VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment Research Articles

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

Turbulent and boundary layer characteristics during VOCALS-REx

Abstract. Boundary layer and turbulent characteristics (surface fluxes, turbulent kinetic energy – TKE, turbulent kinetic energy dissipation rate – ϵ), along with synoptic-scale changes in these properties over time, are examined using data collected from 18 research flights made with the CIRPAS Twin Otter Aircraft. Data were collected during the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study Regional Experiment (VOCALS-REx) at Point Alpha (20∘ S, 72∘ W) in October and November 2008 off the coast of South America. The average boundary layer depth is found to be 1148 m, with 28 % of the boundary layer profiles analyzed displaying decoupling. Analysis of correlation coefficients indicates that as atmospheric pressure decreases, the boundary layer height (zi) increases. As has been shown previously, the increase in zi is accompanied by a decrease in turbulence within the boundary layer. As zi increases, cooling near cloud top cannot sustain mixing over the entire depth of the boundary layer, resulting in less turbulence and boundary layer decoupling. As the latent heat flux (LHF) and sensible heat flux (SHF) increase, zi increases, along with the cloud thickness decreasing with increasing LHF. This suggests that an enhanced LHF results in enhanced entrainment, which acts to thin the cloud layer while deepening the boundary layer. A maximum in TKE on 1 November (both overall average and largest single value measured) is due to sub-cloud precipitation acting to destabilize the sub-cloud layer while acting to stabilize the cloud layer (through evaporation occurring away from the surface, primarily confined between a normalized boundary layer height, z/zi, of 0.40 to 0.60). Enhanced moisture above cloud top from a passing synoptic system also acts to reduce cloud-top cooling, reducing the potential for mixing of the cloud layer. This is observed in both the vertical profiles of the TKE and ϵ, in which it is found that the distributions of turbulence for the sub-cloud and in-cloud layer are completely offset from one another (i.e., the range of turbulent values measured have slight or no overlap for the in-cloud and sub-cloud regions), with the TKE in the sub-cloud layer maximizing for the analysis period, while the TKE in the in-cloud layer is below the average in-cloud value for the analysis period. Measures of vertical velocity variance, TKE, and the buoyancy flux averaged over all 18 flights display a maximum near cloud middle (between normalized in-cloud height, Z*, values of 0.25 and 0.75). A total of 10 of the 18 flights display two peaks in TKE within the cloud layer, one near cloud base and another near cloud top, signifying evaporative and radiational cooling near cloud top and latent heating near cloud base. Decoupled boundary layers tend to have a maximum in turbulence in the sub-cloud layer, with only a single peak in turbulence within the cloud layer.

The efficacy of aerosol–cloud radiative perturbations from near-surface emissions in deep open-cell stratocumuli

Abstract. Aerosol–cloud radiative effects are determined and quantified in simulations of deep open-cell stratocumuli observed during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) campaign off the west coast of Chile. The cloud deck forms in a boundary layer 1.5 km deep, with cell sizes reaching 50 km in diameter. Global databases of ship tracks suggest that these linear structures are seldom found in boundary layers this deep. Here, we quantify the changes in cloud radiative properties to a continuous aerosol point source moving along a fixed emission line releasing 1017 particles per second. We show that a spatially coherent cloud perturbation is not evident along the emission line. Yet our model simulates an increase in domain-mean all-sky albedo of 0.05, corresponding to a diurnally averaged cloud radiative effect of 20 W m−2, given the annual mean solar insolation at the VOCALS-REx site. Therefore, marked changes in cloud radiative properties in precipitating deep open cells may be driven by anthropogenic near-surface aerosol perturbations, such as those generated by ships. Furthermore, we demonstrate that these changes in cloud radiative properties are masked by the naturally occurring variability within the organised cloud field. A clear detection and attribution of cloud radiative effects to a perturbation in aerosol concentrations becomes possible when sub-filtering of the cloud field is applied, using the spatio-temporal distribution of the aerosol perturbation. Therefore, this work has implications for the detection and attribution of effective cloud radiative forcing in marine stratocumuli, which constitutes one of the major physical uncertainties within the climate system. Our results suggest that ships may sometimes have a substantial radiative effect on marine clouds and albedo, even when ship tracks are not readily visible.

