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Aerosol measurements during COPE: composition, size, and sources of CCN and INPs at the interface between marine and terrestrial influences

Heavy rainfall from convective clouds can lead to devastating flash flooding, and observations of aerosols and clouds are required to improve cloud parameterisations used in precipitation forecasts. We present measurements of boundary layer aerosol concentration, size, and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation-mode aerosol mass loadings were typically 2–3 µg m−3 (corrected to standard cubic metres at 1013.25 hPa and 273.15 K), the majority of which was sulfuric acid over the sea, or ammonium sulfate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ∼  150–280 cm−3 at 0.1 % and 400–500 cm−3 at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100 to 500 cm−3. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulfate, meaning marine sulfate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to previous measurements of sea spray OA and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulfate, and black carbon. The CCN concentrations here were around 6 times higher than in the clean cases, and the cloud drop number concentrations were 3–4 times higher. Sources of ice-nucleating particles (INPs) were assessed by comparing different parameterisations used to predict INP concentrations, using measured aerosol concentrations as input. The parameterisations based on total aerosol produced INP concentrations that agreed within an order of magnitude with measured first ice concentrations at cloud temperatures as low as −12 °C. Composition-specific parameterisations for mineral dust, fluorescent particles, and sea spray OA were 3–4 orders of magnitude lower than the measured first ice concentrations, meaning a source of INPs was present that was not characterised by our measurements and/or one or more of the composition-specific parameterisations greatly underestimated INPs in this environment.
The Zugspitze radiative closure experiment for quantifying water vapor absorption over the terrestrial and solar infrared – Part 1: Setup, uncertainty analysis, and assessment of far-infrared water vapor continuum

Quantitative knowledge of water vapor radiative processes in the atmosphere throughout the terrestrial and solar infrared spectrum is still incomplete even though this is crucial input to the radiation codes forming the core of both remote sensing methods and climate simulations. Beside laboratory spectroscopy, ground-based remote sensing field studies in the context of so-called radiative closure experiments are a powerful approach because this is the only way to quantify water absorption under cold atmospheric conditions. For this purpose, we have set up at the Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.) a long-term radiative closure experiment designed to cover the infrared spectrum between 400 and 7800 cm−1 (1.28–25 µm). As a benefit for such experiments, the atmospheric states at the Zugspitze frequently comprise very low integrated water vapor (IWV; minimum  =  0.1 mm, median  =  2.3 mm) and very low aerosol optical depth (AOD  =  0.0024–0.0032 at 7800 cm−1 at air mass 1). All instruments for radiance measurements and atmospheric-state measurements are described along with their measurement uncertainties. Based on all parameter uncertainties and the corresponding radiance Jacobians, a systematic residual radiance uncertainty budget has been set up to characterize the sensitivity of the radiative closure over the whole infrared spectral range. The dominant uncertainty contribution in the spectral windows used for far-infrared (FIR) continuum quantification is from IWV uncertainties, while T profile uncertainties dominate in the mid-infrared (MIR). Uncertainty contributions to near-infrared (NIR) radiance residuals are dominated by water vapor line parameters in the vicinity of the strong water vapor bands. The window regions in between these bands are dominated by solar Fourier transform infrared (FTIR) calibration uncertainties at low NIR wavenumbers, while uncertainties due to AOD become an increasing and dominant contribution towards higher NIR wavenumbers. Exceptions are methane or nitrous oxide bands in the NIR, where the associated line parameter uncertainties dominate the overall uncertainty. As a first demonstration of the Zugspitze closure experiment, a water vapor continuum quantification in the FIR spectral region (400–580 cm−1) has been performed. The resulting FIR foreign-continuum coefficients are consistent with the MT_CKD 2.5.2 continuum model and also agree with the most recent atmospheric closure study carried out in Antarctica. Results from the first determination of the NIR water vapor continuum in a field experiment are detailed in a companion paper (Reichert and Sussmann, 2016) while a novel NIR calibration scheme for the underlying FTIR measurements of incoming solar radiance is presented in another companion paper (Reichert et al., 2016).
Field measurements of trace gases and aerosols emitted by peat fires in Central Kalimantan, Indonesia, during the 2015 El Niño

