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Particle characterization at the Cape Verde atmospheric observatory during the 2007 RHaMBLe intensive

The chemical characterization of filter high volume (HV) and Berner impactor (BI) samples PM during RHaMBLe (Reactive Halogens in the Marine Boundary Layer) 2007 shows that the Cape Verde aerosol particles are mainly composed of sea salt, mineral dust and associated water. Minor components are nss-salts, OC and EC. The influence from the African continent on the aerosol constitution was generally small but air masses which came from south-western Europe crossing the Canary Islands transported dust to the sampling site together with other loadings. The mean mass concentration was determined for PM10 to 17 μg/m3 from impactor samples and to 24.2 μg/m3 from HV filter samples. Non sea salt (nss) components of PM were found in the submicron fractions and nitrate in the coarse mode fraction. Bromide was found in all samples with much depleted concentrations in the range 1–8 ng/m3 compared to fresh sea salt aerosol indicating intense atmospheric halogen chemistry. Loss of bromide by ozone reaction during long sampling time is supposed and resulted totally in 82±12% in coarse mode impactor samples and in filter samples in 88±6% bromide deficits. A chloride deficit was determined to 8% and 1% for the coarse mode particles (3.5–10 μm; 1.2–3.5 μm) and to 21% for filter samples. During 14 May with high mineral dust loads also the maximum of OC (1.71μg/m3) and EC (1.25 μg/m3) was measured. The minimum of TC (0.25 μg/m3) was detected during the period 25 to 27 May when pure marine air masses arrived. The concentrations of carbonaceous material decrease with increasing particle size from 60% for the ultra fine particles to 2.5% in coarse mode PM. Total iron (dust vs. non-dust: 0.53 vs. 0.06 μg m3), calcium (0.22 vs. 0.03 μg m3) and potassium (0.33 vs. 0.02 μg m3) were found as good indicators for dust periods because of their heavily increased concentration in the 1.2 to 3.5 μm fraction as compared to their concentration during the non-dust periods. For the organic constituents, oxalate (78–151 ng/m3) and methanesulfonic acid (MSA, 25–100 ng/m3) are the major compounds identified. A good correlation between nss-sulphate and MSA was found for the majority of days indicating active DMS chemistry and low anthropogenic influences.
Why anisotropic turbulence matters: another reply

We continue the debate on anisotropic but scaling turbulence and its effect on aircraft measurements of turbulence (cf. Lindborg et al., 2010a, b); hereafter LTNCG1, LTNCG2). We revisit the repeatedly presented back-of-the-envelope calculation and discuss wind statistics on real isobars. We then discuss theoretical and empirical evidence that a k−5/3 horizontal wind spectrum could extend out to planetary scales.
Particle number, particle mass and NOx emission factors at a highway and an urban street in Copenhagen

This paper presents measurements of traffic-generated gas and particle pollution at two sites, one near a major highway and one near a busy urban street in Copenhagen, Denmark. Both sites were equipped for a 4-week period with a set of two measurement stations, one close to the kerbside and one background station. Measurements were carried out from March to April~2008, investigating NOx concentrations, submicrometer particle number size distribution (size range 10–700 nm), particle mass (PM2.5, PM10), and meteorological parameters. In this study we also estimate the emission factors for NOx, particle number and particle mass using measured traffic volume and dilution rate calculated by the Operational Street Pollution Model (WinOSPM). The mean concentrations of most of the measured pollutants are similar for the highway and the urban kerbside stations due to similar traffic density. The average concentrations of NOx are 142 μg m−3 and 136 μg m−3 for the highway and the urban kerbside stations, respectively. These values are about 5 times higher compared to the corresponding background values. The average particle number concentration is 24 900 particles cm−3 and 27 100 particles cm−3 for the highway and the urban kerbside stations, respectively, and these values exceed those measured at the background stations by a factor of 3 to 5. The temporal variation of the traffic contribution (difference of kerbside and background concentrations) is analysed for NOx, particle number and mass, and it follows the traffic pattern at the urban and the highway sites. Emission factors for particle number are found to be quite similar at both sites, (215±5) 1012 particles veh−1 km−1 for the highway and (187±3) 1012 particles veh−1 km−1 for the urban site. Heavy duty vehicles (HDVs) are found to emit about 20 times more particles than light duty vehicles (LDVs), which is in good agreement with other published studies. Emission factors are also determined for individual particle modes identified in the size spectra. Average fleet emission factors for PM2.5 at the highway and the urban site are 29 mg veh−1 km−1 and 46 mg veh−1 km−1, respectively. The estimated particle number and size spectra emission factors will provide valuable input for air quality and particle dispersion modelling near highways and in urban areas.
Model of optical response of marine aerosols to Forbush decreases