Evaluation of Warm-Rain Microphysical Parameterizations in Mesoscale Simulations of the Cloudy Marine Boundary Layer

Abstract Several warm-rain microphysical parameterizations are evaluated in a regional forecast model setting (using the Naval Research Laboratory’s Coupled Ocean–Atmosphere Mesoscale Prediction System) by evaluating how accurately the model is able to represent the marine boundary layer (MBL). Cloud properties from a large suite of simulations using different parameterizations and concentrations of cloud condensation nuclei (CCN) are compared to ship-based observations from the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study—Regional Experiment (VOCALS-REx) field campaign conducted over the southeastern Pacific (SEP). As in previous studies, the simulations systematically underestimate liquid water path and MBL cloud depth. On the other hand, the simulations overestimate precipitation rates relative to those derived from the scanning C-band radar on board the ship. Most of the simulations exhibit a diurnal cycle, although details differ somewhat from a recent observational study. In addition to direct comparisons with the observations, the internal microphysical consistency of simulated MBL cloud properties is assessed by comparing simulation output to a number of observationally and theoretically derived scalings for precipitation and coalescence scavenging. Simulation results are broadly consistent with these scalings, suggesting COAMPS is behaving in a microphysically consistent fashion. However, microphysical consistency as defined in the analysis is highly dependent upon the horizontal resolution of the model. Excessive depletion of CCN from large coalescence processing rates suggests the importance of parameterizing a source term for CCN or imposing some form of fixed, climatological background CCN concentration.

Marine Boundary Layer Heights and Their Longitudinal, Diurnal, and Interseasonal Variability in the Southeastern Pacific Using COSMIC, CALIOP, and Radiosonde Data

Abstract The spatial and temporal variability of the marine boundary layer (MBL) over the southeastern Pacific is studied using high-resolution radiosonde data from the VAMOS Ocean–Cloud–Atmosphere–Land Study Regional Experiment (VOCALS-REx), lidar cloud measurements from the CALIOP instrument on the CALIPSO satellite, radio occultation (RO) data from the COSMIC satellites, and the ERA-Interim. The height of the MBL (MBLH) is estimated using three RO-derived parameters: the bending angle, refractivity, and water vapor pressure computed from the refractivity derived from a one-dimensional variational data inversion (1D-VAR) procedure. Two different diagnostic methods (minimum gradient and break point method) are compared. The results show that, although a negative bias in the refractivity exists as a result of superrefraction, the spatial and temporal variations of the MBLH determined from the RO observations are consistent with those from CALIOP and the radiosondes. The authors find that the minimum gradient in the RO bending angle gives the most accurate estimation of the MBL height.

Impact of resolution on simulation of closed mesoscale cellular convection identified by dynamically guided watershed segmentation