Peat fires in Southeast Asia have become a major annual source of trace gases and particles to the regional–global atmosphere. The assessment of their influence on atmospheric chemistry, climate, air quality, and health has been uncertain partly due to a lack of field measurements of the smoke characteristics. During the strong 2015 El Niño event we deployed a mobile smoke sampling team in the Indonesian province of Central Kalimantan on the island of Borneo and made the first, or rare, field measurements of trace gases, aerosol optical properties, and aerosol mass emissions for authentic peat fires burning at various depths in different peat types. This paper reports the trace gas and aerosol measurements obtained by Fourier transform infrared spectroscopy, whole air sampling, photoacoustic extinctiometers (405 and 870 nm), and a small subset of the data from analyses of particulate filters. The trace gas measurements provide emission factors (EFs; grams of a compound per kilogram biomass burned) for up to ∼  90 gases, including CO2, CO, CH4, non-methane hydrocarbons up to C10, 15 oxygenated organic compounds, NH3, HCN, NOx, OCS, HCl, etc. The modified combustion efficiency (MCE) of the smoke sources ranged from 0.693 to 0.835 with an average of 0.772 ± 0.053 (n  =  35), indicating essentially pure smoldering combustion, and the emissions were not initially strongly lofted. The major trace gas emissions by mass (EF as g kg−1) were carbon dioxide (1564 ± 77), carbon monoxide (291 ± 49), methane (9.51 ± 4.74), hydrogen cyanide (5.75 ± 1.60), acetic acid (3.89 ± 1.65), ammonia (2.86 ± 1.00), methanol (2.14 ± 1.22), ethane (1.52 ± 0.66), dihydrogen (1.22 ± 1.01), propylene (1.07 ± 0.53), propane (0.989 ± 0.644), ethylene (0.961 ± 0.528), benzene (0.954 ± 0.394), formaldehyde (0.867 ± 0.479), hydroxyacetone (0.860 ± 0.433), furan (0.772 ± 0.035), acetaldehyde (0.697 ± 0.460), and acetone (0.691 ± 0.356). These field data support significant revision of the EFs for CO2 (−8 %), CH4 (−55 %), NH3 (−86 %), CO (+39 %), and other gases compared with widely used recommendations for tropical peat fires based on a lab study of a single sample published in 2003. BTEX compounds (benzene, toluene, ethylbenzene, xylenes) are important air toxics and aerosol precursors and were emitted in total at 1.5 ± 0.6 g kg−1. Formaldehyde is probably the air toxic gas most likely to cause local exposures that exceed recommended levels. The field results from Kalimantan were in reasonable agreement with recent lab measurements of smoldering Kalimantan peat for “overlap species,” lending importance to the lab finding that burning peat produces large emissions of acetamide, acrolein, methylglyoxal, etc., which were not measurable in the field with the deployed equipment and implying value in continued similar efforts. The aerosol optical data measured include EFs for the scattering and absorption coefficients (EF Bscat and EF Babs, m2 kg−1 fuel burned) and the single scattering albedo (SSA) at 870 and 405 nm, as well as the absorption Ångström exponents (AAE). By coupling the absorption and co-located trace gas and filter data we estimated black carbon (BC) EFs (g kg−1) and the mass absorption coefficient (MAC, m2 g−1) for the bulk organic carbon (OC) due to brown carbon (BrC). Consistent with the minimal flaming, the emissions of BC were negligible (0.0055 ± 0.0016 g kg−1). Aerosol absorption at 405 nm was ∼  52 times larger than at 870 nm and BrC contributed ∼  96 % of the absorption at 405 nm. Average AAE was 4.97 ± 0.65 (range, 4.29–6.23). The average SSA at 405 nm (0.974 ± 0.016) was marginally lower than the average SSA at 870 nm (0.998 ± 0.001). These data facilitate modeling climate-relevant aerosol optical properties across much of the UV/visible spectrum and the high AAE and lower SSA at 405 nm demonstrate the dominance of absorption by the organic aerosol. Comparing the Babs at 405 nm to the simultaneously measured OC mass on filters suggests a low MAC ( ∼  0.1) for the bulk OC, as expected for the low BC/OC ratio in the aerosol. The importance of pyrolysis (at lower MCE), as opposed to glowing (at higher MCE), in producing BrC is seen in the increase of AAE with lower MCE (r2 =  0.65).
The Zugspitze radiative closure experiment for quantifying water vapor absorption over the terrestrial and solar infrared – Part 3: Quantification of the mid- and near-infrared water vapor continuum in the 2500 to 7800 cm−1 spectral range under atmospheric conditions

