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We present observations of biomass burning aerosol from the South American Biomass Burning Analysis (SAMBBA) and other measurement campaigns, and use these to evaluate the representation of biomass burning aerosol properties and processes in a state-of-the-art climate model. The evaluation includes detailed comparisons with aircraft and ground data, along with remote sensing observations from MODIS and AERONET. We demonstrate several improvements to aerosol properties following the implementation of the Global Model for Aerosol Processes (GLOMAP-mode) modal aerosol scheme in the HadGEM3 climate model. This predicts the particle size distribution, composition, and optical properties, giving increased accuracy in the representation of aerosol properties and physical–chemical processes over the Coupled Large-scale Aerosol Scheme for Simulations in Climate Models (CLASSIC) bulk aerosol scheme previously used in HadGEM2. Although both models give similar regional distributions of carbonaceous aerosol mass and aerosol optical depth (AOD), GLOMAP-mode is better able to capture the observed size distribution, single scattering albedo, and Ångström exponent across different tropical biomass burning source regions. Both aerosol schemes overestimate the uptake of water compared to recent observations, CLASSIC more so than GLOMAP-mode, leading to a likely overestimation of aerosol scattering, AOD, and single scattering albedo at high relative humidity. Observed aerosol vertical distributions were well captured when biomass burning aerosol emissions were injected uniformly from the surface to 3 km. Finally, good agreement between observed and modelled AOD was gained only after scaling up GFED3 emissions by a factor of 1.6 for CLASSIC and 2.0 for GLOMAP-mode. We attribute this difference in scaling factor mainly to different assumptions for the water uptake and growth of aerosol mass during ageing via oxidation and condensation of organics. We also note that similar agreement with observed AOD could have been achieved with lower scaling factors if the ratio of organic carbon to primary organic matter was increased in the models toward the upper range of observed values. Improved knowledge from measurements is required to reduce uncertainties in emission ratios for black carbon and organic carbon, and the ratio of organic carbon to primary organic matter for primary emissions from biomass burning.
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Atmospheric aerosol is the primary source of cloud condensation nuclei (CCN). The microphysics and chemical composition of aerosols can affect cloud development and the precipitation process. Among studies conducted in Latin America, only a handful have reported the impact of urban aerosol on CCN activation parameters such as activation ratio (AR) and activation diameter (<i>D</i><sub>act</sub>). With over 20 million inhabitants, the Metropolitan Area of São Paulo (MASP) is the largest megacity in South America. To our knowledge, this is the first study to assess the impact that remote sources and new particle formation (NPF) events have on CCN activation properties in a South American megacity. The measurements were conducted in the MASP between August and September 2014. We measured the CCN within the 0.2–1.0 % range of supersaturation, together with particle number concentration (PNC) and particle number distribution (PND), as well as trace-element concentrations and black carbon (BC). NPF events were identified on 35 % of the sampling days. Combining multivariate analysis in the form of positive matrix factorization (PMF) with an aerosol profile from lidar and HYSPLIT model analyses allowed us to identify the main contribution of vehicular traffic on all days and sea salt and biomass burning from remote regions on 28 and 21 % of the sampling days, respectively. The AR and <i>D</i><sub>act</sub> parameters showed distinct patterns for daytime with intense vehicular traffic and nighttime periods. For example, CCN activation was lower during the daytime than during the nighttime periods, a pattern that was found to be associated mainly with local road-traffic emissions. A decrease in CCN activation was observed on the NPF event days, mainly due to high concentrations of particles with smaller diameters. We also found that aerosols from sea salt, industrial emissions, and biomass burning had minor effects on <i>D</i><sub>act</sub>. For example, nights with biomass burning and vehicular emissions showed slightly lower CCN activation properties than sea-salt, industrial and non-event nights. Our results show that particulate matter from local vehicular emissions during the daytime has a greater effect on CCN activation parameters than that from remote sources.