AbstractOrganized mesoscale cellular convection (MCC) is a common feature of marine stratocumulus clouds that forms in response to interactions among dynamic, microphysical, and radiative processes at the mesoscale. Cloud resolving models begin to resolve some of these processes, but using high resolutions is extremely costly. To understand the impact of limited resolution on MCC, we use the Weather Research and Forecasting model with chemistry and fully coupled cloud‐aerosol interactions to simulate MCC over the southeast Pacific during the Variability of the American Monsoon Systems Ocean‐Cloud‐Atmosphere‐Land Study Regional Experiment (VOCALS‐REx). A suite of experiments with 3 and 9 km grid spacing indicates that the simulations with finer grid spacing have smaller liquid water paths and cloud fractions, while cloud tops are higher. The observed diurnal cycle is reasonably well simulated. To isolate organized MCC characteristics, we develop a new automated method that uses the watershed segmentation combining the detection of cloud boundaries with coincident vertical velocities. This ensures that the detected cloud fields are dynamically consistent for closed MCC, a common feature within the VOCALS‐REx region. We demonstrate that the 3 km simulation is able to reproduce the scaling between horizontal cell size and boundary layer depth seen in satellite observations for the conditions of 900–1400 m deep boundary layers. However, the 9 km simulation is unable to resolve smaller circulations corresponding to shallower boundary layers, instead producing MCC with an invariant horizontal scale for all simulated boundary layers depths. The results demonstrate that the grid spacing needed for proper simulation of the MCC structure in marine stratocumulus regions depends on the boundary layer depth.

Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

Abstract. The chemical composition of aerosol particles (Dp ≤ 1.5 μm) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42−, followed by Na+, Cl−, Org (total organics), NH4+, and NO3−, in decreasing order of importance; CH3SO3− (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH4+ to SO42− equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl− deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO42−. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72° W and 76° W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol concentrations were negligible. The very low levels of CH3SO3− observed as well as the correlation between SO42− and NO3− (which is thought primarily anthropogenic) suggest a limited contribution of DMS to SO42− aerosol production during VOCALS.

Ocean–Cloud–Atmosphere–Land Interactions in the Southeastern Pacific: The VOCALS Program

The present paper describes the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study (VOCALS), an international research program focused on the improved understanding and modeling of the southeastern Pacific (SEP) climate system on diurnal to interannual time scales. In the framework of the SEP climate, VOCALS has two fundamental objectives: 1) improved simulations by coupled atmosphere–ocean general circulation models (CGCMs), with an emphasis on reducing systematic errors in the region; and 2) improved estimates of the indirect effects of aerosols on low clouds and climate, with an emphasis on the more precise quantification of those effects. VOCALS major scientific activities are outlined, and selected achievements are highlighted. Activities described include monitoring in the region, a large international field campaign (the VOCALS Regional Experiment), and two model assessments. The program has already produced significant advances in the understanding of major issues in the SEP: the coastal circulation and the diurnal cycle, the ocean heat budget, factors controlling precipitation and formation of pockets of open cells in stratocumulus decks, aerosol impacts on clouds, and estimation of the first aerosol indirect effect. The paper concludes with a brief presentation on VOCALS contributions to community capacity building before a summary of scientific findings and remaining questions.

Turbulence and Radiation in Stratocumulus-Topped Marine Boundary Layers: A Case Study from VOCALS-REx

AbstractObservations made during a 24-h period as part of the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study Regional Experiment (VOCALS-REx) are analyzed to study the radiation and turbulence associated with the stratocumulus-topped marine boundary layer (BL). The first 14 h exhibited a well-mixed (coupled) BL with an average cloud-top radiative flux divergence of ~130 W m−2; the BL was decoupled during the last 10 h with negligible radiative flux divergence. The averaged radiative cooling very close to the cloud top was −9.04 K h−1 in coupled conditions and −3.85 K h−1 in decoupled conditions. This is the first study that combined data from a vertically pointing Doppler cloud radar and a Doppler lidar to yield the vertical velocity structure of the entire BL. The averaged vertical velocity variance and updraft mass flux during coupled conditions were higher than those during decoupled conditions at all levels by a factor of 2 or more. The vertical velocity skewness was negative in the entire BL during coupled conditions, whereas it was weakly positive in the lower third of the BL and negative above during decoupled conditions. A formulation of velocity scale is proposed that includes the effect of cloud-top radiative cooling in addition to the surface buoyancy flux. When scaled by the velocity scale, the vertical velocity variance and coherent downdrafts had similar magnitude during the coupled and decoupled conditions. The coherent updrafts that exhibited a constant profile in the entire BL during both the coupled and decoupled conditions scaled well with the convective velocity scale to a value of ~0.5.

