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A review of the theoretical basis for bulk mass flux convective parameterization

Most parameterizations for precipitating convection in use today are bulk schemes, in which an ensemble of cumulus elements with different properties is modelled as a single, representative entraining-detraining plume. We review the underpinning mathematical model for such parameterizations, in particular by comparing it with spectral models in which elements are not combined into the representative plume. The chief merit of a bulk model is that the representative plume can be described by an equation set with the same structure as that which describes each element in a spectral model. The equivalence relies on an ansatz for detrained condensate introduced by Yanai et al. (1973) and on a simplified microphysics. There are also conceptual differences in the closure of bulk and spectral parameterizations. In particular, we show that the convective quasi-equilibrium closure of Arakawa and Schubert (1974) for spectral parameterizations cannot be carried over to a bulk parameterization in a straightforward way. Quasi-equilibrium of the cloud work function assumes a timescale separation between a slow forcing process and a rapid convective response. But, for the natural bulk analogue to the cloud-work function, the relevant forcing is characterised by a different timescale, and so its quasi-equilibrium entails a different physical constraint. Closures of bulk parameterizations that use a parcel value of CAPE do not suffer from this timescale issue. However, the Yanai et al. (1973) ansatz must be invoked as a necessary ingredient of those closures.
Turbulence associated with mountain waves over Northern Scandinavia – a case study using the ESRAD VHF radar and the WRF mesoscale model

We use measurements by the 52 MHz wind-profiling radar ESRAD, situated near Kiruna in Arctic Sweden, and simulations using the Advanced Research and Weather Forecasting model, WRF, to study vertical winds and turbulence in the troposphere in mountain-wave conditions on 23, 24 and 25 January 2003. We find that WRF can accurately match the vertical wind signatures at the radar site when the spatial resolution for the simulations is 1 km. The horizontal and vertical wavelengths of the dominating mountain-waves are ~10–20 km and the amplitudes in vertical wind 1–2 m/s. Turbulence below 5500 m height, is seen by ESRAD about 40% of the time. This is a much higher rate than WRF predictions for conditions of Richardson number (Ri) <1 but similar to WRF predictions of Ri<2. WRF predicts that air crossing the 100 km wide model domain centred on ESRAD has a ~10% chance of encountering convective instabilities (Ri<0) somewhere along the path. The cause of low Ri is a combination of wind-shear at synoptic upper-level fronts and perturbations in static stability due to the mountain-waves. Comparison with radiosondes suggests that WRF underestimates wind-shear and the occurrence of thin layers with very low static stability, so that vertical mixing by turbulence associated with mountain waves may be significantly more than suggested by the model.
Chemical transformations of Hg° during Arctic mercury depletion events sampled from the NASA DC-8

Atmospheric Mercury Depletion Events (MDEs) in Arctic springtime were investigated utilizing a box model based on airborne measurements from the NASA DC-8 during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. Measurements showed that MDEs occurred near the surface and always over the Arctic Ocean accompanied by concurrent ozone (O3) depletion, enhancement in Br2 mixing ratios, and decreases in ethyne and light weight alkanes. Backward trajectories indicated that most air masses inside the MDEs originated at low altitude over the ocean presumably generating a halogen-rich environment. We developed a box model which considered only gas phase reactions of mercury, halogen species, and O3 chemistry. We conducted a series of sensitivity simulations to determine the factors that are of most importance to MDE formation. The box model results suggested that continuous enhancement of Br2 mixing ratios, a high intensity of solar radiation, or a relatively high NOx regime expedited Hg° depletion. These environments generated high concentrations of Br radical, and thus the model results indicated that the Br radical was very important for Hg° depletion. Utilizing different rate constants for reaction of Hg° + Br produced times to reach Hg° depletion ranging from 22 to 32 h.
Tracer measurements in the tropical tropopause layer during the AMMA/SCOUT-O3 aircraft campaign

