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Climatology of free-tropospheric humidity: extension into the SEVIRI era, evaluation and exemplary analysis

A new free-tropospheric humidity (FTH) data record is presented. It is based on observations from the Meteosat Visible and Infrared Imager (MVIRI) onboard Meteosat-2–Meteosat-5, as well as Meteosat-7, and the Spinning Enhanced Visible and Infrared Imager (SEVIRI) onboard Meteosat-8 and Meteosat-9 at the water absorption band near 6.3 μm. The data set is available under clear-sky and low-level cloud conditions. With the extension to SEVIRI observations, the data record covers the period 1983–2009 with a spatial resolution of 0.625° × 0.625° and a temporal resolution of 3 h. The FTH is the mean relative humidity (RH) in a broad layer in the free troposphere. The relation between the observed brightness temperature (BT) and the FTH is well established. Previous retrievals are refined by taking into account the relative humidity Jacobians in the training process of the statistical retrieval. The temporal coverage is extended into the SEVIRI period, the homogenization of the BT record is improved, and the full archive is reprocessed using updated regression coefficients. The FTH estimated from the Meteosat observations is compared to the FTH computed from the RH profiles of the Analyzed RadioSoundings Archive (ARSA). An average relative bias of −3.2% and a relative root-mean-square difference (RMSD) of 16.8% are observed. This relative RMSD agrees with the outcome of an analysis of the total uncertainty of the FTH product. The decadal stability of the FTH data record is 0.5 ± 0.45% per decade. As exemplary applications, the interannual standard deviation, the differences on decadal scales, and the linear trend in the FTH data record and in the frequency of occurrence of FTH < 10% (FTHp10) are analyzed per season. Interannual standard deviation maxima and maxima in absolute decadal differences are featured in gradient areas between dry and wet regions, as well as in areas where FTH reaches minima and FTHp10 reaches maxima. An analysis of the FTH linear trends and of the associated uncertainty estimates is achieved to identify possible problems with the data record. Positive trends in FTHp10 are featured in gradient areas between wet and dry regions, in regions where the FTH is minimum, in regions where FTHp10 is maximum, and in regions where differences between FTHp10 averaged over the 2000s and 1990s are negative. However, these positive trends in FTHp10 are associated with maximum standard deviation and are thus hardly significant. This analysis and intercomparisons with other humidity data records are part of the Global Energy and Water Cycle Experiment (GEWEX) Water Vapor Assessment (G-VAP).
Natural or anthropogenic? On the origin of atmospheric sulfate deposition in the Andes of southeastern Ecuador

Atmospheric sulfur deposition above certain limits can represent a threat to tropical forests, causing nutrient imbalances and mobilizing toxic elements that impact biodiversity and forest productivity. Atmospheric sources of sulfur deposited by precipitation have been roughly identified in only a few lowland tropical forests. Even scarcer are studies of this type in tropical mountain forests, many of them mega-diversity hotspots and especially vulnerable to acidic deposition. In these places, the topographic complexity and related streamflow conditions affect the origin, type, and intensity of deposition. Furthermore, in regions with a variety of natural and anthropogenic sulfur sources, like active volcanoes and biomass burning, no source emission data has been used for determining the contribution of each source to the deposition. The main goal of the current study is to evaluate sulfate (SO4- deposition by rain and occult precipitation at two topographic locations in a tropical mountain forest of southern Ecuador, and to trace back the deposition to possible emission sources applying back-trajectory modeling. To link upwind natural (volcanic) and anthropogenic (urban/industrial and biomass-burning) sulfur emissions and observed sulfate deposition, we employed state-of-the-art inventory and satellite data, including volcanic passive degassing as well. We conclude that biomass-burning sources generally dominate sulfate deposition at the evaluated sites. Minor sulfate transport occurs during the shifting of the predominant winds to the north and west. Occult precipitation sulfate deposition and likely rain sulfate deposition are mainly linked to biomass-burning emissions from the Amazon lowlands. Volcanic and anthropogenic emissions from the north and west contribute to occult precipitation sulfate deposition at the mountain crest Cerro del Consuelo meteorological station and to rain-deposited sulfate at the upriver mountain pass El Tiro meteorological station.
New emission factors for Australian vegetation fires measured using open-path Fourier transform infrared spectroscopy – Part 2: Australian tropical savanna fires

