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Observation operator for the assimilation of aerosol type resolving satellite measurements into a chemical transport model

Modelling of aerosol particles with chemical transport models is still based mainly on static emission databases while episodic emissions cannot be treated sufficiently. To overcome this situation, a coupling of chemical mass concentration modelling with satellite-based measurements relying on physical and optical principles has been developed. This study deals with the observation operator for a component-wise assimilation of satellite measurements. It treats aerosol particles classified into water soluble, water insoluble, soot, sea salt and mineral dust containing aerosol particles in the atmospheric boundary layer as separately assimilated aerosol components. It builds on a mapping of aerosol classes used both in observation and model space taking their optical and chemical properties into account. Refractive indices for primary organic carbon particles, anthropogenic particles, and secondary organic species have been defined based on a literature review. Together with a treatment of different size distributions in observations and model state, this allows transforming the background from mass concentrations into aerosol optical depths. A two-dimensional, variational assimilation is applied for component-wise aerosol optical depths. Error covariance matrices are defined based on a validation against AERONET sun photometer measurements. Analysis fields are assessed threefold: (1) through validation against AERONET especially in Saharan dust outbreak situations, (2) through comparison with the British Black Smoke and Sulphur Dioxide Network for soot-containing particles, and (3) through comparison with measurements of the water soluble components SO4, NH4, and NO3 conducted by the EMEP (European Monitoring and Evaluation Programme) network. Separately, for the water soluble, the soot and the mineral dust aerosol components a bias reduction and subsequent a root mean square error reduction is observed in the analysis for a test period from July to November 2003. Additionally, examples of an improved analysis during wildfire and dust outbreak situations are shown.
An overview of current issues in the uptake of atmospheric trace gases by aerosols and clouds

A workshop was held in the framework of the ACCENT (Atmospheric Composition Change – a European Network) Joint Research Programme on "Aerosols" and the Programme on "Access to Laboratory Data". The aim of the workshop was to hold "Gordon Conference" type discussion covering accommodation and reactive uptake of water vapour and trace pollutant gases on condensed phase atmospheric materials. The scope was to review and define the current state of knowledge of accommodation coefficients for water vapour on water droplet and ice surfaces, and uptake of trace gas species on a variety of different surfaces characteristic of the atmospheric condensed phase particulate matter and cloud droplets. Twenty-six scientists participated in this meeting through presentations, discussions and the development of a consensus review. In this review we present an analysis of the state of knowledge on the thermal and mass accommodation coefficient for water vapour on aqueous droplets and ice and a survey of current state-of the-art of reactive uptake of trace gases on a range of liquid and solid atmospheric droplets and particles. The review recommends consistent definitions of the various parameters that are needed for quantitative representation of the range of gas/condensed surface kinetic processes important for the atmosphere and identifies topics that require additional research.
Evaluation of stratocumulus cloud prediction in the Met Office forecast model during VOCALS-REx

Observations in the subtropical southeast Pacific obtained during the VOCALS-REx field experiment are used to evaluate the representation of stratocumulus cloud in the Met Office forecast model and to identify key areas where model biases exist. Marked variations in the large scale structure of the cloud field were observed during the experiment on both day-to-day and on diurnal timescales. In the remote maritime region the model is shown to have a good representation of synoptically induced variability in both cloud cover and marine boundary layer depth. Satellite observations show a strong diurnal cycle in cloud fraction and liquid water path in the stratocumulus with enhanced clearances of the cloud deck along the Chilean and Peruvian coasts on certain days. The model accurately simulates the phase of the diurnal cycle but is unable to capture the coastal clearing of cloud. Observations along the 20° S latitude line show a gradual increase in the depth of the boundary layer away from the coast. This trend is well captured by the model (typical low bias of 200 m) although significant errors exist at the coast where the model marine boundary layer is too shallow and moist. Drizzle in the model responds to changes in liquid water path in a manner that is consistent with previous ship-borne observations in the region although the intensity of this drizzle is likely to be too high, particularly in the more polluted coastal region where higher cloud droplet number concentrations are typical. Another mode of variability in the cloud field that the model is unable to capture are regions of pockets of open cellular convection embedded in the overcast stratocumulus deck and an example of such a feature that was sampled during VOCALS-REx is shown.
Aqueous chemistry and its role in secondary organic aerosol (SOA) formation

There is a growing understanding that secondary organic aerosol (SOA) can form through reactions in atmospheric waters (i.e., clouds, fogs, and aerosol water). In clouds and wet aerosols, water-soluble organic products of gas-phase photochemistry dissolve into the aqueous phase where they can react further (e.g., with OH radicals) to form low volatility products that are largely retained in the particle phase. Organic acids, oligomers and other products form via radical and non-radical reactions, including hemiacetal formation during droplet evaporation, acid/base catalysis, and reaction of organics with other constituents (e.g., NH4+). This paper provides an overview of SOA formation through aqueous chemistry, including atmospheric evidence for this process and a review of radical and non-radical chemistry, using glyoxal as a model precursor. Previously unreported analyses and new kinetic modeling are reported herein to support the discussion of radical chemistry. Results suggest that reactions with OH radicals tend to be faster and form more SOA than non-radical reactions. In clouds these reactions yield organic acids, whereas in wet aerosols they yield large multifunctional humic-like substances formed via radical-radical reactions and their O/C ratios are near 1.
Evaluation of various observing systems for the global monitoring of CO2 surface fluxes

