ALBERT

Description: Meteorological conditions may drive relationships between aerosol and cloud-related properties. It is important to account for the meteorological contribution to observed cloud–aerosol relationships in order to improve understanding of aerosol–cloud–climate interactions. A new method of investigating the contribution of meteorological covariation to observed cloud–aerosol relationships is introduced. Other studies have investigated the contribution of local meteorology to cloud–aerosol relationships. In this paper, a complimentary large-scale view is presented. Extratropical cyclones have been previously shown to affect satellite-retrieved aerosol optical depth (τ), due to enhanced emission of sea salt and sea surface brightness artefacts in regions of higher wind speed. Extratropical cyclones have also been shown to affect cloud-related properties such as cloud fraction (fc) and cloud top temperature (Ttop). Therefore, it seems plausible to hypothesise that extratropical cyclones may drive relationships between cloud-related properties and τ. In this paper, this hypothesis is investigated for extratropical cyclones, henceforth referred to as storms, over the Atlantic Ocean. MODerate resolution Imaging Spectroradiometer (MODIS) retrieved τ, fc and Ttop data are analysed using a storm-centric coordinate system centred on extratropical cyclones which have been tracked using European Centre for Medium Range Weather Forecasts (ECMWF) reanalysis 850 hPa relative vorticity data. The tracked relative vorticity (ω) is used as a measure of storm strength, while position in the storm-centric domain is used to account for storm structure. Relationships between the cloud-related properties and τ are measured by calculating regression slopes and correlations. The fc–τ relationships are positive, while the Ttop–τ relationships are negative. By shuffling the pairing of the cloud and τ data at each location in the storm-centric domain and within narrow ω bins, the contribution of storm strength and storm structure to the observed relationships can be investigated. It is found that storm strength and storm structure can explain only a small component of the relationships observed in the MODIS data. The primary causes for observed cloud–aerosol relationships are likely to be other factors such as retrieval errors, local meteorology or aerosol–cloud interactions.

Description: We performed MAX-DOAS measurements during the PRIDE-PRD2006 campaign in the Pearl River Delta region (PRD), China, for 4 weeks in July 2006 at a site located 60 km north of Guangzhou. The vertical distributions of NO2, HCHO, and CHOCHO were independently retrieved by an automated iteration method. The NO2 mixing ratios measured by MAX-DOAS showed reasonable agreement with the simultaneous, ground based in-situ data. The tropospheric NO2 vertical column densities (VCDs) observed by OMI on board EOS-Aura satellite were higher than with those by MAX-DOAS. The 3-D chemical transport model CMAQ overestimated the NO2 VCDs as well as the surface concentrations by about 65%. From this observation, a reduction of NOx emission strength in CMAQ seems to be necessary in order to well reproduce the NO2 observations. The average mixing ratios of HCHO and CHOCHO were 7 ppb and 0.4 ppb, respectively, higher than in other rural or semirural environments. The high ratio of 0.062 between CHOCHO and HCHO corresponds to the high VOCs reactivity and high HOx turnover rate consistent with other observations during the campaign.

Description: Strong positive relationships between cloud fraction (fc) and aerosol optical depth (τ) have been reported. Data retrieved from the MODerate resolution Imaging Spectroradiometer (MODIS) instrument show positive fc–τ relationships across most of the globe. A global mean fc increase of approximately 0.2 between low and high τ conditions is found for both ocean and land. However, these relationships are not necessarily due to cloud–aerosol interactions. Using state-of-the-art Monitoring Atmospheric Composition and Climate (MACC) reanalysis-forecast τ data, which should be less affected by retrieval artefacts, it is demonstrated that a large part of the observed fc–τ signal may be due to cloud contamination of satellite-retrieved τ. For longer MACC forecast time steps of 24 h, which likely contain less cloud contamination, some negative fc–τ relationships are found. The global mean fc increase between low and high τ conditions is reduced to 0.1, suggesting that cloud contamination may account for approximately one half of the satellite-retrieved increase in fc. ECHAM5-HAM general circulation model (GCM) simulations further demonstrate that positive fc–τ relationships may arise due to covariation with relative humidity. Widespread negative simulated fc–τ relationships in the tropics are shown to arise due to scavenging of aerosol by convective precipitation. Wet scavenging events are likely poorly sampled in satellite-retrieved data, because the properties of aerosol below clouds cannot be retrieved. Quantifying the role of wet scavenging, and assessing GCM representations of this important process, remains a challenge for future observational studies of aerosol–cloud–precipitation interactions.