Evaluation of Modeled Stratocumulus-Capped Boundary Layer Turbulence with Shipborne Data

Abstract Numerically modeled turbulence simulated by the Advanced Research Weather Research and Forecasting Model (ARW) is evaluated with turbulence measurements from NOAA’s high-resolution Doppler lidar on the NOAA Research Vessel Ronald H. Brown during the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study—Regional Experiment (VOCALS-Rex) field program. A nonprecipitating nocturnal marine stratocumulus case is examined, and a nudging technique is applied to allow turbulence to spin up and come into a statistically stationary state with the initial observed cloud field. This “stationary” state is then used as the initial condition for the subsequent free-running simulation. The comparison shows that the modeled turbulence is consistently weaker than that observed. For the same resolution, the turbulence becomes stronger, especially for the horizontal component, as the length of the horizontal domain increases from 6.4 to 25.6 km. Analysis of the power spectral density shows that, even for the largest domain, the horizontal component of the turbulence is limited by the upper limit of the domain size; supporting evidence from past studies is provided. Results suggest that convergence is expected for (i) energy spectra of turbulence with a sufficiently large domain and (ii) liquid water path with an adequately large domain and fine resolution. Additional tests are performed by changing momentum advection and turning off subgrid-scale diffusion. These exhibit more significant changes in turbulence characteristics compared to the sensitivity to domain size and resolution, suggesting that the model behavior is essentially established by the configuration of the model dynamics and physics and that the simulation only gradually improves when domain size and resolution are increased.

Ultrafine sea spray aerosol over the southeastern Pacific: open-ocean contributions to marine boundary layer CCN

Abstract. Accurate measurements of natural aerosol emissions over the ocean are needed to estimate the anthropogenic impact on the environment. In this study, we measured sea spray aerosol (SSA) concentrations with diameters larger than 0.040 μm produced by open-ocean breaking waves over the SEP (southeastern Pacific). Robust statistics were established through repeated airborne flights over 1000 km along 20° S from the coastline of Chile to 85° W during VOCALS-REx (VAMOS Ocean-Cloud-Atmosphere-Land-Study Regional Experiment). Non-volatile SSA number concentrations were inferred using a thermally resolved technique constrained for clean conditions with an Ångström exponent below 0.5, black carbon mass concentration at values lower than 15 ng m−3 and organic aerosol concentration less than 0.02 μg m−3. We found that number concentrations of SSAs active as cloud condensation nuclei (CCN) for a supersaturation of 0.25% varied between 17 and 36 cm−3, but these did not increase with the increasing mean wind speed typically observed further offshore along 20° S. Concurrent increases in mean offshore precipitation rate in excess of about 1 mm d−1 indicate that scavenging of SSAs by precipitation exceeds increases in production at wind speeds above about 8 m s−1. This demonstrates the critical role of precipitation as a major sink of SSA over the remote ocean. Finally, we found that under clean conditions and for estimated stratus supersaturations between 0.20 and 0.43%, SSA represented about 20% of the total potential CCN along 20° S.

Development and impact of hooks of high droplet concentration on remote southeast Pacific stratocumulus

