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Analysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela

The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.
Space-based evaluation of interactions between aerosols and low-level Arctic clouds during the Spring and Summer of 2008

This study explores the indirect effects of anthropogenic and biomass burning aerosols on Arctic clouds by co-locating a combination of MODIS and POLDER cloud products with output from the FLEXPART tracer transport model. During the activities of the International Polar Year for the Spring and Summer of 2008, we find a high sensitivity of Arctic cloud radiative properties to both anthropogenic and biomass burning pollution plumes, particularly at air temperatures near freezing or potential temperatures near 286 K. However, the sensitivity is much lower at both colder and warmer temperatures, possibly due to increases in the wet and dry scavenging of cloud condensation nuclei: the pollution plumes remain but the component that influences Arctic clouds has been removed along transport pathways. The analysis shows that, independent of local temperature, cloud optical depth is approximately four times more sensitive to changes in pollution levels than is cloud effective radius. This suggests that some form of feedback mechanism amplifies the radiative response of Arctic clouds to pollution through changes in cloud liquid water path.
Rate coefficients for the gas-phase reaction of OH with (Z)-3-hexen-1-ol, 1-penten-3-ol, (E)-2-penten-1-ol, and (E)-2-hexen-1-ol between 243 and 404 K

Rate coefficients, k, for the gas-phase reaction of the OH radical with (Z)-3-hexen-1-ol (Z)-CH3CH2CH = CHCH2CH2OH) (k1), 1-penten-3-ol (CH3CH2CH(OH)CH = CH2) (k2), (E)-2-penten-1-ol ((E)-CH3CH2CH = CHCH2OH) (k3), and (E)-2-hexen-1-ol ((E)-CH3CH2CH2CH = CHCH2OH) (k4), unsaturated alcohols that are emitted into the atmosphere following vegetation wounding, are reported. Rate coefficients were measured under pseudo-first-order conditions in OH over the temperature range 243–404 K at pressures between 20 and 100 Torr (He) using pulsed laser photolysis (PLP) to produce OH radicals and laser induced fluorescence (LIF) to monitor the OH temporal profile. The obtained rate coefficients were independent of pressure with negative temperature dependences that are well described by the Arrhenius expressions k1(T) = (1.3 ± 0.1) × 10−11 exp[(580 ± 10)/T]; k1(297 K) = (1.06 ± 0.12) × 10−10 k2(T) = (6.8 ± 0.7) × 10−12 exp[(690 ± 20)/T]; k2(297 K) = (7.12 ± 0.73) × 10−11 k3(T) = (6.8 ± 0.8) × 10−12 exp[(680 ± 20)/T]; k3(297 K) = (6.76 ± 0.70) × 10−11 k4(T) = (5.4 − 0.6) × 10−12 exp[(690 ± 20)/T]; k4(297 K) = (6.15 ± 0.75) × 10−11 (in units of cm3 molecule−1 s−1). The quoted uncertainties are at the 2σ (95% confidence) level and include estimated systematic errors. The rate coefficients obtained in this study are compared with literature values where possible.
Surface heterogeneity impacts on boundary layer dynamics via energy balance partitioning

The role of land-atmosphere interactions under heterogeneous surface conditions is investigated in order to identify mechanisms responsible for altering surface heat and moisture fluxes. Twelve coupled land surface – large eddy simulation scenarios with four different length scales of surface variability under three different horizontal wind speeds are used in the analysis. The base case uses Landsat ETM imagery over the Cloud Land Surface Interaction Campaign (CLASIC) field site for 3 June 2007. Using wavelets, the surface fields are band-pass filtered in order to maintain the spatial mean and variances to length scales of 200 m, 1600 m, and 12.8 km as lower boundary conditions to the model (approximately 0.25, 1.2 and 9.5 times boundary layer height). The simulations exhibit little variation in net radiation. Rather, there is a pronounced change in the partitioning of the surface energy between sensible and latent heat flux. The sensible heat flux is dominant for intermediate surface length scales. For smaller and larger scales of surface heterogeneity, which can be viewed as being more homogeneous, the latent heat flux becomes increasingly important. The simulations showed approximately 50 Wm−2 difference in the spatially averaged latent heat flux. The results reflect a general decrease of the Bowen ratio as the surface conditions transition from heterogeneous to homogeneous. Air temperature is less sensitive to variations in surface heterogeneity than water vapor, which implies that the role of surface heterogeneity may be to maximize convective heat fluxes through modifying and maintaining local temperature gradients. More homogeneous surface conditions (i.e. smaller length scales), on the other hand, tend to maximize latent heat flux. The intermediate scale (1600 m) this does not hold, and is a more complicated interaction of scales. Scalar vertical profiles respond predictably to the partitioning of surface energy. Fourier spectra of the vertical wind speed, air temperature and specific humidity (w~, T~ and q~) and associated cospectra (w~T~, w~q~ and T~q~), however, are insensitive to the length scale of surface heterogeneity, but the near surface spectra are sensitive to the mean wind speed.
Trajectory analysis on the origin of air mass and moisture associated with Atmospheric Rivers over the west coast of the United States

