Gulf Of Mexico Atmospheric Composition And Climate Study Research Articles

Droplet inhomogeneity in shallow cumuli: the effects of in-cloud location and aerosol number concentration

Abstract. Aerosol–cloud interactions are complex, including albedo and lifetime effects that cause modifications to cloud characteristics. With most cloud–aerosol interactions focused on the previously stated phenomena, there have been no in situ studies that focus explicitly on how aerosols can affect large-scale (centimeters to tens of meters) droplet inhomogeneities within clouds. This research therefore aims to gain a better understanding of how droplet inhomogeneities within cumulus clouds can be influenced by in-cloud droplet location (cloud edge vs. center) and the surrounding environmental aerosol number concentration. The pair-correlation function (PCF) is used to identify the magnitude of droplet inhomogeneity from data collected on board the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft, flown during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS). Time stamps (at 10−4 m spatial resolution) of cloud droplet arrival times were measured by the Artium Flight phase-Doppler interferometer (PDI). Using four complete days of data with 81 non-precipitating cloud penetrations organized into two flights of low-pollution (L1, L2) and high-pollution (H1, H2) data shows enhanced inhomogeneities near cloud edge as compared to cloud center for all four cases. Low-pollution clouds are shown to have enhanced overall inhomogeneity, with flight L2 being solely responsible for this enhanced inhomogeneity. Analysis suggests cloud age plays a larger role in the amount of inhomogeneity experienced than the aerosol number concentration, with dissipating clouds showing increased inhomogeneities as compared to growing or mature clouds. Results using a single, vertically developed cumulus cloud demonstrate enhanced droplet inhomogeneity near cloud top as compared to cloud base.

Observational estimates of detrainment and entrainment in non-precipitating shallow cumulus

Abstract. Vertical transport associated with cumulus clouds is important to the redistribution of gases, particles, and energy, with subsequent consequences for many aspects of the climate system. Previous studies have suggested that detrainment from clouds can be comparable to the updraft mass flux, and thus represents an important contribution to vertical transport. In this study, we describe a new method to deduce the amounts of gross detrainment and entrainment experienced by non-precipitating cumulus clouds using aircraft observations. The method utilizes equations for three conserved variables: cloud mass, total water, and moist static energy. Optimizing these three equations leads to estimates of the mass fractions of adiabatic mixed-layer air, entrained air and detrained air that the sampled cloud has experienced. The method is applied to six flights of the CIRPAS Twin Otter during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) which took place in the Houston, Texas region during the summer of 2006 during which 176 small, non-precipitating cumuli were sampled. Using our novel method, we find that, on average, these clouds were comprised of 30 to 70 % mixed-layer air, with entrained air comprising most of the remainder. The mass fraction of detrained air was usually very small, less than 2 %, although values larger than 10 % were found in 15 % of clouds. Entrained and detrained air mass fractions both increased with altitude, consistent with some previous observational studies. The largest detrainment events were almost all associated with air that was at their level of neutral buoyancy, which has been hypothesized in previous modeling studies. This new method could be readily used with data from other previous aircraft campaigns to expand our understanding of detrainment for a variety of cloud systems.

Aerosol and gas re‐distribution by shallow cumulus clouds: An investigation using airborne measurements

Aircraft measurements during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) are used to examine the influence of shallow cumulus clouds on vertical profiles of aerosol chemical composition, size distributions, and secondary aerosol precursor gases. The data show signatures of convective transport of particles, gases and moisture from near the surface to higher altitudes, and of aqueous‐phase production of aerosol mass (sulfate and organics) in cloud droplets and aerosol water. In cloudy conditions, the average aerosol volume concentration at an altitude of 2850 m, above typical cloud top levels, was found to be 34% of that at 450 m; for clear conditions, the same ratio was 13%. Both organic and sulfate mass fractions were on average constant with altitude (around 50%); however, the ratio of oxalate to organic mass increased with altitude (from 1% at 450 m to almost 9% at 3450 m), indicative of the influence of in‐cloud production on the vertical abundance and characteristics of secondary organic aerosol (SOA) mass. A new metric termed “residual cloud fraction” is introduced as a way of quantifying the “cloud processing history” of an air parcel. Results of a parcel model simulating aqueous phase production of sulfate and organics reproduce observed trends and point at a potentially important role of SOA production, especially oligomers, in deliquesced aerosols. The observations emphasize the importance of shallow cumulus clouds in altering the vertical distribution of aerosol properties that influence both their direct and indirect effect on climate.

Performance of an Eddy Diffusivity–Mass Flux Scheme for Shallow Cumulus Boundary Layers

Abstract Comparisons between single-column (SCM) simulations with the total energy–mass flux boundary layer scheme (TEMF) and large-eddy simulations (LES) are shown for four cases from the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) 2006 field experiment in the vicinity of Houston, Texas. The SCM simulations were run with initial soundings and surface forcing identical to those in the LES, providing a clean comparison with the boundary layer scheme isolated from any other influences. Good agreement is found in the simulated vertical transport and resulting moisture profiles. Notable differences are seen in the cloud base and in the distribution of moisture between the lower and upper cloud layer. By the end of the simulations, TEMF has dried the subcloud layer and moistened the lower cloud layer more than LES. TEMF gives more realistic profiles for shallow cumulus conditions than traditional boundary layer schemes, which have no transport above the dry convective boundary layer. Changes to the formulation and its parameters from previous publications are discussed.