Abstract. Over the southeastern Pacific (SEP), droplet concentration (Nd) in the typically unpolluted marine stratocumulus west of 80° W (> 1000 km offshore) is periodically strongly enhanced in zonally elongated "hook"-shaped features that increase albedo. Here, we examine three hook events using the chemistry version of the Weather Research and Forecasting model (WRF-Chem) with 14 km horizontal resolution, satellite data, and aircraft data from the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). A particularly strong hook yields insights into the development, decay, and radiative impact of these features. Hook development occurs with Nd increasing to polluted levels over the remote ocean primarily due to entrainment of cloud condensation nuclei (CCN) from the lower free troposphere (FT). The feature advects northwestward until the FT CCN source is depleted, after which Nd decreases over a few days due to precipitation and dilution. The model suggests that the FT CCN source supplying the hook consists of high concentrations of small accumulation-mode aerosols that contribute a relatively small amount of aerosol mass to the MBL, in agreement with near-coast VOCALS measurements of polluted layers in the FT. The aerosol particles in this hook originate mainly from a pulse of offshore flow that transports Santiago-region (33–35° S) emissions to the remote marine FT. To provide pollution CCN that can sustain hooks, the FT transport of pollution plumes to the remote ocean requires strong, deep offshore flow. Such flow is favored by a trough approaching the South American coast and a southeastward shift of the climatological subtropical high-pressure system. The model simulations show precipitation suppression in the hook and a corresponding increase in liquid water path (LWP) compared with a simulation without anthropogenic sources. LWP also increases as the hook evolves over time due to increasing stability and decreasing subsidence. WRF-Chem suggests that dimethyl sulfide (DMS) significantly influences the aerosol number and size distributions in a hook, but that hooks do not form without FT CCN. The Twomey effect contributes ~ 50–70% of the albedo increase due to the presence of the hook, while secondary aerosol indirect effects and meteorological influences also contribute significantly. The source of hook aerosols is difficult to determine with the available observations alone. The model provides further explanation of the factors influencing hook formation. Two other weaker hooks during VOCALS-REx are not as well simulated but are also associated with FT offshore flow near Santiago. Hooks demonstrate the importance of free-tropospheric transport of aerosols in modulating the droplet concentration in the southeastern Pacific stratocumulus deck, and present a formidable challenge to simulate accurately in large-scale models.

Meteorological observations on the northern Chilean coast during VOCALS-REx

Abstract. Surface coastal observations from two automatic weather stations at Paposo (~25° S) and radiosonde observations at Paposo and Iquique (~20° S) were carried out during VOCALS-REx (VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment). Within the coastal marine boundary layer (MBL), sea–land breezes are superimposed on the prevailing southerlies, resulting in light northeasterly winds from midnight to early morning and strong southwesterlies in the afternoon. The prevailing northerlies above the MBL and below the top of the Andes are modulated by the onshore-offshore (zonal) flow forced by the diurnal cycle of surface heating/cooling along the western slope of the Andes. The daytime phase of this diurnal cycle is consistent with an enhanced afternoon coastal subsidence manifested in afternoon warming near the top of the subsidence inversion (~1.8 K at 800 hPa), lowering (~130 m) of its base (top of the MBL), and clearing of coastal Sc (stratocumulus) clouds. Results from a numerical simulation of the atmospheric circulation in a mean zonal cross section over the study area capture the afternoon zonal wind divergence and resulting subsidence of about 2 cm s−1 along a narrow (~10 km) coastal strip maximizing at around 800 hPa. Day-to-day variability in the MBL depth during VOCALS-REx shows sub-synoptic oscillations, aside from two major disruptions in connection with a deep trough and a cutoff low, as described elsewhere. These oscillations are phase-locked to those in sea-level pressure and afternoon alongshore southerlies, as found in connection with coastal lows farther south. From 24-h forward trajectories issued from significant points at the coast and inland at the extremes of the diurnal cycle, it can be concluded that the strong mean daytime Andean pumping prevents any possibility of continental sulfur sources from reaching the free troposphere above the Sc cloud deck in at least a one-day timescale, under mean conditions. Conversely, coastal sources could contribute with sulfur aerosols preferentially in the morning, provided that the weak daytime inland flow becomes partially blocked by the coastal terrain.