The origins and pathways of air masses leading to heavy rainfall over the west coast of the United States are examined by computing the back-trajectories in a Lagrangian quasi-isentropic trajectory model. Extreme precipitation over the west coast of the United States often coincides with transport in a deep and narrow corridor of concentrated water vapor band from the ocean, commonly referred to as Atmospheric Rivers (ARs). They also occur in conjunction with moisture plumes emanating from the tropics, or along the mid-latitude storm track. However, the actual moisture sources and the dynamic and thermodynamic processes of the moisture transport, are still unclear. Trajectories are found to be insensitive to the reanalysis data set used; we examined NCEP, GMAO MERRA, and ECMWF ERA-Interim. Reconstructed water vapor mixing ratios along trajectories are in generally good agreement among the reanalysis datasets in most of the subtropics and extratropics, indicating that the large-scale circulation is a primary control for moisture transport over those regions. Clustering and pdf (probability density function) analyses illustrate that trajectories over the west coast of United States have different origins. One group of trajectories (cluster 1) originates in the warm part of extratropical cyclones in the low level. The other group of trajectories (cluster 2) originates in the cold and dry regions in the mid-level (pressures less than 600 hPa) over northeastern Asia, then cross the Pacific Ocean. This study demonstrates that the quasi-isentropic Lagrangian trajectory model and clustering analysis (that have been typically used to analyze trajectories in the upper troposphere and higher altitudes) can be used to examine sources of air masses and moisture, and also associated transport processes in the lower troposphere.
Understanding effective diameter and its application to terrestrial radiation in ice clouds

The cloud property known as "effective diameter" or "effective radius", which in essence is the cloud particle size distribution (PSD) volume at bulk density divided by its projected area, is used extensively in atmospheric radiation transfer, climate modeling and remote sensing. This derives from the assumption that PSD optical properties can be uniquely described in terms of their effective diameter, De, and their cloud water content (CWC), henceforth referred to as the De-CWC assumption. This study challenges this assumption, showing that while the De-CWC assumption appears generally valid for liquid water clouds, it appears less valid for ice clouds in regions where (1) absorption is not primarily a function of either the PSD ice water content (IWC) or the PSD projected area, and (2) where wave resonance (i.e. photon tunneling) contributes significantly to absorption. These two regions often strongly coincide at terrestrial wavelengths when De<~60 μm, which is where this De-CWC assumption appears poorest. Treating optical properties solely in terms of De and IWC may lead to errors up to 24%, 26% and 20% for terrestrial radiation in the window region regarding the absorption and extinction coefficients and the single scattering albedo, respectively. Outside the window region, errors may reach 33% and 42% regarding absorption and extinction. The magnitude and sign of these errors can change rapidly with wavelength, which may produce significant errors in climate modeling, remote sensing and other applications concerned with the wavelength dependence of radiation. Where the De-CWC assumption breaks down, ice cloud optical properties appear to depend on De, IWC and the PSD shape. Optical property parameterizations in climate models and remote sensing algorithms based on historical PSD measurements may exhibit errors due to previously unknown PSD errors (i.e. the presence of ice artifacts due to the shattering of larger ice particles on the probe inlet tube during sampling). More recently developed cloud probes are designed to mitigate this shattering problem. Using realistic PSD shapes for a given temperature (and/or IWC) and cloud type may minimize errors associated with PSD shape in ice optics parameterizations and remote sensing algorithms. While this topic was investigated using two ice optics schemes (the Yang et al., 2005 database and the modified anomalous diffraction approximation, or MADA), a physical understanding of the limitations of the De-IWC assumption was made possible by using MADA. MADA allows one to approximate the contribution of photon tunneling to absorption relative to other optical processes, which reveals that part of the error regarding the De-IWC assumption can be associated with tunneling. By relating the remaining error to the radiation penetration depth in bulk ice (ΔL) due to absorption, the domain where the De-IWC assumption is weakest was described in terms of De and ΔL.
Parameterization of ion-induced nucleation rates based on ambient observations

Atmospheric ions participate in the formation of new atmospheric aerosol particles, yet their exact role in this process has remained unclear. Here we derive a new simple parameterization for ion-induced nucleation or, more precisely, for the formation rate of charged 2-nm particles. The parameterization is semi-empirical in the sense that it is based on comprehensive results of one-year-long atmospheric cluster and particle measurements in the size range ~1–42 nm within the EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions) project. Data from 12 field sites across Europe measured with different types of air ion and cluster mobility spectrometers were used in our analysis, with more in-depth analysis made using data from four stations with concomitant sulphuric acid measurements. The parameterization is given in two slightly different forms: a more accurate one that requires information on sulfuric acid and nucleating organic vapor concentrations, and a simpler one in which this information is replaced with the global radiation intensity. These new parameterizations are applicable to all large-scale atmospheric models containing size-resolved aerosol microphysics, and a scheme to calculate concentrations of sulphuric acid, condensing organic vapours and cluster ions.
Three-year observations of halocarbons at the Nepal Climate Observatory at Pyramid (NCO-P, 5079 m a.s.l.) on the Himalayan range