In order to elucidate the effect of galactic cosmic rays on cloud formation, we investigate the optical response of marine aerosols to Forbush decreases – abrupt decreases in galactic cosmic rays – by means of modeling. We vary the nucleation rate of new aerosols, in a sectional coagulation and condensation model, according to changes in ionization by the Forbush decrease. From the resulting size distribution we then calculate the aerosol optical thickness and Angstrom exponent, for the wavelength pairs 350, 450 nm and 550, 900 nm. In the cases where the output parameters from the model seem to compare best with atmospheric observations we observe, for the shorter wavelength pair, a change in Angstrom exponent, following the Forbush Decrease, of −6 to +3%. In some cases we also observe a delay in the change of Angstrom exponent, compared to the maximum of the Forbush decrease, which is caused by different sensitivities of the probing wavelengths to changes in aerosol number concentration and size. For the long wavelengths these changes are generally smaller. The types and magnitude of change is investigated for a suite of nucleation rates, condensable gas production rates, and aerosol loss rates. Furthermore we compare the model output with observations of 5 of the largest Forbush decreases after year 2000. For the 350, 450 nm pair we use AERONET data and find a comparable change in signal while the Angstrom Exponent is lower in the model than in the data, due to AERONET being mainly sampled over land. For 550, 900 nm we compare with both AERONET and MODIS and find little to no response in both model and observations. In summary our study shows that the optical properties of aerosols show a distinct response to Forbush Decreases, assuming that the nucleation of fresh aerosols is driven by ions. Shorter wavelengths seem more favorable for observing these effects and great care should be taken when analyzing observations, in order to avoid the signal being drowned out by noise.
Simultaneous retrieval of aerosol and surface optical properties from combined airborne- and ground-based direct and diffuse radiometric measurements

This paper presents a new method for simultaneously retrieving aerosol and surface reflectance properties from combined airborne and ground-based direct and diffuse radiometric measurements. The method is based on the standard Aerosol Robotic Network (AERONET) method for retrieving aerosol size distribution, complex index of refraction, and single scattering albedo, but modified to retrieve aerosol properties in two layers, below and above the aircraft, and parameters on surface optical properties from combined datasets (Cloud Absorption Radiometer (CAR) and AERONET data). A key advantage of this method is the inversion of all available spectral and angular data at the same time, while accounting for the influence of noise in the inversion procedure using statistical optimization. The wide spectral (0.34–2.30 μm) and angular range (180°) of the CAR instrument, combined with observations from an AERONET sunphotometer, provide sufficient measurement constraints for characterizing aerosol and surface properties with minimal assumptions. The robustness of the method was tested on observations made during four different field campaigns: (a) the Southern African Regional Science Initiative 2000 over Mongu, Zambia, (b) the Intercontinental Transport Experiment-Phase B over Mexico City, Mexico (c) Cloud and Land Surface Interaction Campaign over the Atmospheric Radiation Measurement (ARM) Central Facility, Oklahoma, USA, and (d) the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) over Elson Lagoon in Barrow, Alaska, USA. The four areas are dominated by different surface characteristics and aerosol types, and therefore provide good test cases for the new inversion method.
Nocturnal nitrogen oxides at a rural mountain-site in south-western Germany

A new, two-channel instrument for simultaneous NO3 and N2O5 monitoring was used to make the first comprehensive set of nocturnal NOx measurements (NO, NO2, NO3 and N2O5) at the Taunus Observatory, a rural mountain site (Kleiner Feldberg) in South-western Germany. In May 2008, NO3 and N2O5 mixing ratios were well above the instrumental detection limit (a few ppt) on all nights of the campaign and were characterised by large variability. The concentrations of NO3, N2O5 and NO2 were consistent with the equilibrium constant, K2, defining the rates of formation and thermal dissociation of N2O5. A steady-state lifetime analysis is consistent with the loss of nocturnal NOx being dominated by the reaction of NO3 with volatile organic compounds in this forested region, with N2O5 uptake to aerosols of secondary importance. Analysis of a limited dataset obtained at high relative humidity indicated that the loss of N2O5 by reaction with water vapour is less efficient (>factor 3) than derived using laboratory kinetic data. The fraction of NOx present as NO3 and N2O5 reached ~20% on some nights, with night-time losses of NOx competing with daytime losses.
Lidar characterization of the Arctic atmosphere during ASTAR 2007: four cases studies of boundary layer, mixed-phase and multi-layer clouds