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Increasing wildfire activities in the mountainous western US may present a challenge for the region to attain a recently revised ozone air quality standard in summer. Using current Eulerian chemical transport models to examine the wildfire ozone influences is difficult due to uncertainties in fire emissions, inadequate model chemistry, and resolution. Here we quantify the wildfire influence on the ozone variability, trends, and number of high MDA8 (daily maximum 8 h average) ozone days over this region in summers (June, July, and August) 1989–2010 using a new approach. We define a fire index using retroplumes (plumes of back-trajectory particles) computed by a Lagrangian dispersion model (FLEXPART) and develop statistical models based on the fire index and meteorological parameters to interpret MDA8 ozone concentrations measured at 13 Intermountain West surface sites. We show that the statistical models are able to capture the ozone enhancements by wildfires and give results with some features different from the GEOS-Chem Eulerian chemical transport model. Wildfires enhance the Intermountain West regional summer mean MDA8 ozone by 0.3–1.5 ppbv (daily episodic enhancements reach 10–20 ppbv at individual sites) with large interannual variability, which are strongly correlated with the total MDA8 ozone. We find large fire impacts on the number of exceedance days; for the 13 CASTNet sites, 31 % of the summer days with MDA8 ozone exceeding 70 ppbv would not occur in the absence of wildfires.
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To understand the long-range transport of monocarboxylic acids from the Asian continent to the Japanese islands, we collected snowpack samples from a pit sequence (depth ca. 6 m) at the Murodo-Daira snowfield near the summit of Mt. Tateyama, central Japan, in 2009 and 2011. Snow samples (<i>n</i> = 16) were analyzed for normal (C<sub>1</sub>–C<sub>10</sub>), branched chain (iC<sub>4</sub>–iC<sub>6</sub>), aromatic (benzoic and toluic acid isomers), and hydroxyl (glycolic and lactic) monocarboxylic acids, together with inorganic ions and dissolved organic carbon (DOC). Acetic acid (C<sub>2</sub>) was found to be a dominant species (average 125 ng g<sup>−1</sup>), followed by formic acid (C<sub>1</sub>) (85.7 ng g<sup>−1</sup>) and isopentanoic acid (iC<sub>5</sub>) (20.0 ng g<sup>−1</sup>). We found a strong correlation (<i>r</i> = 0.88) between formic plus acetic acids and non-sea-salt Ca<sup>2+</sup> that is a proxy of Asian dust. Contributions of total monocarboxylic acids to DOC in 2009 (21.2 ± 11.6 %) were higher than that in 2011 (3.75 ± 2.62 %), being consistent with higher intensity of Asian dust in 2009 than in 2011. Formic plus acetic acids also showed a positive correlation (<i>r</i> = 0.90) with benzoic acid that is a tracer of automobile exhaust, indicating that monocarboxylic acids and their precursors are largely emitted from anthropogenic sources in China and/or secondarily produced in the atmosphere by photochemical processing. In addition, the ratio of formic plus acetic acids to nss–Ca<sup>2+</sup> (0.27) was significantly higher than those (0.00036–0.0018) obtained for reference dust materials of Chinese loess deposits from the Tengger and Gobi deserts. This result suggests that volatile and semi-volatile organic acids are adsorbed on the alkaline dust particles during long-range atmospheric transport. Entrainment of organic acids by dusts is supported by a good correlation (<i>r</i> = 0.87) between formic plus acetic acids and pH of melt snow samples. Our study suggests that Asian alkaline dusts may be a carrier of volatile monocarboxylic acids.
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The South Asian High (SAH) is an important component of the summer monsoon system in Asia. In this study we investigate the location and drivers of the SAH at 100 hPa during the boreal summers of 1979 to 2014 on interannual, seasonal and synoptic timescales using seven reanalyses and observational data. Our comparison of the different reanalyses focuses especially on the bimodality of the SAH, i.e. the two preferred modes of the SAH centre location: the Iranian Plateau to the west and the Tibetan Plateau to the east. We find that only the National Centers for Environmental Prediction–National Center of Atmospheric Research (NCEP–NCAR) reanalysis shows a clear bimodal structure of the SAH centre distribution with respect to daily and pentad (5 day) mean data. Furthermore, the distribution of the SAH centre location is highly variable from year to year. As in simple model studies, which connect the SAH to heating in the tropics, we find that the mean seasonal cycle of the SAH and its centre are dominated by the expansion of convection in the South Asian region (70–130° E × 15–30° N) on the south-eastern border of the SAH. A composite analysis of precipitation and outgoing long-wave radiation data with respect to the location of the SAH centre reveals that a more westward (eastward) location of the SAH is related to stronger (weaker) convection and rainfall over India and weaker (stronger) precipitation over the western Pacific.