We present airborne in situ measurements made during the AMMA (African Monsoon Multidisciplinary Analysis)/SCOUT-O3 campaign between 31 July and 17 August 2006 on board the M55 Geophysica aircraft, based in Ouagadougou, Burkina Faso. CO2 and N2O were measured with the High Altitude Gas Analyzer (HAGAR), CO was measured with the Cryogenically Operated Laser Diode (COLD) instrument, and O3 with the Fast Ozone ANalyzer (FOZAN). We analyse the data obtained during five local flights to study the dominant transport processes controlling the tropical tropopause layer (TTL, here ~350–375 K) and lower stratosphere above West-Africa: deep convection up to the level of main convective outflow, overshooting of deep convection, and horizontal inmixing across the subtropical tropopause. Besides, we examine the morphology of the stratospheric subtropical barrier. Except for the flight of 13 August, distinct minima in CO2 mixing ratios indicate convective outflow of boundary layer air in the TTL. The CO2 profiles show that the level of main convective outflow was mostly located at potential temperatures between 350 and 360 K, and for 11 August reached up to 370 K. While the CO2 minima indicate quite significant convective influence, the O3 profiles suggest that the observed convective signatures were mostly not fresh, but of older origin (several days or more). When compared with the mean O3 profile measured during a previous campaign over Darwin in November 2005, the O3 minimum at the main convective outflow level was less pronounced over Ouagadougou. Furthermore O3 mixing ratios were much higher throughout the whole TTL and, unlike over Darwin, rarely showed low values observed in the regional boundary layer. Signatures of irreversible mixing following overshooting of convective air were scarce in the tracer data. Some small signatures indicative of this process were found in CO2 profiles between 390 and 410 K during the flights of 4 and 8 August, and in CO data at 410 K on 7 August. However, the absence of expected corresponding signatures in other tracer data makes this evidence inconclusive, and overall there is little indication from the observations that overshooting convection has a profound impact on gas-phase tracer TTL composition during AMMA. We find the amount of photochemically aged air isentropically mixed into the TTL across the subtropical tropopause to be not significant. Using the N2O observations we estimate the fraction of aged extratropical stratospheric air in the TTL to be 0.0±0.1 up to 370 K during the local flights. Above the TTL this fraction increases to 0.3±0.1 at 390 K. The subtropical barrier, as indicated by the slope of the correlation between N2O and O3 between 415 and 490 K, does not appear as a sharp border between the tropics and extratropics, but rather as a gradual transition region between 10° N and 25° N where isentropic mixing between these two regions may occur.
Heterogeneous freezing of droplets with immersed mineral dust particles – measurements and parameterization

During the measurement campaign FROST (FReezing Of duST), LACIS (Leipzig Aerosol Cloud Interaction Simulator) was used to investigate the immersion freezing behavior of size selected, coated and uncoated Arizona Test Dust (ATD) particles with a mobility diameter of 300 nm. Particles were coated with succinic acid (C4H6O4), sulfuric acid (H2SO4) and ammonium sulfate ((NH4)2SO4). Ice fractions at mixed-phase cloud temperatures ranging from 233.15 K to 239.15 K (±0.60 K) were determined for all types of particles. In this temperature range, pure ATD particles and those coated with C4H6O4 or small amounts of H2SO4 were found to be the most efficient ice nuclei (IN). ATD particles coated with (NH4)2SO4 were the most inefficient IN. Since the supercooled droplets were highly diluted before freezing occurred, a freezing point suppression due to the soluble material on the particles (and therefore in the droplets) cannot explain this observation. Therefore, it is reasonable to assume that the coatings lead to particle surface alterations which cause the differences in the IN abilities. Two different theoretical approaches based on the stochastic and the singular hypotheses were applied to clarify and parameterize the freezing behavior of the particles investigated. Both approaches describe the experimentally determined results, yielding parameters that can subsequently be used to compare our results to those from other studies. However, we cannot clarify at the current state which of the two approaches correctly describes the investigated immersion freezing process. But both approaches confirm the assumption that the coatings lead to particle surface modifications lowering the nucleation efficiency. The stochastic approach interprets the reduction in nucleation rate from coating as primarily due to an increase in the thermodynamic barrier for ice formation (i.e., changes in interfacial free energies). The singular approach interprets the reduction as resulting from a reduced surface density of active sites.
Kinetic multi-layer model of aerosol surface and bulk chemistry (KM-SUB): the influence of interfacial transport and bulk diffusion on the oxidation of oleic acid by ozone