Description: Ground-based measurements of scattered sunlight by the Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) have been carried out at an urban site (39.95° N, 116.32° E) in Beijing megacity since 6 August 2008. In this study, we retrieved the tropospheric NO2 vertical column densities (VCDs) over Beijing from these MAX-DOAS observations from August 2008 to September 2011. Over this period, the daytime (08:00–17:00 Beijing Time (BJT, which equals UTC + 8)) mean tropospheric NO2 VCDs varied from 0.5 to 13.3 with an average of 3.6 during summertime, and from 0.2 to 16.8 with an average of 5.8 during wintertime, all in units of 1016 molecules cm−2. The average diurnal variation patterns of tropospheric NO2 over Beijing appeared to be rather different from one season to another, indicating differences in the emission strength and atmospheric lifetime. In contrast to previous studies, we find a small weekly cycle of the tropospheric NO2 VCD over Beijing. The NO2 VCD in the late afternoon was the largest on Saturday and the lowest on Sunday, and in the morning it reached a clear maximum on Wednesday. We also find a post-Olympic Games effect, with 39–54% decrease in the tropospheric NO2 VCD over Beijing estimated for August of 2008, compared to the following years. The tropospheric NO2 VCDs derived by our ground MAX-DOAS measurements show a good correlation with SCIAMACHY and OMI satellite data. However, compared with the MAX-DOAS measurements, the satellite observations underestimate the tropospheric NO2 VCDs over Beijing systematically, by 43% for SCIAMACHY and 26–38% for OMI (DOMINO v2.0 and DOMINO v1.02). Based on radiative transfer simulations, we show that the aerosol shielding effect can explain this underestimation, while the gradient smoothing effect caused by the coarse spatial resolution of the satellite observations could play an additional role.

Description: It has become possible to retrieve the global, long-term trends of trace gases that are important to atmospheric chemistry, climate, and air quality from satellite data records that span more than a decade. However, many of the satellite remote sensing techniques produce measurements that have variable sensitivity to the vertical profiles of atmospheric gases. In the case of constrained retrievals like optimal estimation, this leads to a varying amount of a priori information in the retrieval and is represented by an averaging kernel (AK). In this study, we investigate to what extent the estimation of trends from retrieved data can be biased by temporal changes of averaging kernels used in the retrieval algorithm. In particular, the surface carbon monoxide data retrieved from the Measurements Of Pollution In The Troposphere (MOPITT) instrument from 2001 to 2010 were analyzed. As a practical example based on the MOPITT data, we show that if the true atmospheric mixing ratio is continuously 50% higher or lower than the a priori state, the temporal change of the averaging kernel at the surface level gives rise to an artificial trend in retrieved surface carbon monoxide, ranging from −10.71 to +13.21 ppbv yr−1 (−5.68 to +8.84 % yr−1) depending on location. Therefore, in the case of surface (or near-surface level) CO derived from MOPITT, the AKs trends multiplied by the difference between true and a priori states must be quantified in order to estimate trend biases.

Description: During recent years, volcanic emissions turned out to be a natural source of bromine compounds in the atmosphere. While the initial formation process of bromine monoxide (BrO) has been successfully studied in local ground-based measurements at quiescent degassing volcanoes worldwide, literature on the chemical evolution of BrO on large spatial and temporal scales is sparse. The first space-based observation of a volcanic BrO plume following the Kasatochi eruption in 2008 demonstrated the capability of satellite instruments to monitor such events on a global scale. In this study, we systematically examined GOME-2 observations from January 2007 until June 2011 for significantly enhanced BrO slant column densities (SCDs) in the vicinity of volcanic plumes. In total, 772 plumes from at least 37 volcanoes have been found by using sulphur dioxide (SO2) as a tracer for a volcanic plume. All captured SO2 plumes were subsequently analysed for a simultaneous enhancement of BrO and the data were checked for a possible spatial correlation between the two species. Additionally, the mean BrO/SO2 ratios for all volcanic plumes have been calculated by the application of a bivariate linear fit. A total number of 64 volcanic plumes from at least 11 different volcanoes showed clear evidence for BrO of volcanic origin, revealing large differences in the BrO/SO2 ratios (ranging from some 10−5 to several 10−4) and the spatial distribution of both species. A close correlation between SO2 and BrO occurred only for some of the observed eruptions or just in certain parts of the examined plumes. For other cases, only a rough spatial relationship was found. We discuss possible explanations for the occurrence of the different spatial SO2 and BrO distributions in aged volcanic plumes.