Savanna fires contribute approximately 40–50% of total global annual biomass burning carbon emissions. Recent comparisons of emission factors from different savanna regions have highlighted the need for a regional approach to emission factor development, and better assessment of the drivers of the temporal and spatial variation in emission factors. This paper describes the results of open-path Fourier transform infrared (OP-FTIR) spectroscopic field measurements at 21 fires occurring in the tropical savannas of the Northern~Territory, Australia, within different vegetation assemblages and at different stages of the dry season. Spectra of infrared light passing through a long (22–70 m) open-path through ground-level smoke released from these fires were collected using an infrared lamp and a field-portable FTIR system. The IR spectra were used to retrieve the mole fractions of 14 different gases present within the smoke, and these measurements used to calculate the emission ratios and emission factors of the various gases emitted by the burning. Only a handful of previous emission factor measures are available specifically for the tropical savannas of Australia and here we present the first reported emission factors for methanol, acetic acid, and formic acid for this biome. Given the relatively large sample size, it was possible to study the potential causes of the within-biome variation of the derived emission factors. We find that the emission factors vary substantially between different savanna vegetation assemblages; with a majority of this variation being mirrored by variations in the modified combustion efficiency (MCE) of different vegetation classes. We conclude that a significant majority of the variation in the emission factor for trace gases can be explained by MCE, irrespective of vegetation class, as illustrated by variations in the calculated methane emission factor for different vegetation classes using data sub-set by different combustion efficiencies. Therefore, the selection of emission factors for emissions modelling purposes need not necessarily require detailed fuel type information, if data on MCE (e.g. from future spaceborne total column measurements) or a correlated variable were available. From measurements at 21 fires, we recommend the following emission factors for Australian tropical savanna fires (in grams of gas emitted per kilogram of dry fuel burned), which are our mean measured values: 1674 ± 56 g kg−1 of carbon dioxide; 87 ± 33 g kg−1 of carbon monoxide; 2.1 ± 1.2 g kg−1 of methane; 0.11 ± 0.04 g kg−1 of acetylene; 0.49 ± 0.22 g kg−1 of ethylene; 0.08 ± 0.05 g kg−1 of ethane; 1.57 ± 0.44 g kg−1 of formaldehyde; 1.06 ± 0.87 g kg−1 of methanol; 1.54 ± 0.64 g kg−1 of acetic acid; 0.16 ± 0.07 g kg−1 of formic acid; 0.53 ± 0.31 g kg−1 of hydrogen cyanide; and 0.70 ± 0.36 g kg−1 of ammonia. In a companion paper, similar techniques are used to characterise the emissions from Australian temperate forest fires.
New emission factors for Australian vegetation fires measured using open-path Fourier transform infrared spectroscopy – Part 1: Methods and Australian temperate forest fires

Biomass burning releases trace gases and aerosol particles that significantly affect the composition and chemistry of the atmosphere. Australia contributes approximately 8% of gross global carbon emissions from biomass burning, yet there are few previous measurements of emissions from Australian forest fires available in the literature. This paper describes the results of field measurements of trace gases emitted during hazard reduction burns in Australian temperate forests using open-path Fourier transform infrared spectroscopy. In a companion paper, similar techniques are used to characterise the emissions from hazard reduction burns in the savanna regions of the Northern Territory. Details of the experimental methods are explained, including both the measurement set-up and the analysis techniques employed. The advantages and disadvantages of different ways to estimate whole-fire emission factors are discussed and a measurement uncertainty budget is developed. Emission factors for Australian temperate forest fires are measured locally for the first time for many trace gases. Where ecosystem-relevant data are required, we recommend the following emission factors for Australian temperate forest fires (in grams of gas emitted per kilogram of dry fuel burned) which are our mean measured values: 1620 ± 160 g kg−1 of carbon dioxide; 120 ± 20 g kg−1 of carbon monoxide; 3.6 ± 1.1 g kg−1 of methane; 1.3 ± 0.3 g kg−1 of ethylene; 1.7 ± 0.4 g kg−1 of formaldehyde; 2.4 ± 1.2 g kg−1 of methanol; 3.8 ± 1.3 g kg−1 of acetic acid; 0.4 ± 0.2 g kg−1 of formic acid; 1.6 ± 0.6 g kg−1 of ammonia; 0.15 ± 0.09 g kg−1 of nitrous oxide and 0.5 ± 0.2 g kg−1 of ethane.
Constraining mass–diameter relations from hydrometeor images and cloud radar reflectivities in tropical continental and oceanic convective anvils