During the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR), which was conducted in Svalbard in March and April 2007, tropospheric Arctic clouds were observed with two ground-based backscatter lidar systems (micro pulse lidar and Raman lidar) and with an airborne elastic lidar. In the time period of the ASTAR 2007 campaign, an increase in low-level cloud cover (cloud tops below 2.5 km) from 51% to 65% was observed above Ny-Ålesund. Four different case studies of lidar cloud observations are analyzed: With the ground-based Raman lidar, a layer of spherical particles was observed at an altitude of 2 km after the dissolution of a cloud. The layer probably consisted of small hydrated aerosol (radius of 280 nm) with a high number concentration (around 300 cm−3) at low temperatures (−30 °C). Observations of a boundary layer mixed-phase cloud by airborne lidar and concurrent airborne in situ and spectral solar radiation sensors revealed the localized process of total glaciation at the boundary of different air masses. In the free troposphere, a cloud composed of various ice layers with very different optical properties was detected by the Raman lidar, suggesting large differences of ice crystal size, shape and habit. Further, a mixed-phase double layer cloud was observed by airborne lidar in the free troposphere. Local orography influenced the evolution of this cloud. The four case studies revealed relations of cloud properties and specific atmospheric conditions, which we plan to use as the base for numerical simulations of these clouds.
Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.
Toward real-time measurement of atmospheric mercury concentrations using cavity ring-down spectroscopy

Cavity ring-down spectroscopy (CRDS) is a direct absorption technique that utilizes path lengths up to multiple kilometers in a compact absorption cell and has a significantly higher sensitivity than conventional absorption spectroscopy. This tool opens new prospects for study of gaseous elemental mercury (Hg0) because of its high temporal resolution and reduced sample volume requirements (<0.5 l of sample air). We developed a new sensor based on CRDS for measurement of (Hg0) mass concentration. Sensor characteristics include sub-ng m−3 detection limit and high temporal resolution using a frequency-doubled, tuneable dye laser emitting pulses at ~253.65 nm with a pulse repetition frequency of 50 Hz. The dye laser incorporates a unique piezo element attached to its tuning grating allowing it to tune the laser on and off the Hg0 absorption line on a pulse-to-pulse basis to facilitate differential absorption measurements. Hg0 absorption measurements with this CRDS laboratory prototype are highly linearly related to Hg0 concentrations determined by a Tekran 2537B analyzer over an Hg0 concentration range from 0.2 ng m−3 to 573 ng m−3, implying excellent linearity of both instruments. The current CRDS instrument has a sensitivity of 0.10 ng Hg0 m−3 at 10-s time resolution. Ambient-air tests showed that background Hg0 levels can be detected at low temporal resolution (i.e., 1 s), but also highlight a need for high-frequency (i.e., pulse-to-pulse) differential on/off-line tuning of the laser wavelength to account for instabilities of the CRDS system and variable background absorption interferences. Future applications may include ambient Hg0 flux measurements with eddy covariance techniques, which require measurements of Hg0 concentrations with sub-ng m−3 sensitivity and sub-second time resolution.
Derivation of the stoichiometric coefficient of water (νw) to account for water uptake by atmospheric aerosols

In this work we derive the effective stoichiometric coefficient of water (vw), introduced by Metzger and Lelieveld, 2007 (ML07), from first principles. We give examples of the application of vw in CPU efficient computations of the Deliquescence Relative Humidity (DRH) and the water uptake of atmospheric aerosols, being important parameters in atmospheric chemistry and climate modeling. We show that the application of vw in a gas/liquid/solid aerosol equilibrium partitioning model (EQSAM3) leads to results that are in excellent agreement with those of widely used thermodynamic (reference) models (E-AIM and ISORROPIA2) for various single salt solutions (NaCl, NH4NO3, (NH4)2SO4, NH4HSO4, NaHSO4) and the corresponding mixed solutions (including (NH4)3H(SO4)2 and Na3H(SO4)2), notwithstanding the distinct different theoretical and numerical concepts on which these models are based.