Evaluating MODIS cloud retrievals with in situ observations from VOCALS-REx

Abstract. Microphysical measurements collected during eleven profiles, by the UK BAe-146 aircraft, through marine stratocumulus as part of the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) are compared to collocated overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Aqua and Terra satellite platforms. The full depth of the cloud is sampled in each case using a Cloud Droplet Probe (CDP) and a Two-Dimensional Stereo Probe (2DS) together sizing cloud and precipitation droplets in the diameter range 2–1260 μm. This allows the total optical depth (τc) of the cloud and effective radius (re) of the droplet size distribution to be compared to MODIS cloud retrievals of the same quantities along with the secondarily derived total liquid water path. When compared to the effective radius at cloud top, the MODIS retrieved re using the 2.1 μm wavelength channel overestimates the in situ measurements on average by 13% with the largest overestimations coinciding with the detection by the 2DS of drizzle sized droplets. We show through consideration of the full vertical profile and penetration depths of the wavelengths used in the retrieval that the expected retrieved values are less than those at cloud top thus increasing the apparent bias in re retrievals particularly when using the 1.6 and 2.1 μm channels, with the 3.7 μm channel retrievals displaying the best agreement with in situ values. Retrievals of τc also tend to overestimate in situ values which, coupled with a high bias in re retrievals, lead to an overestimation of liquid water path. There is little apparent correlation between the variation of the three near-infrared re retrievals and the vertical structure of the cloud observed in situ. Retrievals are performed using measured profiles of water vapour and temperature along with an accurate knowledge of the width of the droplet size distribution which improve agreement between in situ and retrieved values but cannot completely explain the observed biases. Additionally we show that cloud heterogeneity and three-dimensional radiative effects may high skew the mean when averaging over comparison domains but cannot explain all of the apparent high bias. An intercomparison between in situ measurements from the BAe-146 and C-130 platforms is also presented, highlighting the uncertainties associated with in situ observations.

Impact of natural and anthropogenic aerosols on stratocumulus and precipitation in the Southeast Pacific: a regional modelling study using WRF-Chem

Abstract. Cloud-system resolving simulations with the chemistry version of the Weather Research and Forecasting (WRF-Chem) model are used to quantify the relative impacts of regional anthropogenic and oceanic emissions on changes in aerosol properties, cloud macro- and microphysics, and cloud radiative forcing over the Southeast Pacific (SEP) during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) (15 October–16 November 2008). Two distinct regions are identified. The near-coast polluted region is characterized by low surface precipitation rates, the strong suppression of non-sea-salt particle activation due to sea-salt particles, a predominant albedo effect in aerosol indirect effects, and limited impact of aerosols associated with anthropogenic emissions on clouds. Opposite sensitivities to natural marine and anthropogenic aerosol perturbations are seen in cloud properties (e.g., cloud optical depth and cloud-top and cloud-base heights), precipitation, and the top-of-atmosphere and surface shortwave fluxes over this region. The relatively clean remote region is characterized by large contributions of aerosols from non-regional sources (lateral boundaries) and much stronger drizzle at the surface. Under a scenario of five-fold increase in regional anthropogenic emissions, this relatively clean region shows large cloud responses, for example, a 13% increase in cloud-top height and a 9% increase in albedo in response to a moderate increase (25% of the reference case) in cloud condensation nuclei (CCN) concentration. The reduction of precipitation due to this increase in anthropogenic aerosols more than doubles the aerosol lifetime in the clean marine boundary layer. Therefore, the aerosol impacts on precipitation are amplified by the positive feedback of precipitation on aerosol, which ultimately alters the cloud micro- and macro-physical properties, leading to strong aerosol-cloud-precipitation interactions. The high sensitivity is also related to an increase in cloud-top entrainment rate (by 16% at night) due to the increased anthropogenic aerosols. The simulated aerosol-cloud-precipitation interactions due to the increased anthropogenic aerosols have a stronger diurnal cycle over the clean region compared to the near-coast region with stronger interactions at night. During the day, solar heating results in more frequent decoupling of the cloud and sub-cloud layers, thinner clouds, reduced precipitation, and reduced sensitivity to the increase in anthropogenic emissions. This study shows the importance of natural aerosols in accurately quantifying anthropogenic forcing within a regional modeling framework. The results of this study also imply that the energy balance perturbations from increased anthropogenic emissions are larger in the more susceptible clean environment than in already polluted environment and are larger than possible from the first indirect effect alone.