In this study the density of ice hydrometeors in tropical clouds is derived from a combined analysis of particle images from 2-D-array probes and associated reflectivities measured with a Doppler cloud radar on the same research aircraft. Usually, the mass–diameter m(D) relationship is formulated as a power law with two unknown coefficients (pre-factor, exponent) that need to be constrained from complementary information on hydrometeors, where absolute ice density measurement methods do not apply. Here, at first an extended theoretical study of numerous hydrometeor shapes simulated in 3-D and arbitrarily projected on a 2-D plan allowed to constrain the exponent βof the m(D) relationship from the exponent σ of the surface–diameterS(D)relationship, which is likewise written as a power law. Since S(D) always can be determined for real data from 2-D optical array probes or other particle imagers, the evolution of the m(D) exponent can be calculated. After that, the pre-factor α of m(D) is constrained from theoretical simulations of the radar reflectivities matching the measured reflectivities along the aircraft trajectory. The study was performed as part of the Megha-Tropiques satellite project, where two types of mesoscale convective systems (MCS) were investigated: (i) above the African continent and (ii) above the Indian Ocean. For the two data sets, two parameterizations are derived to calculate the vertical variability of m(D) coefficients α and β as a function of the temperature. Originally calculated (with T-matrix) and also subsequently parameterized m(D) relationships from this study are compared to other methods (from literature) of calculating m(D) in tropical convection. The significant benefit of using variable m(D) relations instead of a single m(D) relationship is demonstrated from the impact of all these m(D) relations on Z-CWC (Condensed Water Content) and Z-CWC-T-fitted parameterizations.
Impacts of new particle formation on aerosol cloud condensation nuclei (CCN) activity in Shanghai: case study

New particle formation (NPF) events and their impacts on cloud condensation nuclei (CCN) were investigated using continuous measurements collected in urban Shanghai from 1 to 30 April 2012. During the campaign, NPF occurred in 8 out of the 30 days and enhanced CCN number concentration (NCCN) by a factor of 1.2–1.8, depending on supersaturation (SS). The NPF event on 3 April 2012 was chosen as an example to investigate the NPF influence on CCN activity. In this NPF event, secondary aerosols were produced continuously and increased PM2.5 mass concentration at a rate of 4.33 μg cm−3 h−1, and the growth rate (GR) and formation rate (FR) were on average 5 nm h−1 and 0.36 cm−3 s−1, respectively. The newly formed particles grew quickly from nucleation mode (10–20 nm) into CCN size range. NCCN increased rapidly at SS of 0.4–1.0% but weakly at SS of 0.2%. Correspondingly, aerosol CCN activities (fractions of activated aerosol particles in total aerosols, NCCN/NCN) were significantly enhanced from 0.24–0.60 to 0.30–0.91 at SS of 0.2–1.0% due to the NPF. On the basis of the κ-Köhler theory, aerosol size distributions and chemical composition measured simultaneously were used to predict NCCN. There was a good agreement between the predicted and measured NCCN (R2=0.96, Npredicted/Nmeasured=1.04). This study reveals that NPF exerts large impacts on aerosol particle abundance and size spectra; thus, it significantly promotes NCCN and aerosol CCN activity in this urban environment. The GR of NPF is the key factor controlling the newly formed particles to become CCN at all SS levels, whereas the FR is an effective factor only under high SS (e.g., 1.0%) conditions.
Airborne observations of IEPOX-derived isoprene SOA in the Amazon during SAMBBA

Isoprene is a potentially highly significant but currently poorly quantified source of secondary organic aerosols (SOA). This is especially important in the tropics, where large rainforests act as significant sources of isoprene. Methylfuran, produced through thermal decomposition during analysis, has recently been suggested as a marker for isoprene SOA formation through the isoprene epoxydiol (IEPOX) route, which mostly occurs under low NOx conditions. This is manifested as a peak at m/z=82 in Aerodyne Aerosol Mass Spectrometer (AMS) data. Here we present a study of this marker measured during five flights over the Amazon rainforest on board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft during the South American Biomass Burning Analysis (SAMBBA) campaign. Cases where this marker is and is not present are contrasted and linked to the presence of acidic seed particles, lower NOx concentrations and higher humidities. There are also data to suggest a role of organic nitrogen in the particulate composition. Furthermore, an inspection of the vertical trends of the marker indicates that concentrations are highest at the top of the boundary layer (possibly due to semivolatile repartitioning) and that upwards through the free troposphere, the mass spectral profile evolves towards that of low volatility oxygenated aerosol. These observations offer insights into the behaviour of IEPOX-derived SOA formation above the Amazon rainforest and the suitability of methylfuran as a marker for this process.
Impact of the Asian monsoon anticyclone on the variability of mid-to-upper tropospheric methane above the Mediterranean Basin

