Items

Advanced search

The effects of turbulent collision–coalescence on precipitation formation and precipitation-dynamical feedbacks in simulations of stratocumulus and shallow cumulus convection

A double moment warm rain scheme that includes the effects of turbulence on droplet collision rates has been implemented in a large-eddy model to investigate the impact of turbulence effects on clouds and precipitation. Simulations of shallow cumulus and stratocumulus show that different precipitation-dynamical feedbacks occur in these regimes when the effects of turbulence are included in the microphysical processes. In both cases inclusion of turbulent microphysics increases precipitation due to a more rapid conversion of cloud water to rain. In the shallow convection case, the greater water loading in the upper cloud levels reduces the buoyancy production of turbulent kinetic energy and the entrainment. The stratocumulus case on the other hand shows a weak positive precipitation feedback, with enhanced rainwater producing greater evaporation, stronger circulations and more turbulence. Sensitivity studies in which the cloud droplet number was varied show that greater number concentrations suppress the stratocumulus precipitation leading to larger liquid water paths. This positive second indirect aerosol effect shows no sensitivity to whether or not the effects of turbulence on droplet collision rates are included. While the sign of the second indirect effect is negative in the shallow convection case whether the effects of turbulence are considered or not, the magnitude of the effect is doubled when the turbulent microphysics are used. It is found that for these two different cloud regimes turbulence has a larger effect than cloud droplet number and the use of a different bulk microphysics scheme on producing rainfall in shallow cumuli. However, for the stratocumulus case examined here, the effects of turbulence on rainfall are not statistically significant and instead it is the cloud droplet number concentration or the choice of bulk microphysics scheme that has the largest control on the rain water.
CARIBIC DOAS observations of nitrous acid and formaldehyde in a large convective cloud

The chemistry in large thunderstorm clouds is influenced by local lightning-NOx production and uplift of boundary layer air. Under these circumstances trace gases like nitrous acid (HONO) or formaldehyde (HCHO) are expected to be formed or to reach the tropopause region. However, up to now only few observations of HONO at this altitude have been reported. Here we report on a case study where enhancements in HONO, HCHO and nitrogen oxides (NOx) were observed by the CARIBIC flying laboratory (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container). The event took place in a convective system over the Caribbean Sea in August 2011. Inside the cloud the light path reaches up to 100 km. Therefore the DOAS instrument on CARIBIC was very sensitive to the tracers inside the cloud. Based on the enhanced slant column densities of HONO, HCHO and NO2, average mixing ratios of 37, 468 and 210 ppt, respectively, were calculated. These data represent averages for constant mixing ratios inside the cloud. However, a large dependency on the assumed profile is found; for HONO a mixing ratio of 160 ppt is retrieved if the total amount is assumed to be situated in the uppermost 2 km of the cloud. The NO in situ instrument measured peaks up to 5 ppb NO inside the cloud; the background in the cloud was about 1.3 ppb, and hence clearly above the average outside the cloud (≈ 150 ppt). The high variability and the fact that the enhancements were observed over a pristine marine area led to the conclusion that, in all likelihood, the high NO concentrations were caused by lighting. This assumption is supported by the number of flashes that the World Wide Lightning Location Network (WWLLN) counted in this area before and during the overpass. The chemical box model CAABA is used to estimate the NO and HCHO source strengths which are necessary to explain our measurements. For NO a source strength of 10 × 109 molec cm−2 s−1 km−1 is found, which corresponds to the lightning activity as observed by the World Wide Lightning Location network, and lightning emissions of 5 × 1025 NO molec flash−1 (2.3–6.4 × 1025). The uncertainties are determined by a change of the input parameters in the box model, the cloud top height and the flash density. The emission rate per flash is scaled up to a global scale and 1.9 (1.4–2.5) tg N a−1 is estimated. The HCHO updraught is of the order of 120 × 109 molec cm−2 s−1 km−1. Also isoprene and CH3OOH as possible HCHO sources are discussed.
The effect of atmospheric aerosol particles and clouds on net ecosystem exchange in the Amazon

