. Initial measurements of absorption by the 22 GHz line made along a 5.4 km path between two mountaintops captured a large increase in water vapor similar to that measured by several nearby hygrometers. A storm passage between the two instruments yielded our first measurements of extinction by rain and cloud droplets. Comparisons of ATOMMS 1.5 mm opacity measurements with measured visible opacity and backscatter from a weather radar revealed features simultaneously evident in all three datasets confirming the ATOMMS measurements. The combined ATOMMS, radar and visible information revealed the evolution of rain and cloud amounts along the signal path during the passage of the storm. The derived average cloud water content reached typical continental cloud amounts. These results demonstrated a significant portion of the information content of ATOMMS and its ability to penetrate through clouds and rain which is critical to its all-weather, climate monitoring capability.

Atmospheric chemistry of carboxylic acids: microbial implication versus photochemistry

Abstract. The objective of this work was to compare experimentally the contribution of photochemistry vs. microbial activity to the degradation of carboxylic acids present in cloud water. For this, we selected 17 strains representative of the microflora existing in real clouds and worked on two distinct artificial cloud media that reproduce marine and continental cloud chemical composition. Photodegradation experiments with hydrogen peroxide (H2O2) as a source of hydroxyl radicals were performed under the same microcosm conditions using two irradiation systems. Biodegradation and photodegradation rates of acetate, formate, oxalate and succinate were measured on both media at 5 °C and 17 °C and were shown to be on the same order of magnitude (around 10−10–10−11 M s−1). The chemical composition (marine or continental origin) had little influence on photodegradation and biodegradation rates while the temperature shift from 17 °C to 5 °C decreased biodegradation rates of a factor 2 to 5. In order to test other photochemical scenarios, theoretical photodegradation rates were calculated considering hydroxyl (OH) radical concentration values in cloud water estimated by cloud chemistry modelling studies and available reaction rate constants of carboxylic compounds with both hydroxyl and nitrate radicals. Considering high OH concentration ([OH] = 1 × 10−12 M) led to no significant contribution of microbial activity in the destruction of carboxylic acids. On the contrary, for lower OH concentration (at noon, [OH] = 1 × 10−14 M), microorganisms could efficiently compete with photochemistry and in similar contributions than the ones estimated by our experimental approach. Combining these two approaches (experimental and theoretical), our results led to the following conclusions: oxalate was only photodegraded; the photodegradation of formate was usually more efficient than its biodegradation; the biodegradation of acetate and succinate seemed to exceed their photodegradation.

The response of precipitation to aerosol through riming and melting in deep convective clouds

Abstract. We have used a 2-D axisymmetric, non-hydrostatic, bin-resolved cloud model to examine the impact of aerosol changes on the development of mixed-phase convective clouds. We have simulated convective clouds from four different sites (three continental and one tropical marine) with a wide range of realistic aerosol loadings and initial thermodynamic conditions (a total of 93 different clouds). It is found that the accumulated precipitation responds very differently to changing aerosol in the marine and continental environments. For the continental clouds, the scaled total precipitation reaches a maximum for aerosol that produce drop numbers at cloud base between 180–430 cm−3 when other conditions are the same. In contrast, all the tropical marine clouds show an increase in accumulated precipitation and deeper convection with increasing aerosol loading. For continental clouds, drops are rapidly depleted by ice particles shortly after the onset of precipitation. The precipitation is dominantly produced by melting ice particles. The riming rate increases with aerosol when the loading is very low, and decreases when the loading is high. Peak precipitation intensities tend to increase with aerosol up to drop concentrations (at cloud base) of ~500 cm−3 then decrease with further aerosol increases. This behaviour is caused by the initial transition from warm to mixed-phase rain followed by reduced efficiency of mixed-phase rain at very high drop concentrations. The response of tropical marine clouds to increasing aerosol is different to, and larger than, that of continental clouds. In the more humid tropical marine environment with low cloud bases we find that accumulated precipitation increases with increasing aerosol. The increase is driven by the transition from warm to mixed-phase rain. Our study suggests that the response of deep convective clouds to aerosol will be an important contribution to the spatial and temporal variability in cloud microphysics and precipitation.