We present a first quantification of the near-infrared (NIR) water vapor continuum absorption from an atmospheric radiative closure experiment carried out at the Zugspitze (47.42° N, 10.98° E; 2964 m a.s.l.). Continuum quantification is achieved via radiative closure using radiometrically calibrated solar Fourier transform infrared (FTIR) absorption spectra covering the 2500 to 7800 cm−1 spectral range. The dry atmospheric conditions at the Zugspitze site (IWV 1.4 to 3.3 mm) enable continuum quantification even within water vapor absorption bands, while upper limits for continuum absorption can be provided in the centers of window regions. Throughout 75 % of the 2500 to 7800 cm−1 spectral range, the Zugspitze results agree within our estimated uncertainty with the widely used MT_CKD 2.5.2 model (Mlawer et al., 2012). In the wings of water vapor absorption bands, our measurements indicate about 2–5 times stronger continuum absorption than MT_CKD, namely in the 2800 to 3000 cm−1 and 4100 to 4200 cm−1 spectral ranges. The measurements are consistent with the laboratory measurements of Mondelain et al. (2015), which rely on cavity ring-down spectroscopy (CDRS), and the calorimetric–interferometric measurements of Bicknell et al. (2006). Compared to the recent FTIR laboratory studies of Ptashnik et al. (2012, 2013), our measurements are consistent within the estimated errors throughout most of the spectral range. However, in the wings of water vapor absorption bands our measurements indicate typically 2–3 times weaker continuum absorption under atmospheric conditions, namely in the 3200 to 3400, 4050 to 4200, and 6950 to 7050 cm−1 spectral regions.
Trends analysis of PM source contributions and chemical tracers in NE Spain during 2004–2014: a multi-exponential approach

In this work for the first time data from two twin stations (Barcelona, urban background, and Montseny, regional background), located in the northeast (NE) of Spain, were used to study the trends of the concentrations of different chemical species in PM10 and PM2.5 along with the trends of the PM10 source contributions from the positive matrix factorization (PMF) model. Eleven years of chemical data (2004–2014) were used for this study. Trends of both species concentrations and source contributions were studied using the Mann–Kendall test for linear trends and a new approach based on multi-exponential fit of the data. Despite the fact that different PM fractions (PM2.5, PM10) showed linear decreasing trends at both stations, the contributions of specific sources of pollutants and of their chemical tracers showed exponential decreasing trends. The different types of trends observed reflected the different effectiveness and/or time of implementation of the measures taken to reduce the concentrations of atmospheric pollutants. Moreover, the trends of the contributions of specific sources such as those related with industrial activities and with primary energy consumption mirrored the effect of the financial crisis in Spain from 2008. The sources that showed statistically significant downward trends at both Barcelona (BCN) and Montseny (MSY) during 2004–2014 were secondary sulfate, secondary nitrate, and V–Ni-bearing source. The contributions from these sources decreased exponentially during the considered period, indicating that the observed reductions were not gradual and consistent over time. Conversely, the trends were less steep at the end of the period compared to the beginning, thus likely indicating the attainment of a lower limit. Moreover, statistically significant decreasing trends were observed for the contributions to PM from the industrial/traffic source at MSY (mixed metallurgy and road traffic) and from the industrial (metallurgy mainly) source at BCN. These sources were clearly linked with anthropogenic activities, and the observed decreasing trends confirmed the effectiveness of pollution control measures implemented at European or regional/local levels. Conversely, at regional level, the contributions from sources mostly linked with natural processes, such as aged marine and aged organics, did not show statistically significant trends. The trends observed for the PM10 source contributions reflected the trends observed for the chemical tracers of these pollutant sources well.
Can simple models predict large-scale surface ocean isoprene concentrations?

We use isoprene and related field measurements from three different ocean data sets together with remotely sensed satellite data to model global marine isoprene emissions. We show that using monthly mean satellite-derived chl a concentrations to parameterize isoprene with a constant chl a normalized isoprene production rate underpredicts the measured oceanic isoprene concentration by a mean factor of 19 ± 12. Improving the model by using phytoplankton functional type dependent production values and by decreasing the bacterial degradation rate of isoprene in the water column results in only a slight underestimation (factor 1.7 ± 1.2). We calculate global isoprene emissions of 0.21 Tg C for 2014 using this improved model, which is twice the value calculated using the original model. Nonetheless, the sea-to-air fluxes have to be at least 1 order of magnitude higher to account for measured atmospheric isoprene mixing ratios. These findings suggest that there is at least one missing oceanic source of isoprene and, possibly, other unknown factors in the ocean or atmosphere influencing the atmospheric values. The discrepancy between calculated fluxes and atmospheric observations must be reconciled in order to fully understand the importance of marine-derived isoprene as a precursor to remote marine boundary layer particle formation.
Origin of energetic ions in the polar cusp inferred from ion composition measurements by the Viking satellite