Limited-are a modelling of stratocumulus over South-Eastern Pacific

Abstract. This paper presents application of the Weather Research and Forecasting (WRF) model to limited-area modeling of atmospheric processes over the subtropical south-eastern Pacific, with the emphasis on the stratocumulus-topped boundary layer. The simulations cover a domain from the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) field project conducted in the subtropical south-eastern Pacific in October and November 2008. We focus on a day where the UK's BAe-146 research aircraft encountered Pockets of Open Cells (POCs) at the very western edge of its flight track, rather than on the entire campaign as investigated in previous limited-area modeling studies. Model results are compared to aircraft observations with the main conclusion that the simulated stratocumulus-topped boundary layer is significantly too shallow. This appears to be a combination of an already too shallow boundary layer in the dataset used to provide initial and lateral boundary conditions, and the inability of the WRF model to increase the boundary-layer height. Several sensitivity simulations, applying different subgrid-scale parameterizations available in the model, a larger computational domain and longer simulations, as well as a different dataset providing initial and lateral boundary conditions were all tried to improve the simulation. These changes appeared to have a rather small effect on the results. The model does simulate the formation of mesoscale cloud-free regions that one might consider similar to Pockets of Open Cells observed in nature. However, formation of these regions does not seem to be related to drizzle-induced transition from open- to closed-cell circulations as simulated by LES models. Instead, the cloud-free regions appear to result from mesoscale variations of the lower-tropspheric vertical velocity. Areas of negative vertical velocity with minima (a few cm s−1) near the boundary layer top seem to induce direct evaporation of the cloud layer. It remains to be seen in LES studies whether the mechanism seen in the model is realistic or if it is simply an artifact of interactions between resolved and parameterized processes.

Thermodynamic and Aerosol Controls in Southeast Pacific Stratocumulus

Abstract A near-large-eddy simulation approach with size-revolving (bin) microphysics is employed to evaluate the relative sensitivity of southeast Pacific marine boundary layer cloud properties to thermodynamic and aerosol parameters. Simulations are based on a heavily drizzling cloud system observed by the NOAA ship Ronald H. Brown during the Variability of the American Monsoon Systems (VAMOS) Ocean–Cloud–Atmosphere–Land Study—Regional Experiment (VOCALS-Rex) field campaign. A suite of numerical experiments examines the sensitivity of drizzle to variations in boundary layer depth and cloud condensation nuclei (CCN) concentration in a manner consistent with the variability of those parameters observed during VOCALS-Rex. All four simulations produce cellular structures and turbulence characteristics of a circulation driven predominantly in a bottom-up fashion. The cloud and subcloud layers are coupled by strong convective updrafts that provide moisture to the cloud layer. Distributions of reflectivity calculated from model droplet spectra agree well with reflectivity distributions from the 5-cm-wavelength scanning radar aboard the ship, and the statistical behavior of cells over the course of the simulation is similar to that documented in previous studies of southeast Pacific stratocumulus. The simulations suggest that increased aerosol concentration delays the onset of drizzle, whereas changes in the boundary layer height are more important in modulating drizzle intensity.

Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

Abstract. We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and three aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign-averaged longitudinal gradients, and highlight differences in model simulations with (W) and without (NW) wet deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptual model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, especially in the activation parameterization, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions, and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, and may do so with the reliability required for policy analysis.