Carbon cycling in the Amazon is closely linked to atmospheric processes and climate in the region as a consequence of the strong coupling between the atmosphere and biosphere. This work examines the effects of changes in net radiation due to atmospheric aerosol particles and clouds on the net ecosystem exchange (NEE) of CO2 in the Amazon region. Some of the major environmental factors affecting the photosynthetic activity of plants, such as air temperature and relative humidity, were also examined. An algorithm for clear-sky irradiance was developed and used to determine the relative irradiance, f, which quantifies the percentage of solar radiation absorbed and scattered due to atmospheric aerosol particles and clouds. Aerosol optical depth (AOD) was calculated from irradiances measured with the MODIS (Moderate Resolution Imaging Spectroradiometer) sensor, onboard the Terra and Aqua satellites, and was validated with ground-based AOD measurements from AERONET (Aerosol Robotic Network) sun photometers. Carbon fluxes were measured using eddy covariance technique at the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) flux towers. Two sites were studied: the Jaru Biological Reserve (RBJ), located in Rondonia, and the Cuieiras Biological Reserve at the K34 LBA tower (located in a preserved region in the central Amazon). Analysis was performed continuously from 1999 to 2009 at K34 and from 1999 to 2002 at RBJ, and includes wet, dry and transition seasons. In the Jaru Biological Reserve, a 29% increase in carbon uptake (NEE) was observed when the AOD ranged from 0.10 to 1.5 at 550 nm. In the Cuieiras Biological Reserve, the aerosol effect on NEE was smaller, accounting for an approximate 20% increase in NEE. High aerosol loading (AOD above 3 at 550 nm) or high cloud cover leads to reductions in solar flux and strong decreases in photosynthesis up to the point where NEE approaches zero. The observed increase in NEE is attributed to an enhancement (~50%) in the diffuse fraction of photosynthetic active radiation (PAR). The enhancement in diffuse PAR can be done through increases in aerosols and/or clouds. In the present study, it was not possible to separate these two components. Significant changes in air temperature and relative humidity resulting from changes in solar radiation fluxes under high aerosol loading were also observed at both sites. Considering the long-range transport of aerosols in the Amazon, the observed changes in NEE for these two sites may occur over large areas in the Amazon, significantly altering the carbon balance in the largest rainforest in the world.
Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES

Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.
Global top-down smoke-aerosol emissions estimation using satellite fire radiative power measurements

Fire emissions estimates have long been based on bottom-up approaches that are not only complex, but also fraught with compounding uncertainties. We present the development of a global gridded (1° × 1°) emission coefficients (Ce) product for smoke total particulate matter (TPM) based on a top-down approach using coincident measurements of fire radiative power (FRP) and aerosol optical thickness (AOT) from the Moderate-resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Terra and Aqua satellites. This new Fire Energetics and Emissions Research version 1.0 (FEER.v1) Ce product has now been released to the community and can be obtained from <a href="http://feer.gsfc.nasa.gov/"target=_blank">http://feer.gsfc.nasa.gov/</a>, along with the corresponding 1-to-1 mapping of their quality assurance (QA) flags that will enable the Ce values to be filtered by quality for use in various applications. The regional averages of Ce values for different ecosystem types were found to be in the ranges of 16–21 g MJ−1 for savanna and grasslands, 15–32 g MJ−1 for tropical forest, 9–12 g MJ−1 for North American boreal forest, and 18–26 g MJ−1 for Russian boreal forest, croplands and natural vegetation. The FEER.v1 Ce product was multiplied by time-integrated FRP data to calculate regional smoke TPM emissions, which were compared with equivalent emissions products from three existing inventories. FEER.v1 showed higher and more reasonable smoke TPM estimates than two other emissions inventories that are based on bottom-up approaches and already reported in the literature to be too low, but portrayed an overall reasonable agreement with another top-down approach. This suggests that top-down approaches may hold better promise and need to be further developed to accelerate the reduction of uncertainty associated with fire emissions estimation in air-quality and climate research and applications. Results of the analysis of FEER.v1 data for 2004–2011 show that 65–85 Tg yr−1 of TPM is emitted globally from open biomass burning, with a generally decreasing trend over this short time period. The FEER.v1 Ce product is the first global gridded product in the family of "emission factors", that is based essentially on satellite measurements, and requires only direct satellite FRP measurements of an actively burning fire anywhere to evaluate its emission rate in near-real time, which is essential for operational activities, such as the monitoring and forecasting of smoke emission impacts on air quality.
The impact of monoaromatic hydrocarbons on OH reactivity in the coastal UK boundary layer and free troposphere

Reaction with the hydroxyl radical (OH) is the dominant removal mechanism for virtually all volatile organic compounds (VOCs) in the atmosphere; however, it can be difficult to reconcile measured OH reactivity with known sinks. Unresolved higher molecular weight VOCs contribute to OH sinks, of which monoaromatics are potentially an important sub-class. A method based on comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC × GC-TOFMS) has been developed that extends the degree with which larger VOCs can be individually speciated from whole air samples (WAS). The technique showed excellent sensitivity, resolution and good agreement with an established gas chromatography–flame ionisation (GC-FID) method, for compounds amenable to analysis on both instruments. Measurements have been made of VOCs within the UK east coast marine boundary layer and free troposphere, using samples collected from five aircraft flights in winter 2011. Ten monoaromatic compounds with an array of different alkyl ring substituents have been quantified, in addition to the simple aromatics, benzene, toluene, ethyl benzene and Σm- and p-xylene. These additional compounds were then included in constrained box model simulations of atmospheric chemistry occurring at two UK rural and suburban field sites in order to assess the potential impact of these larger monoaromatics species on OH reactivity; they have been calculated to contribute an additional 2–6% to the overall modelled OH loss rate, providing a maximum additional OH sink of ~0.9 s−1.
Atmospheric tar balls: aged primary droplets from biomass burning?