Overview of the Second Texas Air Quality Study (TexAQS II) and the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

The Second Texas Air Quality Study (TexAQS II) was conducted in eastern Texas during 2005 and 2006. This 2‐year study included an intensive field campaign, TexAQS 2006/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), conducted in August–October 2006. The results reported in this special journal section are based on observations collected on four aircraft, one research vessel, networks of ground‐based air quality and meteorological (surface and radar wind profiler) sites in eastern Texas, a balloon‐borne ozonesonde‐radiosonde network (part of Intercontinental Transport Experiment Ozonesonde Network Study (IONS‐06)), and satellites. This overview paper provides operational and logistical information for those platforms and sites, summarizes the principal findings and conclusions that have thus far been drawn from the results, and directs readers to appropriate papers for the full analysis. Two of these findings deserve particular emphasis. First, despite decreases in actual emissions of highly reactive volatile organic compounds (HRVOC) and some improvements in inventory estimates since the TexAQS 2000 study, the current Houston area emission inventories still underestimate HRVOC emissions by approximately 1 order of magnitude. Second, the background ozone in eastern Texas, which represents the minimum ozone concentration that is likely achievable through only local controls, can approach or exceed the current National Ambient Air Quality Standard of 75 ppbv for an 8‐h average. These findings have broad implications for air quality control strategies in eastern Texas.

Cloud condensation nuclei activity, closure, and droplet growth kinetics of Houston aerosol during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

In situ cloud condensation nuclei (CCN) measurements were obtained in the boundary layer over Houston, Texas, during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) campaign onboard the CIRPAS Twin Otter. Polluted air masses in and out of cloudy regions were sampled for a total of 22 flights, with CCN measurements obtained for 17 of these flights. In this paper, we focus on CCN closure during two flights, within and downwind of the Houston regional plume and over the Houston Ship Channel. During both flights, air was sampled with particle concentrations exceeding 25,000 cm−3 and CCN concentrations exceeding 10,000 cm−3. CCN closure is evaluated by comparing measured concentrations with those predicted on the basis of measured aerosol size distributions and aerosol mass spectrometer particle composition. Different assumptions concerning the internally mixed chemical composition result in average CCN overprediction ranging from 3% to 36% (based on a linear fit). It is hypothesized that the externally mixed fraction of the aerosol contributes much of the CCN closure scatter, while the internally mixed fraction largely controls the overprediction bias. On the basis of the droplet sizes of activated CCN, organics do not seem to impact, on average, the CCN activation kinetics.

Measurements of volatile organic compounds during the 2006 TexAQS/GoMACCS campaign: Industrial influences, regional characteristics, and diurnal dependencies of the OH reactivity

An extensive set of volatile organic compounds (VOCs) and other gas phase species were measured in situ aboard the NOAA R/V Ronald H. Brown as the ship sailed in the Gulf of Mexico and the Houston and Galveston Bay (HGB) area as part of the Texas Air Quality (TexAQS)/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) conducted from July–September 2006. The magnitudes of the reactivities of CH4, CO, VOCs, and NO2 with the hydroxyl radical, OH, were determined in order to quantify the contributions of these compounds to potential ozone formation. The average total OH reactivity (ROH,TOTAL) increased from 1.01 s−1 in the central gulf to 10.1 s−1 in the HGB area as a result of the substantial increase in the contribution from VOCs and NO2. The increase in the measured concentrations of reactive VOCs in the HGB area compared to the central gulf was explained by the impact of industrial emissions, the regional distribution of VOCs, and the effects of local meteorology. By compensating for the effects of boundary layer mixing, the diurnal profiles of the OH reactivity were used to characterize the source signatures and relative magnitudes of biogenic, anthropogenic (urban + industrial), and oxygenated VOCs as a function of the time of day. The source of reactive oxygenated VOCs (e.g., formaldehyde) was determined to be almost entirely from secondary production. The secondary formation of oxygenated VOCs, in addition to the continued emissions of reactive anthropogenic VOCs, served to sustain elevated levels of OH reactivity throughout the time of peak ozone production.