The magnetospheric ion composition spectrometer MICS on the Swedish Viking satellite provided measurements of the ion composition in the energy range 10.1 keV/eleqE/Qleq326.0 keV/e. Data obtained during orbit 842 were used to investigate the ion distribution in the northern polar cusp and its vicinity. The satellite traversed the outer ring current, boundary region, cusp proper and plasma mantle during its poleward movement. H+ and He++ ions were encountered in all of these regions. He+ ions were present only in the ring current. The number of O+ and O++ ions was very small. Heavy high-charge state ions typical for the solar wind were observed for the first time, most of them in the poleward part of the boundary region and in the cusp proper. The H+ ions exhibited two periods with high intensities. One of them, called the BR/CP event, appeared at energies up to 50 keV. It started at the equatorward limit of the boundary region and continued into the cusp proper. Energy spectra indicate a ring current origin for the BR/CP event. Pitch angle distributions show downward streaming of H+ ions at its equatorward limit and upward streaming on the poleward side. This event is interpreted as the result of pitch angle scattering of ring current ions by fluctuations in the magnetopause current layer in combination with poleward convection. The other of the two periods with high H+ ion intensities, called the accelerated ion event, was superimposed on the BR/CP event. It was restricted to energies leq15 keV and occurred in the poleward part of the boundary region. This event is regarded as the high-energy tail of magnetosheath ions that were accelerated while penetrating into the magnetosphere. The cusp region thus contains ions of magnetospheric as well as of magnetosheath origin. The appearance of the ions depends, in addition to the ion source, on the magnetic field configuration and dynamic processes inside and close to the cusp.
The use of a model current wedge in the determination of the position of substorm current systems

We present a technique for determination of the position and extent of the current systems present during substorm breakup. The parameters of a three-dimensional model of the currents are determined by fitting the model to data from the SAMNET magnetometer array, a midlatitude array of seven stations. The model used is a fully 3D current wedge aligned along dipolar field lines, the parameters being the meridians of upward and downward field-aligned currents (FACs), the latitude of the auroral electrojet and the magnitude of current growth over the observation interval. The method is novel in that the three geometrical parameters are first determined with the fourth arrived at via a secondary process. It has been applied to a number of events and appears to make estimates of the longitudes of the FACs consistent with the predictions of previous methods. Since the method employs a fully 3D model of the substorm current wedge as opposed to an idealised 2D model, it is reasonable to place more reliance on the results so obtained. Moreover, the method also has the additional benefit of a prediction of the latitude of the substorm electrojet and the nature of the current growth through the wedge at substorm onset.
On the computation of the barotropic mode of a free-surface world ocean model

The free-surface formulation of the equations of our world ocean model is briefly described. The barotropic mode equations are solved according to the split-explicit method, using different time steps for the external and internal modes. Because the numerical algorithm is implemented on the B-grid, a spurious, free-surface, two-grid interval mode may develop. This mode must be filtered out. The properties of two filters are theoretically investigated and their actual performance is tested in a series of numerical experiments. It is seen that one of these filters may severely perturb the local mass conservation, rendering it impossible to enforce the impermeability of the surface or the bottom of the ocean. The dynamics of the external mode is also examined, by studying the depth-integrated momentum equations. The depth-integral of the pressure force due to the slope of the ocean surface is approximately balanced by the depth-integral of the force ensuing from the horizontal variations of the density. The depth-integral of the Coriolis force is an order of magnitude smaller, except in the Southern Ocean. Two variational principles are resorted to for computing the fictitious ocean surface elevation corresponding to the approximate equilibrium between the dominant forces of the barotropic momentum equations.
A possible mechanism for <theta> aurora formation

A mechanism for the formation of <theta> aurora connected with the development of an interchange instability on the plasma sheet boundary layer (PSBL) is suggested. The PSBL is assumed to be deep inside the region of closed magnetic field lines. A system of equations connecting currents in the ionosphere and magnetosphere is solved numerically. It is found, using realistic ionospheric and magnetospheric parameters, that in a period of 8–10 min a system of plasma bars directed to the Sun arises at high latitudes. The system of bars is about 1000 km in width and 3000 km in length and approximates the Θ aurora. The suggested mechanism allows an explanation of a number of Θ aurora features such as the appearance probability, electric field directions, energy spectra of precipitating particles, and its location.