In the context of rising greenhouse gas concentrations, and the potential feedbacks between climate and the carbon cycle, there is an urgent need to monitor the exchanges of carbon between the atmosphere and both the ocean and the land surfaces. In the so-called top-down approach, the surface fluxes of CO2 are inverted from the observed spatial and temporal concentration gradients. The concentrations of CO2 are measured in-situ at a number of surface stations unevenly distributed over the Earth while several satellite missions may be used to provide a dense and better-distributed set of observations to complement this network. In this paper, we compare the ability of different CO2 concentration observing systems to constrain surface fluxes. The various systems are based on realistic scenarios of sampling and precision for satellite and in-situ measurements. It is shown that satellite measurements based on the differential absorption technique (such as those of SCIAMACHY, GOSAT or OCO) provide more information than the thermal infrared observations (such as those of AIRS or IASI). The OCO observations will provide significantly better information than those of GOSAT. A CO2 monitoring mission based on an active (lidar) technique could potentially provide an even better constraint. This constraint can also be realized with the very dense surface network that could be built with the same funding as that of the active satellite mission. Despite the large uncertainty reductions on the surface fluxes that may be expected from these various observing systems, these reductions are still insufficient to reach the highly demanding requirements for the monitoring of anthropogenic emissions of CO2 or the oceanic fluxes at a spatial scale smaller than that of oceanic basins. The scientific objective of these observing system should therefore focus on the fluxes linked to vegetation and land ecosystem dynamics.
NOx and O3 above a tropical rainforest: an analysis with a global and box model

A cross-platform field campaign, OP3, was conducted in the state of Sabah in Malaysian Borneo between April and July of 2008. Among the suite of observations recorded, the campaign included measurements of NOx and O3 – crucial outputs of any model chemistry mechanism. We describe the measurements of these species made from both the ground site and aircraft. We then use the output from two resolutions of the chemistry transport model p-TOMCAT to illustrate the ability of a global model chemical mechanism to capture the chemistry at the rainforest site. The basic model performance is good for NOx and poor for ozone. A box model containing the same chemical mechanism is used to explore the results of the global model in more depth and make comparisons between the two. Without some parameterization of the nighttime boundary layer – free troposphere mixing (i.e. the use of a dilution parameter), the box model does not reproduce the observations, pointing to the importance of adequately representing physical processes for comparisons with surface measurements. We conclude with a discussion of box model budget calculations of chemical reaction fluxes, deposition and mixing, and compare these results to output from p-TOMCAT. These show the same chemical mechanism behaves similarly in both models, but that emissions and advection play particularly strong roles in influencing the comparison to surface measurements.
Peroxy radical partitioning during the AMMA radical intercomparison exercise

Peroxy radicals were measured onboard two scientific aircrafts during the AMMA (African Monsoon Multidisciplinary Analysis) campaign in summer 2006. This paper reports results from the flight on 16 August 2006 during which measurements of HO2 by laser induced fluorescence spectroscopy at low pressure (LIF-FAGE) and total peroxy radicals (RO2* = HO2+ΣRO2, R = organic chain) by two similar instruments based on the peroxy radical chemical amplification (PeRCA) technique were subject of a blind intercomparison. The German DLR-Falcon and the British FAAM-BAe-146 flew wing tip to wing tip for about 30 min making concurrent measurements on 2 horizontal level runs at 697 and 485 hPa over the same geographical area in Burkina Faso. A full set of supporting measurements comprising photolysis frequencies, and relevant trace gases like CO, NO, NO2, NOy, O3 and a wider range of VOCs were collected simultaneously. Results are discussed on the basis of the characteristics and limitations of the different instruments used. Generally, no data bias are identified and the RO2* data available agree quite reasonably within the instrumental errors. The [RO2*]/[HO2] ratios, which vary between 1:1 and 3:1, as well as the peroxy radical variability, concur with variations in photolysis rates and in other potential radical precursors. Model results provide additional information about dominant radical formation and loss processes.
Annual variation of methane emissions from forested bogs in West Siberia (2005–2009): a case of high CH4 and precipitation rate in the summer of 2007