We present a novel kinetic multi-layer model that explicitly resolves mass transport and chemical reaction at the surface and in the bulk of aerosol particles (KM-SUB). The model is based on the PRA framework of gas-particle interactions (Pöschl-Rudich-Ammann, 2007), and it includes reversible adsorption, surface reactions and surface-bulk exchange as well as bulk diffusion and reaction. Unlike earlier models, KM-SUB does not require simplifying assumptions about steady-state conditions and radial mixing. The temporal evolution and concentration profiles of volatile and non-volatile species at the gas-particle interface and in the particle bulk can be modeled along with surface concentrations and gas uptake coefficients. In this study we explore and exemplify the effects of bulk diffusion on the rate of reactive gas uptake for a simple reference system, the ozonolysis of oleic acid particles, in comparison to experimental data and earlier model studies. We demonstrate how KM-SUB can be used to interpret and analyze experimental data from laboratory studies, and how the results can be extrapolated to atmospheric conditions. In particular, we show how interfacial and bulk transport, i.e., surface accommodation, bulk accommodation and bulk diffusion, influence the kinetics of the chemical reaction. Sensitivity studies suggest that in fine air particulate matter oleic acid and compounds with similar reactivity against ozone (carbon-carbon double bonds) can reach chemical lifetimes of many hours only if they are embedded in a (semi-)solid matrix with very low diffusion coefficients (≤10−10 cm2 s−1). Depending on the complexity of the investigated system, unlimited numbers of volatile and non-volatile species and chemical reactions can be flexibly added and treated with KM-SUB. We propose and intend to pursue the application of KM-SUB as a basis for the development of a detailed master mechanism of aerosol chemistry as well as for the derivation of simplified but realistic parameterizations for large-scale atmospheric and climate models.
Mercury emission from crematories in Japan

Anthropogenic sources of mercury emissions have a significant impact on global pollution. Therefore, finding uncharacterised sources and assessing the emissions from these sources are important. However, limited data are available worldwide on mercury emissions from crematories. In Japan, 99.9% of dead bodies are cremated, which is the highest percentage in the world, and more than 1600 crematories are in operation. We thus focused on emissions from crematories in Japan. The number of targeted facilities was seven, and we used continuous emission monitoring to measure the mercury concentrations and investigate mercury behaviour. The total mercury concentrations in stack gases were a few μg/Nm3 (normal cubic meters). Considering the time profile of mercury and its species in cremations, the findings confirmed that the mercury in stack gas originated from dental amalgam. The amount of mercury emissions was calculated using the total concentration and gas flow rate. Furthermore, the annual amount of mercury emission from crematories in Japan was estimated by using the total number of corpses. The emission amount was considerably lower than that estimated in the United Kingdom. From statistical analyses on population demographics and measurements, future total emissions from crematories were also predicted. As a result, the amount of mercury emitted by crematories will likely increase by 2.6-fold from 2007 to 2037.
Measurements of iodine monoxide at a semi polluted coastal location