Aerosol‐cloud relationships in continental shallow cumulus

Aerosol‐cloud relationships are derived from 14 warm continental cumuli cases sampled during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) by the Center for Interdisciplinary Remotely‐Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. Cloud droplet number concentration is clearly proportional to the subcloud accumulation mode aerosol number concentration. An inverse correlation between cloud top effective radius and subcloud aerosol number concentration is observed when cloud depth variations are accounted for. There are no discernable aerosol effects on cloud droplet spectral dispersion; the averaged spectral relative dispersion is 0.30 ± 0.04. Aerosol‐cloud relationships are also identified from comparison of two isolated cloud cases that occurred under different degrees of anthropogenic influence. Cloud liquid water content, cloud droplet number concentration, and cloud top effective radius exhibit subadiabaticity resulting from entrainment mixing processes. The degree of LWC subadiabaticity is found to increase with cloud depth. Impacts of subadiabaticity on cloud optical properties are assessed. It is estimated that owing to entrainment mixing, cloud LWP, effective radius, and cloud albedo are decreased by 50–85%, 5–35%, and 2–26%, respectively, relative to adiabatic values of a plane‐parallel cloud. The impact of subadiabaticity on cloud albedo is largest for shallow clouds. Results suggest that the effect of entrainment mixing must be accounted for when evaluating the aerosol indirect effect.

Statistical comparison of properties of simulated and observed cumulus clouds in the vicinity of Houston during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

We present statistical comparisons of properties of clouds generated by Large Eddy Simulations (LES) with aircraft observations of nonprecipitating, warm cumulus clouds made in the vicinity of Houston, TX during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), carried out in the summer of 2006. Aircraft data were sampled with the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter airplane. Five flights (days) that are most suitable for studying aerosol‐cloud interactions are selected from the 22 flights. The model simulations are initiated with observed environmental profiles. The simulations are used to generate an ensemble of thousands of cumulus clouds for statistically meaningful evaluations. Statistical comparisons focus on the properties of a set of dynamical and thermodynamical variables, sampled either in the cloud or the cloud updraft core. The set of variables includes cloud liquid water content (LWC), number mixing ratio of cloud droplets (Nd), cloud effective radius (re), updraft velocity (w), and the distribution of cloud sizes. In general, good agreement between the simulated and observed clouds is achieved in the normalized frequency distribution functions, the profiles averaged over the cloudy regions, the cross‐cloud averages, and the cloud size distributions, despite big differences in sample size between the model output and the aircraft data. Some unresolved differences in frequency distributions of w and possible differences in cloud fraction are noted. These comparisons suggest that the LES is able to successfully generate the cumulus cloud populations that were present during GoMACCS. The extent to which this is true will depend on the specific application.

Particulate organic acids and overall water‐soluble aerosol composition measurements from the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

The Center for Interdisciplinary Remotely‐Piloted Aircraft Studies (CIRPAS) Twin Otter participated in the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) mission during August–September 2006. A particle‐into‐liquid sampler (PILS) coupled to ion chromatography was used to characterize the water‐soluble ion composition of aerosol and cloud droplet residual particles (976 5‐min PM1.0samples in total). Sulfate and ammonium dominated the water‐soluble mass (NH4++ SO42−= 84 ± 14%), while organic acids contributed 3.4 ± 3.7%. The average NH4+:SO42−molar ratio was 1.77 ± 0.85. Particulate concentrations of organic acids increased with decreasing carbon number from C9to C2. Organic acids were most abundant above cloud, presumably as a result of aqueous phase chemistry in cloud droplets, followed by subsequent droplet evaporation above cloud tops; the main product of this chemistry was oxalic acid. The evolution of organic acids with increasing altitude in cloud provides evidence for the multistep nature of oxalic acid production; predictions from a cloud parcel model are consistent with the observed oxalate:glyoxylate ratio as a function of altitude in GoMACCS cumuli. Suppressed organic acid formation was observed in clouds with relatively acidic droplets, as determined by high particulate nitrate concentrations (presumably high HNO3levels too) and lower liquid water content, as compared to other cloud fields probed. In the Houston Ship Channel region, an area with significant volatile organic compound emissions, oxalate, acetate, formate, benzoate, and pyruvate, in decreasing order, were the most abundant organic acids. Photo‐oxidation ofm‐xylene in laboratory chamber experiments leads to a particulate organic acid product distribution consistent with the Ship Channel area observations.

On the Source of Organic Acid Aerosol Layers above Clouds

During the July 2005 Marine Stratus/Stratocumulus Experiment (MASE) and the August-September 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed aerosols and cumulus clouds in the eastern Pacific Ocean off the coast of northern California and in southeastern Texas, respectively. An on-board particle-into-liquid sampler (PILS) quantified inorganic and organic acid species with < or = 5-min time resolution. Ubiquitous organic aerosol layers above cloud with enhanced organic acid levels were observed in both locations. The data suggest that aqueous-phase reactions to produce organic acids, mainly oxalic acid, followed by droplet evaporation is a source of elevated organic acid aerosol levels above cloud. Oxalic acid is observed to be produced more efficiently relative to sulfate as the cloud liquid water content increases, corresponding to larger and less acidic droplets. As derived from large eddy simulations of stratocumulus underthe conditions of MASE, both Lagrangian trajectory analysis and diurnal cloudtop evolution provide evidence that a significant fraction of the aerosol mass concentration above cloud can be accounted for by evaporated droplet residual particles. Methanesulfonate data suggest that entrainment of free tropospheric aerosol can also be a source of organic acids above boundary layer clouds.