A monitoring programme for halogenated climate-altering gases has been established in the frame of the SHARE EV-K2-CNR project at the Nepal Climate Laboratory – Pyramid in the Himalayan range at the altitude of 5079 m a.s.l. The site is very well located to provide important insights on changes in atmospheric composition in a region that is of great significance for emissions of both anthropogenic and biogenic halogenated compounds. Measurements are performed since March 2006, with grab samples collected on a weekly basis. The first three years of data have been analysed. After the identification of the atmospheric background values for fourteen halocarbons, the frequency of occurrence of pollution events have been compared with the same kind of analysis for data collected at other global background stations. The analysis showed the fully halogenated species, whose production and consumption are regulated under the Montreal Protocol, show a significant occurrence of "above the baseline" values, as a consequence of their current use in the developing countries surrounding the region, meanwhile the hydrogenated gases, more recently introduced into the market, show less frequent spikes. Atmospheric concentration trends have been calculated as well, and they showed a fast increase, ranging from 5.7 to 12.6%, of all the hydrogenated species, and a clear decrease of methyl chloroform (−17.7%). The comparison with time series from other stations has also allowed to derive Meridional gradients, which are absent for long living well mixed species, while for the more reactive species, the gradient increases inversely with respect to their atmospheric lifetime. The effect of long range transport and of local events on the atmospheric composition at the station has been analysed as well, allowing the identification of relevant source regions the Northern half of the Indian sub-continent. Also, at finer spatial scales, a smaller, local contribution of forest fires from the Khumbu valley has been detected.
Comparison of aerosol properties from the Indian Himalayas and the Indo-Gangetic plains

Gual Pahari is a polluted semi-urban background measurement site at the Indo-Gangetic plains close to New Delhi and Mukteshwar is a relatively clean background measurement site at the foothills of the Himalayas about 270 km NE from Gual Pahari and about 2 km above the nearby plains. Two years long data sets including aerosol and meteorological parameters as well as modeled backward trajectories and boundary layer heights were compared. The purpose was to see how aerosol concentrations vary between clean and polluted sites not very far from each other. Specifically, we were exploring the effect of boundary layer evolution on aerosol concentrations. The measurements showed that especially during the coldest winter months, aerosol concentrations are significantly lower in Mukteshwar. On the other hand, the difference is smaller and also the concentration trends are quite similar from April to October. With the exception of the monsoon season, when rains are affecting on aerosol concentrations, clear but practically opposite diurnal cycles are observed. When the lowest daily aerosol concentrations are seen during afternoon hours in Gual Pahari, there is a peak in Mukteshwar aerosol concentrations. In addition to local sources and long-range transport of dust, boundary layer dynamics can explain the observed differences and similarities. When mixing of air masses is limited during the relatively cool winter months, aerosol pollutions are accumulated to the plains, but Mukteshwar is above the pollution layer. When mixing increases in the spring, aerosol concentrations are increased in Mukteshwar and decreased in Gual Pahari. The effect of mixing is also clear in the diurnal concentration cycles. When daytime mixing decreases aerosol concentrations in Gual Pahari, those are increased in Mukteshwar.
The effect of sea ice loss on sea salt aerosol concentrations and the radiative balance in the Arctic

Understanding Arctic climate change requires knowledge of both the external and the local drivers of Arctic climate as well as local feedbacks within the system. An Arctic feedback mechanism relating changes in sea ice extent to an alteration of the emission of sea salt aerosol and the consequent change in radiative balance is examined. A set of idealized climate model simulations were performed to quantify the radiative effects of changes in sea salt aerosol emissions induced by prescribed changes in sea ice extent. The model was forced using sea ice concentrations consistent with present day conditions and projections of sea ice extent for 2100. Sea salt aerosol emissions increase in response to a decrease in sea ice, the model results showing an annual average increase in number emission over the polar cap (70–90° N) of 86 × 106 m−2 s−1 (mass emission increase of 23 μg m−2 s−1). This in turn leads to an increase in the natural aerosol optical depth of approximately 23%. In response to changes in aerosol optical depth, the natural component of the aerosol direct forcing over the Arctic polar cap is estimated to be between −0.2 and −0.4 W m−2 for the summer months, which results in a negative feedback on the system. The model predicts that the change in first indirect aerosol effect (cloud albedo effect) is approximately a factor of ten greater than the change in direct aerosol forcing although this result is highly uncertain due to the crude representation of Arctic clouds and aerosol-cloud interactions in the model. This study shows that both the natural aerosol direct and first indirect effects are strongly dependent on the surface albedo, highlighting the strong coupling between sea ice, aerosols, Arctic clouds and their radiative effects.