Atmospheric tar balls are particles of special morphology and composition that are fairly abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and, by extension, climate forcing. Here we suggest that tar balls are produced by the direct emission of liquid tar droplets followed by heat transformation upon biomass burning. For the first time in atmospheric chemistry we generated tar-ball particles from liquid tar obtained previously by dry distillation of wood in an all-glass apparatus in the laboratory with the total exclusion of flame processes. The particles were perfectly spherical with a mean optical diameter of 300 nm, refractory, externally mixed, and homogeneous in the contrast of the transmission electron microscopy (TEM) images. They lacked any graphene-like microstructure and exhibited a mean carbon-to-oxygen ratio of 10. All of the observed characteristics of laboratory-generated particles were very similar to those reported for atmospheric tar-ball particles in the literature, strongly supporting our hypothesis regarding the formation mechanism of atmospheric tar-ball particles.
Short vertical-wavelength inertia-gravity waves generated by a jet–front system at Arctic latitudes – VHF radar, radiosondes and numerical modelling

Inertia-gravity waves with very short vertical wavelength (λz≤1000 m) are a very common feature of the lowermost stratosphere as observed by the 52 MHz radar ESRAD (Esrange MST radar) in northern Scandinavia (67.88° N, 21.10° E). The waves are seen most clearly in radar-derived profiles of buoyancy frequency (N). Here, we present a case study of typical waves from 21 February to 22 February 2007. Good agreement between N2 derived from radiosondes and by radar shows the validity of the radar determination of N2. Large-amplitude wave signatures in N2 are clearly observed by the radar and the radiosondes in the lowermost stratosphere, from 9 km to 14–16 km height. Vertical profiles of horizontal wind components and potential temperature from the radiosondes show the same waves. Mesoscale simulations with the Weather Research and Forecasting (WRF) model are carried out to complement the analysis of the waves. Good agreement between the radar and radiosonde measurements and the model (except for the wave amplitude) shows that the model gives realistic results and that the waves are closely associated to the upper-level front in an upper-troposphere jet–front system. Hodographs of the wind fluctuations from the radiosondes and model data show that the waves propagate upward in the lower stratosphere confirming that the origin of the waves is in the troposphere. The observations and modelling all indicate vertical wavelengths of 700 ± 200 m. The radiosonde hodograms indicate horizontal wavelengths between 40 and 110 km and intrinsic periods between 6 and 9 h. The wave amplitudes indicated by the model are however an order of magnitude less than in the observations. Finally, we show that the profiles of N2 measured by the radar can be used to estimate wave amplitudes, horizontal wavelengths, intrinsic periods and momentum fluxes which are consistent with the estimates from the radiosondes.
Technical Note: Particulate reactive oxygen species concentrations and their association with environmental conditions in an urban, subtropical climate

Reactions between hydrocarbons and ozone or hydroxyl radicals lead to the formation of oxidized species, including reactive oxygen species (ROS), and secondary organic aerosol (SOA) in the troposphere. ROS can be carried deep into the lungs by small aerodynamic particles where they can cause oxidative stress and cell damage. While environmental studies have focused on ROS in the gas phase and rainwater, it is also important to determine concentrations of ROS on respirable particles. Samples of PM2.5 collected over 3 h at midday on 40 days during November 2011 and September 2012 show that the particulate ROS concentration in Austin, Texas, ranged from a minimum value of 0.02 nmoles H2O2 m−3 air in December to 3.81 nmoles H2O2 m−3 air in September. Results from correlation tests and linear regression analysis on particulate ROS concentrations and environmental conditions (which included ozone and PM2.5 concentrations, temperature, relative humidity, precipitation and solar radiation) indicate that ambient particulate ROS is significantly influenced by the ambient ozone concentration, temperature and incident solar radiation. Particulate ROS concentrations measured in this study were in the range reported by other studies in the US, Taiwan and Singapore. This study is one of the first to assess seasonal variations in particulate ROS concentrations and helps explain the influence of environmental conditions on particulate ROS concentrations.
Comparison of GEOS-5 AGCM planetary boundary layer depths computed with various definitions

Accurate models of planetary boundary layer (PBL) processes are important for forecasting weather and climate. The present study compares seven methods of calculating PBL depth in the GEOS-5 atmospheric general circulation model (AGCM) over land. These methods depend on the eddy diffusion coefficients, bulk and local Richardson numbers, and the turbulent kinetic energy. The computed PBL depths are aggregated to the Köppen–Geiger climate classes, and some limited comparisons are made using radiosonde profiles. Most methods produce similar midday PBL depths, although in the warm, moist climate classes the bulk Richardson number method gives midday results that are lower than those given by the eddy diffusion coefficient methods. Additional analysis revealed that methods sensitive to turbulence driven by radiative cooling produce greater PBL depths, this effect being most significant during the evening transition. Nocturnal PBLs based on Richardson number methods are generally shallower than eddy diffusion coefficient based estimates. The bulk Richardson number estimate is recommended as the PBL height to inform the choice of the turbulent length scale, based on the similarity to other methods during the day, and the improved nighttime behavior.