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To evaluate CO<sub>2</sub> emissions in urban areas and their temporal and spatial variability, continuous measurements of CO<sub>2</sub> fluxes were conducted using the eddy covariance method at three locations in Sakai, Osaka, Japan. Based on the flux footprint at the measurement sites, CO<sub>2</sub> fluxes from the three sites were partitioned into five datasets representing a dense urban center, a moderately urban area, a suburb, an urban park, and a rural area. A distinct biological uptake of CO<sub>2</sub> was observed in the suburb, urban park, and rural areas in the daytime, whereas high emissions were observed in the dense and moderate urban areas in the daytime. Weekday CO<sub>2</sub> emissions in the dense urban center and suburban area were approximately 50 % greater than emissions during weekends and holidays, but the other landscapes did not exhibit a clear weekly cycle. Seasonal variations in the urban park, rural area, and suburban area were influenced by photosynthetic uptake, exhibiting the lowest daily emissions or even uptake during the summer months. In contrast, the dense and moderately urban areas emitted CO<sub>2</sub> in all seasons. CO<sub>2</sub> emissions in the urban areas were high in the winter and summer months, and they significantly increased with the increase in air temperature in the summer and the decrease in air temperature in the winter. Irrespective of the land cover type, all urban landscapes measured in this study acted as net annual CO<sub>2</sub> sources, with emissions ranging from 0.5 to 4.9 kg C m<sup>−2</sup> yr<sup>−1</sup>. The magnitude of the annual CO<sub>2</sub> emissions was negatively correlated with the green fraction; areas with a smaller green fraction had higher annual CO<sub>2</sub> emissions. Upscaled flux estimated based on the green fraction indicated that the emissions for the entire city were 3.3 kg C m<sup>−2</sup> yr<sup>−1</sup>, which is equivalent to 0.5 Tg C yr<sup>−1</sup> or 1.8 Mt CO<sub>2</sub> yr<sup>−1</sup>, based on the area of the city (149.81 km<sup>2</sup>). A network of eddy covariance measurements is useful for characterizing the spatial and temporal variations in net CO<sub>2</sub> fluxes from urban areas. Multiple methods would be required to evaluate the rationale behind the fluxes and overcome the limitations in the future.
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We have observed a number of strong echoes with the European incoherent-scatter (EISCAT) UHF (930-MHz) radar at angles 83.5° and 78.6° with the geomagnetic field and at about 100-km altitude north in the auroral zone. The echoes are short-lived and occur in single 2- or 10-s data dumps. They are offset by 125–130 kHz with respect to the transmitted frequency. In most cases the offset compares well with the frequency of gyro lines in the incoherent-scatter spectrum, as given by the standard linear dispersion relation. But sometimes the measured offsets deviate significantly from the model calculations, and the interpretation in terms of gyro lines becomes questionable. The discrepancy could possibly be explained by local deviations in the magnetic field from the model (IGRF 1987), which are generated by incoming particle beams. A more serious problem with the gyro-line theory is how the line can be excited at altitudes where the collisional damping is substantial. The high intensity and short lifetime of the signal point to a fast-growing plasma instability as the likely excitation mechanism, if the gyro-line interpretation is correct. The cause of the instability could be the same particle beams as those causing the disturbances in the magnetic field. Alternatively, the observations may be interpreted as meteor head echoes. The large Doppler shifts, the short lifetimes and the altitudes of the signals support this explanation. The main difficulty is that the distribution of measured offsets appears to be different in magnetically active conditions and in less active conditions. Also, the occurrence of echoes does not seem to follow the expected changes in meteor density. More observations in different conditions are needed to decide between the two interpretations. As it is, we are inclined to believe in the meteor head echo theory, the objections to the gyro-line theory being more fundamental.