The space and time variabilities of methane (CH4) total column and upper tropospheric mixing ratios are analysed above the Mediterranean Basin (MB) as part of the Chemical and Aerosol Mediterranean Experiment (ChArMEx) programme. Since the analysis of the mid-to-upper tropospheric CH4 distribution from spaceborne sensors and model outputs is challenging, we have adopted a climatological approach and have used a wide variety of data sets. We have combined spaceborne measurements from the Thermal And Near infrared Sensor for carbon Observations – Fourier Transform Spectrometer (TANSO-FTS) instrument on the Greenhouse gases Observing SATellite (GOSAT) satellite, the Atmospheric InfraRed Spectrometer (AIRS) on the AURA platform and the Infrared Atmospheric Sounder Interferometer (IASI) instrument aboard the MetOp-A platform with model results from the Chemical Transport Model (CTM) MOCAGE, and the Chemical Climate Models (CCMs) CNRM-AOCCM and LMDz-OR-INCA (according to different emission scenarios). In order to minimize systematic errors in the spaceborne measurements, we have only considered maritime pixels over the MB. The period of interest spans from 2008 to 2011 considering satellite and MOCAGE data and, regarding the CCMs, from 2001 to 2010. Although CH4 is a long-lived tracer with lifetime of ~12 years and is supposed to be well mixed in the troposphere, an east–west gradient in CH4 is observed and modelled in the mid-to-upper troposphere with a maximum in the Western MB in all seasons except in summer when CH4 accumulates above the Eastern MB. The peak-to-peak amplitude of the east–west seasonal variation in CH4 above the MB in the upper troposphere (300 hPa) is weak but almost twice as great in the satellite measurements (~25 ppbv) as in the model data (~15 ppbv). The maximum of CH4 in summer above the eastern MB can be explained by a series of dynamical processes only occurring in summer. The Asian monsoon traps and uplifts high amounts of CH4 to the upper troposphere where they build up. The Asian Monsoon Anticyclone redistributes these elevated CH4 amounts towards North Africa and the Middle East to finally reach and descend in the eastern MB. In the lower troposphere, the CH4 variability is mainly driven by the local sources of emission in the vicinity of the MB.
The effect of low solubility organic acids on the hygroscopicity of sodium halide aerosols

In order to accurately assess the influence of fatty acids on the hygroscopic and other physicochemical properties of sea salt aerosols, hexanoic, octanoic or lauric acid together with sodium halide salts (NaCl, NaBr and NaI) have been chosen to be investigated in this study. The hygroscopic properties of sodium halide sub-micrometre particles covered with organic acids have been examined by Fourier-transform infrared spectroscopy in an aerosol flow cell. Covered particles were generated by flowing atomized sodium halide particles (either dry or aqueous) through a heated oven containing the gaseous acid. The obtained results indicate that gaseous organic acids easily nucleate onto dry and aqueous sodium halide particles. On the other hand, scanning electron microscopy (SEM) images indicate that lauric acid coating on NaCl particles makes them to aggregate in small clusters. The hygroscopic behaviour of covered sodium halide particles in deliquescence mode shows different features with the exchange of the halide ion, whereas the organic surfactant has little effect in NaBr particles, NaCl and NaI covered particles experience appreciable shifts in their deliquescence relative humidities, with different trends observed for each of the acids studied. In efflorescence mode, the overall effect of the organic covering is to retard the loss of water in the particles. It has been observed that the presence of gaseous water in heterogeneously nucleated particles tends to displace the cover of hexanoic acid to energetically stabilize the system.
Simulating black carbon and dust and their radiative forcing in seasonal snow: a case study over North China with field campaign measurements

A state-of-the-art regional model, the Weather Research and Forecasting (WRF) model (Skamarock et al., 2008) coupled with a chemistry component (Chem) (Grell et al., 2005), is coupled with the snow, ice, and aerosol radiative (SNICAR) model that includes the most sophisticated representation of snow metamorphism processes available for climate study. The coupled model is used to simulate black carbon (BC) and dust concentrations and their radiative forcing in seasonal snow over North China in January–February of 2010, with extensive field measurements used to evaluate the model performance. In general, the model simulated spatial variability of BC and dust mass concentrations in the top snow layer (hereafter BCS and DSTS, respectively) are consistent with observations. The model generally moderately underestimates BCS in the clean regions but significantly overestimates BCS in some polluted regions. Most model results fall within the uncertainty ranges of observations. The simulated BCS and DSTS are highest with > 5000 ng g−1 and up to 5 mg g−1, respectively, over the source regions and reduce to < 50 ng g−1 and < 1 μg g−1, respectively, in the remote regions. BCS and DSTS introduce a similar magnitude of radiative warming (~ 10 W m−2) in the snowpack, which is comparable to the magnitude of surface radiative cooling due to BC and dust in the atmosphere. This study represents an effort in using a regional modeling framework to simulate BC and dust and their direct radiative forcing in snowpack. Although a variety of observational data sets have been used to attribute model biases, some uncertainties in the results remain, which highlights the need for more observations, particularly concurrent measurements of atmospheric and snow aerosols and the deposition fluxes of aerosols, in future campaigns.