We have been conducting continuous measurements of CH4 and CO2 on a network of towers (JR-STATION: Japan–Russia Siberian Tall Tower Inland Observation Network) located in taiga, steppe, and wetland biomes of Siberia. Here we describe measurements from two forested bog sites, Karasevoe (KRS; 58°15′ N, 82°25′ E) and Demyanskoe (DEM; 59°47′ N, 70°52′ E), in West Siberia from 2005 to 2009. Although both CH4 and CO2 accumulation (ΔCH4 and ΔCO2) during nighttime (duration of 7 h beginning 21:30 LST) at KRS in July 2007 showed an anomalously high concentration, the higher ratios of ΔCH4/ΔCO2 compared with those in other years indicate that a considerably more CH4 flux occurred relative to the CO2 flux in response to large precipitation recorded in 2007 (~2.7 mm d−1 higher than the climatological 1979–1998 base). Estimated seasonal CH4 fluxes based on the ratio of ΔCH4/ΔCO2 and the CASA 3-hourly CO2 flux for the 2005–2009 period exhibited a seasonal variation with a maximum in July at both sites. Annual values of the CH4 emission from the forested bogs around KRS (approx. 7.8×104 km2) calculated from a process-based ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT), showed inter-annual variation of 0.54, 0.31, 0.94, 0.44, and 0.41 Tg CH4 yr−1 from 2005 to 2009, respectively, with the highest values in 2007. It was assumed in the model that the area flooded with water is proportional to the cumulative anomaly in monthly precipitation rate.
Seasonal variations of aerosol size distributions based on long-term measurements at the high altitude Himalayan site of Nepal Climate Observatory-Pyramid (5079 m), Nepal

The present paper investigates the diurnal and seasonal variability of the aerosol total number concentration, number and volume size distribution between 10 nm and 10 μm, from a combination of a scanning mobility particle sizer (SMPS) and an optical counter (OPC), performed over a two-year period (January 2006–February 2008) at the Nepal Climate Observatory-Pyramid (NCO-P) research station, (5079 m a.s.l.). The annual average number concentration measured over the two-year period at the NCO-P is 860 cm−3. Total concentrations show a strong seasonality with maxima during pre-monsoon and post-monsoon seasons and minima during the dry and monsoon seasons. A diurnal variation is also clearly observed, with maxima between 09:00 and 12:00 UTC. The aerosol concentration maxima are mainly due to nucleation processes during the post-monsoon season, as witnessed by high nucleation mode integrated number concentrations, and to transport of high levels of pollution from the plains by valley breezes during the pre-monsoon season, as demonstrated by high accumulation mode integrated number concentrations. Night-time number concentration of particles (from 03:00 to 08:00 NST) are relatively low throughout the year (from 450 cm−3 during the monsoon season to 675 cm−3 during the pre-monsoon season), indicating the of high altitudes background level, as a result of downslope winds during this part of the day. However, it was found that these background concentrations are strongly influenced by the daytime concentrations, as they show the same seasonal variability. If nighttime concentrations were presumed to be representative of free troposphere (FT)/residual layer concentrations, they would be found to be two times higher than at other lower altitudes European sites, such as the Jungfraujoch. However, BL intrusions might contaminate the free troposphere/residual layer even at this altitude, especially during regional air masses influence. Night-time measurements were subsequently selected to study the FT composition according to different air masses, and the effect of long range transport to the station.
IASI carbon monoxide validation over the Arctic during POLARCAT spring and summer campaigns

In this paper, we provide a detailed comparison between carbon monoxide (CO) data measured by the Infrared Atmospheric Sounding Interferometer (IASI)/MetOp and aircraft observations over the Arctic. The CO measurements were obtained during North American (NASA ARCTAS and NOAA ARCPAC) and European campaigns (POLARCAT-France, POLARCAT-GRACE and YAK-AEROSIB) as part of the International Polar Year (IPY) POLARCAT activity in spring and summer 2008. During the campaigns different air masses were sampled including clean air, polluted plumes originating from anthropogenic sources in Europe, Asia and North America, and forest fire plumes originating from Siberia and Canada. The paper illustrates that CO-rich plumes following different transport pathways were well captured by the IASI instrument, in particular due to the high spatial coverage of IASI. The comparison between IASI CO total columns, 0–5 km partial columns and profiles with collocated aircraft data was achieved by taking into account the different sensitivity and geometry of the sounding instruments. A detailed analysis is provided and the agreement is discussed in terms of information content and surface properties at the location of the observations. For profiles, the data were found to be in good agreement in spring with differences lower than 17%, whereas in summer the difference can reach 20% for IASI profiles below 8 km for polluted cases. For total columns the correlation coefficients ranged from 0.15 to 0.74 (from 0.47 to 0.77 for partial columns) in spring and from 0.26 to 0.84 (from 0.66 to 0.88 for partial columns) in summer. A better agreement is seen over the sea in spring (0.73 for total column and 0.78 for partial column) and over the land in summer (0.69 for total columns and 0.81 for partial columns). The IASI vertical sensitivity was better over land than over sea, and better over land than over sea ice and snow allowing a higher potential to detect CO vertical distribution during summer.