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When travelling through the ionosphere the signals of space-based radio navigation systems such as the Global Positioning System (GPS) are subject to modifications in amplitude, phase and polarization. In particular, phase changes due to refraction lead to propagation errors of up to 50 m for single-frequency GPS users. If both the L1 and the L2 frequencies transmitted by the GPS satellites are measured, first-order range error contributions of the ionosphere can be determined and removed by difference methods. The ionospheric contribution is proportional to the total electron content (TEC) along the ray path between satellite and receiver. Using about ten European GPS receiving stations of the International GPS Service for Geodynamics (IGS), the TEC over Europe is estimated within the geographic ranges -20°≤ λ ≤40°E and 32.5°≤ <i>Φ</i> ≤70°N in longitude and latitude, respectively. The derived TEC maps over Europe contribute to the study of horizontal coupling and transport proces- ses during significant ionospheric events. Due to their comprehensive information about the high-latitude ionosphere, EISCAT observations may help to study the influence of ionospheric phenomena upon propagation errors in GPS navigation systems. Since there are still some accuracy limiting problems to be solved in TEC determination using GPS, data comparison of TEC with vertical electron density profiles derived from EISCAT observations is valuable to enhance the accuracy of propagation-error estimations. This is evident both for absolute TEC calibration as well as for the conversion of ray-path-related observations to vertical TEC. The combination of EISCAT data and GPS-derived TEC data enables a better understanding of large-scale ionospheric processes.
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Near-earth plasma parameters were calculated using a global numerical self-consistent and time-dependent model of the thermosphere, ionosphere and protonosphere (GSM TIP). The model results are compared with experimental data of different origin, mainly EISCAT measurements and simultaneous satellite data (<i>N<sub>e</sub></i> and ion composition). Model runs with varying inputs of auroral FAC distributions, temperature of vibrationally excited nitrogen and photoelectron energy escape fluxes are used to make adjustments to the observations. The satellite data are obtained onboard Active and its subsatellite Magion-2 when they passed nearby the EISCAT station around 0325 and 1540 UT on 31 July 1990 at a height of about 2000 and 2200 km, respectively. A strong geomagnetic disturbance was observed two days before the period under study. Numerical calculations were performed with consideration of vibrationally excited nitrogen molecules for high solar-activity conditions. The results show good agreement between the incoherent-scatter radar measurements (<i>N<sub>e</sub></i>, <i>T<sub>e</sub></i>, <i>T<sub>i</sub></i>) and model calculations, taking into account the excited molecular nitrogen reaction rates. The comparison of model results of the thermospheric neutral wind shows finally a good agreement with the HWM93 empirical wind model.
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A set of EISCAT UHF and VHF observations is used for calibrating a coupled fluid-kinetic model of the ionosphere. The data gathered in the period 1200- 2400 UT on 24 March 1995 had various intervals of interest for such a calibration. The magnetospheric activity was very low during the afternoon, allowing for a proper examination of a case of quiet ionospheric conditions. The radars entered the auroral oval just after 1900 UT: a series of dynamic events probably associated with rapidly moving auroral arcs was observed until after 2200 UT. No attempts were made to model the dynamical behaviour during the 1900–2200 UT period. In contrast, the period 2200–2400 UT was characterised by quite steady precipitation: this latter period was then chosen for calibrating the model during precipitation events. The adjustment of the model on the four primary parameters observed by the radars (namely the electron concentration and temperature and the ion temperature and velocity) needed external inputs (solar fluxes and magnetic activity index) and the adjustments of a neutral atmospheric model in order to reach a good agreement. It is shown that for the quiet ionosphere, only slight adjustments of the neutral atmosphere models are needed. In contrast, adjusting the observations during the precipitation event requires strong departures from the model, both for the atomic oxygen and hydrogen. However, it is argued that this could well be the result of inadequately representing the vibrational states of N<sub>2</sub> during precipitation events, and that these factors have to be considered only as ad hoc corrections.