Description: It is now possible to monitor the global and long-term trends of trace gases that are important to atmospheric chemistry, climate, and air quality with satellite data records that span more than a decade. However, many of the remote sensing techniques used by satellite instruments produce measurements that have variable sensitivity to the vertical profiles of atmospheric gases. In the case of constrained retrievals like optimal estimation, this leads to a varying amount of a priori information in the retrieval and is represented by an averaging kernel. In this study, we investigate to what extent such trends can be biased by temporal changes of averaging kernels used in the retrieval algorithm. In particular, the surface carbon monoxide data retrieved from the Measurements Of Pollution In The Troposphere (MOPITT) instrument from 2001 to 2010 were analysed. As a practical example based on the MOPITT data, we show that if the true atmospheric mixing ratio is continuously 50% higher or lower than the a priori state, the temporal change of the averaging kernel at the surface level gives rise to an artificial trend in retrieved surface carbon monoxide, ranging from −10.71 to +13.21 ppbv yr−1 (−5.68 to +8.84% yr−1) depending on location. Therefore, in the case of surface (or near-surface level) CO derived from MOPITT, the AKs trends multiplied by the difference between true and a priori states must be quantified in order to estimate trend biases.

Description: The CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory measures once per month the chemical composition at cruise altitude (10...12 km) during 4 consecutive Lufthansa flights. Here we present a case study of enhanced nitrogen oxides (NOx), nitrous acid (HONO), and formaldehyde (HCHO) in a thunderstorm cloud over the Caribbean islands of Guadeloupe in August 2011. Nitrous acid is an important reservoir gas for OH radicals, and only few observations of HONO at cruise altitude exist. CARIBIC is designed as a long period atmospheric observation system, the actual system has been flying almost monthly since 8 yr now. During this period only very few similar events (one since 2008) were observed. Due to multiple scattering the light path inside clouds is enhanced, thereby lowering the detection limit of the DOAS instrument. Under background conditions the detection limits are 46 ppt for HONO, 387 ppt for chem{HCHO}, and 100 ppt for NO2 and are roughly three times lower inside the cloud. Based on radiative transfer simulations we estimate the path length to 90{ldots}100 km and the cloud top height to ≈15 km. The inferred mixing ratios of HONO, HCHO and NO2 are 37 ppt, 400 ppt and 170 ppt, respectively. Bromine monoxide (BrO) remained below the detection limit of 1 ppt. Because the uplifted air masses originated from the remote marine boundary layer and lightning was observed in the area by the World Wide Lightning Location Network several hours prior to the measurement, the NO (≈1.5 ppb) enhancement was in all likelihood caused by lightning. The main source for the observed HCHO is probably updraught from the boundary layer, because the chemical formation of formaldehyde due to methane oxidation is too weak. Besides HCHO also CH3OOH and isoprene are considered as precursors. The chemical box model CAABA is used to estimate the chem{NO} and HCHO source strengths, which are necessary to explain our measurements. For NO a source strength of 8.25 × 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 a lightning emission of 4.2 × 1025 NO molec/flash. The HCHO updraught is of the order of 121 × 109 molec cm−2 s−1 km−1. Also isoprene and CH3OOH as possible HCHO sources were studied and similar source strengths were found.

Description: We apply a cloud slicing technique (CST), originally developed for Total Ozone Mapping Spectrometer (TOMS) ozone observations, to CO vertical column densities retrieved from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). CST makes use of the shielding effect of clouds and combines trace gas column measurements of cloudy pixels with different cloud heights to retrieve fractional columns aloft. Here we determine seasonal mean tropospheric CO profiles at a vertical resolution of 1 km, which is much finer than what can be obtained from thermal IR instruments. However, since both the atmospheric CO profiles and the effective cloud heights depend systematically on meteorology, the profiles retrieved from the CST have to be interpreted with care. We compare the seasonal mean SCIAMACHY CO profiles with the output from two atmospheric models sampled in the same way as the satellite observations. We find systematic differences both in the absolute values and vertical and horizontal gradients. The results indicate that vertical (re)distributions of emissions and their strengths are not well represented in the models. It seems likely that deep convective transport is underestimated.