Point source measurements of IO by laser induced fluorescence spectroscopy were made at a semi-polluted coastal location during the Reactive Halogens in the Marine Boundary Layer (RHaMBLe) campaign in September 2006. The site, on the NW French coast in Roscoff, was characterised by extensive intertidal macroalgae beds which were exposed at low tide. The closest known iodine active macroalgae beds were at least 300 m from the measurement point. From 20 days of measurements, IO was observed above the instrument limit of detection on 14 days, of which a clear diurnal profile was observed on 11 days. The maximum IO mixing ratio was 30.0 pptv (10 s integration period) during the day, amongst the highest concentrations ever observed in the atmosphere, and 1–2 pptv during the night. IO concentrations were strongly dependent on tidal height, the intensity of solar irradiation and meteorological conditions. An intercomparison of IO measurements made using point source and spatially averaged DOAS instruments confirms the presence of hot-spots of IO caused by an inhomogeneous distribution of macroalgae. The co-incident, point source measurement of IO and ultra fine particles (2.5 nm≥d≥10 nm) displayed a strong correlation, providing evidence that IO is involved in the production pathway of ultra fine particles at coastal locations. Finally, a modelling study shows that high IO concentrations which are likely to be produced in a macrolagae rich environment can significantly perturb the concentrations of OH and HO2 radicals. The effect of IO on HOx is reduced as NOx concentrations increase.
A new ENSO index derived from satellite measurements of column ozone

Column Ozone measured in tropical latitudes from Nimbus 7 total ozone mapping spectrometer (TOMS), Earth Probe TOMS, solar backscatter ultraviolet (SBUV), and Aura ozone monitoring instrument (OMI) are used to derive an El Nino-Southern Oscillation (ENSO) index. This index, which covers a time period from 1979 to the present, is defined as the "Ozone ENSO Index" (OEI) and is the first developed from atmospheric trace gas measurements. The OEI is constructed by first averaging monthly mean column ozone over two broad regions in the western and eastern Pacific and then taking their difference. This differencing yields a self-calibrating ENSO index which is independent of individual instrument calibration offsets and drifts in measurements over the long record. The combined Aura OMI and MLS ozone data confirm that zonal variability in total column ozone in the tropics caused by ENSO events lies almost entirely in the troposphere. As a result, the OEI can be derived directly from total column ozone instead of tropospheric column ozone. For clear-sky ozone measurements a +1 K change in Nino 3.4 index corresponds to +2.9 Dobson Unit (DU) change in the OEI, while a +1 hPa change in SOI coincides with a −1.7 DU change in the OEI. For ozone measurements under all cloud conditions these numbers are +2.4 DU and −1.4 DU, respectively. As an ENSO index based upon ozone, it is potentially useful in evaluating climate models predicting long term changes in ozone and other trace gases.
Sulfur cycle and sulfate radiative forcing simulated from a coupled global climate-chemistry model

The sulfur cycle and radiative effects of sulfate aerosol on climate are studied with a Global tropospheric Climate-Chemistry Model in which chemistry, radiation and dynamics are fully coupled. Production and removal mechanisms of sulfate are analyzed for the conditions of natural and anthropogenic sulfur emissions. Results show that the 1985 anthropogenic emission tripled the global SO2 and sulfate loadings from its natural value of 0.16 and 0.10 Tg S, respectively. Under natural conditions, the fraction of sulfate produced in-cloud is 74%; whereas with anthropogenic emissions, the fraction of in-cloud sulfate production slightly increased to 76%. Lifetimes of SO2 and sulfate under polluted conditions are estimated to be 1.7 and 2.0 days, respectively. The tripling of sulfate results in a direct radiative forcing of −0.43 W m−2 (clear-sky) or −0.24 W m−2 (all-sky), and a significant first indirect forcing of −1.85 W m−2, leading to a mean global cooling of about 0.1 K. Regional forcing and responses are significantly stronger than the global values. The first indirect forcing is sensitive to the relationship between aerosol concentration and cloud droplet number concentration which requires further investigation. Two aspects of chemistry-climate interaction are addressed. Firstly, the coupling effects lead to a slight decrease of 1% in global sulfate loading for both the cases of natural and anthropogenic added sulfur emissions. Secondly, only the indirect effect of sulfate aerosols yields significantly stronger signals in changes of near surface temperature and sulfate loading than changes due to intrinsic climate variability, while other responses to the indirect effect and all responses to the direct effect are below noise level.