Assessing regional scale predictions of aerosols, marine stratocumulus, and their interactions during VOCALS-REx using WRF-Chem

Abstract. This study assesses the ability of the recent chemistry version (v3.3) of the Weather Research and Forecasting (WRF-Chem) model to simulate boundary layer structure, aerosols, stratocumulus clouds, and energy fluxes over the Southeast Pacific Ocean. Measurements from the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) and satellite retrievals (i.e., products from the MODerate resolution Imaging Spectroradiometer (MODIS), Clouds and Earth's Radiant Energy System (CERES), and GOES-10) are used for this assessment. The Morrison double-moment microphysics scheme is newly coupled with interactive aerosols in the model. The 31-day (15 October–16 November 2008) WRF-Chem simulation with aerosol-cloud interactions (AERO hereafter) is also compared to a simulation (MET hereafter) with fixed cloud droplet number concentrations in the microphysics scheme and simplified cloud and aerosol treatments in the radiation scheme. The well-simulated aerosol quantities (aerosol number, mass composition and optical properties), and the inclusion of full aerosol-cloud couplings lead to significant improvements in many features of the simulated stratocumulus clouds: cloud optical properties and microphysical properties such as cloud top effective radius, cloud water path, and cloud optical thickness. In addition to accounting for the aerosol direct and semi-direct effects, these improvements feed back to the simulation of boundary-layer characteristics and energy budgets. Particularly, inclusion of interactive aerosols in AERO strengthens the temperature and humidity gradients within the capping inversion layer and lowers the marine boundary layer (MBL) depth by 130 m from that of the MET simulation. These differences are associated with weaker entrainment and stronger mean subsidence at the top of the MBL in AERO. Mean top-of-atmosphere outgoing shortwave fluxes, surface latent heat, and surface downwelling longwave fluxes are in better agreement with observations in AERO, compared to the MET simulation. Nevertheless, biases in some of the simulated meteorological quantities (e.g., MBL temperature and humidity) and aerosol quantities (e.g., underestimations of accumulation mode aerosol number) might affect simulated stratocumulus and energy fluxes over the Southeastern Pacific, and require further investigation. The well-simulated timing and outflow patterns of polluted and clean episodes demonstrate the model's ability to capture daily/synoptic scale variations of aerosol and cloud properties, and suggest that the model is suitable for studying atmospheric processes associated with pollution outflow over the ocean. The overall performance of the regional model in simulating mesoscale clouds and boundary layer properties is encouraging and suggests that reproducing gradients of aerosol and cloud droplet concentrations and coupling cloud-aerosol-radiation processes are important when simulating marine stratocumulus over the Southeast Pacific.

Cloud water composition over the southeastern Pacific Ocean during the VOCALS regional experiment

Abstract Relatively few measurements exist of cloud water composition over the open ocean, despite the importance of clouds as processors of atmospheric aerosols and trace gases in such regions. In order to improve understanding of cloud water composition in the southeast Pacific, and to determine the capacity of regional clouds for aqueous sulfate production, cloud water was collected aboard the NCAR C-130 during VOCALS-REx (VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment) in October and November, 2008. A total of 72 cloud water samples were collected on 14 flights using the NCAR/CSU airborne cloud water collector. Cloud water samples were collected over a region extending from approximately 71–85° west and from approximately 18–30° south. Cloud water pH ranged from 2.9 to 7.2 with an average of 4.3. Samples were also analyzed for major inorganic ions, hydrogen peroxide, sulfur(IV), carboxylic and dicarboxylic acids, formaldehyde, total Fe and Mn, and total organic carbon. Sodium and chloride were the most abundant solutes, while organic matter was found to contribute only 12%, on average, of the total measured solute load. Cloud water and trace gas measurements aboard the aircraft were used to examine the importance of various oxidation pathways for in-cloud sulfate production. S(IV) oxidation by H 2 O 2 was found to be the most important pathway and excess cloud water H 2 O 2 concentrations revealed considerable potential for additional, rapid in-cloud sulfate production by this mechanism. S(IV) oxidation by ozone was important when cloud water pH climbed above 5.5 and was the fastest oxidation pathway 24% of the time.