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Modelling light scattering by mineral dust using spheroids: assessment of applicability

We study the applicability of spheroidal model particles for simulating the single-scattering optical properties of mineral dust aerosols. To assess the range of validity of this model, calculations are compared to laboratory observations for five different dust samples at two wavelengths. We further investigate whether the best-fit shape distributions of spheroids for different mineral dust samples have any similarities that would allow us to suggest a generic first-guess shape distribution for suspended mineral dust. We find that best-fit shape distributions vary considerably between samples and even between wavelengths, making definitive suggestions for a shape distribution difficult. The best-fit shape distribution also depends strongly on the refractive index assumed and the cost function adopted. However, a power-law shape distribution which favours those spheroids that depart most from the spherical shape is found to work well in most cases. To reproduce observed asymmetry parameters, best results are obtained with a power-law shape distribution with an exponent around three.
Theoretical basis for convective invigoration due to increased aerosol concentration

The potential effects of increased aerosol loading on the development of deep convective clouds and resulting precipitation amounts are studied by employing the Weather Research and Forecasting (WRF) model as a detailed high-resolution cloud resolving model (CRM) with both detailed bulk and bin microphysics schemes. Both models include a physically-based activation scheme that incorporates a size-resolved aerosol population. We demonstrate that the aerosol-induced effect is controlled by the balance between latent heating and the increase in condensed water aloft, each having opposing effects on buoyancy. It is also shown that under polluted conditions, increases in the CCN number concentration reduce the cumulative precipitation due to the competition between the sedimentation and evaporation/sublimation timescales. The effect of an increase in the IN number concentration on the dynamics of deep convective clouds is small and the resulting decrease in domain-averaged cumulative precipitation is shown not to be statistically significant, but may act to suppress precipitation. It is also shown that even in the presence of a decrease in the domain-averaged cumulative precipitation, an increase in the precipitation variance, or in other words, andincrease in rainfall intensity, may be expected in more polluted environments, especially in moist environments. A significant difference exists between the predictions based on the bin and bulk microphysics schemes of precipitation and the influence of aerosol perturbations on updraft velocity within the convective core. The bulk microphysics scheme shows little change in the latent heating rates due to an increase in the CCN number concentration, while the bin microphysics scheme demonstrates significant increases in the latent heating aloft with increasing CCN number concentration. This suggests that even a detailed two-bulk microphysics scheme, coupled to a detailed activation scheme, may not be sufficient to predict small changes that result from perturbations in aerosol loading.
Understanding evolution of product composition and volatility distribution through in-situ GC × GC analysis: a case study of longifolene ozonolysis

A method for predicting volatility and polarity based on chromatographic information was developed and applied to the smog chamber ozonolysis of the sesquiterpene longifolene. The products were collected and analyzed using a GC × GC Thermal Desorption Aerosol Gas Chromatograph/Mass Spectrometer (2D-TAG) and a quadrupole Aerodyne Aerosol Mass Spectrometer (AMS). All the secondary organic aerosol (SOA) was produced within the first half hour of the experiment. However, the oxidation level of the organic aerosol, as inferred from the fraction of ion m/z 44, suggested continued evolution of the SOA over the subsequent hours. Measurements of speciated organic compounds using 2D-TAG confirm that the composition of the particles changed over the course of the experiment. Nearly 200 oxidation products (thought to be mostly ketones and acids) were observed with 2D-TAG, but most could not be identified definitively due to a lack of standards and the absence of likely sesquiterpene oxidation products in available mass spectral databases. To categorize the observed products, the vapor pressure and oxygen-to-carbon ratio (O/C) of observed compounds were estimated based on their two-dimensional chromatographic retention times relative to those of known standards, establishing a retention time correlation (RTC) method for using 2D-TAG to better constrain important modelling parameters. The product distribution continuously evolved in volatility and oxygenation during 5 h of oxidation. Using peak area as the best available proxy for mass, we conclude that the product mixture includes many non-negligible products; the most abundant 3 compounds accounted for only half of the total observed peak area and 80 % of peak area was spread across 15 compounds. The data provide evidence for three conclusions: (1) 2D-TAG provides valuable volatility and oxygenation information even in the absence of definitive species identification, (2) complex particle-phase chemistry causes continued evolution of particle composition after new particles formation, and (3) minor products contribute significantly to SOA from the ozonolysis of longifolene.
Analysis of HCl and ClO time series in the upper stratosphere using satellite data sets

Previous analyses of satellite and ground-based measurements of hydrogen chloride (HCl) and chlorine monoxide (ClO) have suggested that total inorganic chlorine in the upper stratosphere is on the decline. We create HCl and ClO time series using satellite data sets extended to November 2008, so that an update can be made on the long term evolution of these two species. We use the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data for the HCl analysis, and the Odin Sub-Millimetre Radiometer (SMR) and the Aura Microwave Limb Sounder (Aura-MLS) measurements for the study of ClO. Altitudes between 35 and 45 km and two mid-latitude bands: 30° S–50° S and 30° N–50° N, for HCl, and 20° S–20° N for ClO and HCl are studied. ACE-FTS and HALOE HCl anomaly time series (with QBO and seasonal contributions removed) are combined to produce all instrument average time series, which show HCl to be reducing from peak 1997 values at a linear estimated rate of −5.1 % decade−1 in the Northern Hemisphere and −5.2 % decade−1 in the Southern Hemisphere, while the tropics show a linear trend of −5.8 % per decade (although we do not remove the QBO contribution there due to sparse data). Trend values are significantly different from a zero trend at the 2 sigma level. ClO is decreasing in the tropics by −7.1 % ± 7.8 % decade−1 based on measurements made from December 2001 to November 2008. The statistically significant downward trend found in HCl after 1997 and the apparent downward ClO trend since 2001 (although not statistically significant) confirm how effective the 1987 Montreal protocol objectives and its amendments have been in reducing the total amount of inorganic chlorine.
Simultaneous trace gas measurements using two Fourier transform spectrometers at Eureka, Canada during spring 2006, and comparisons with the ACE-FTS

The 2006 Canadian Arctic ACE (Atmospheric Chemistry Experiment) Validation Campaign collected measurements at the Polar Environment Atmospheric Research Laboratory (PEARL, 86.42° W, 80.05° N, 610 m a.s.l.) at Eureka, Canada from 17 February to 31 March 2006. Two of the ten instruments involved in the campaign, both Fourier transform spectrometers (FTSs), were operated simultaneously, recording atmospheric solar absorption spectra. The first instrument was an ABB Bomem DA8 high-resolution infrared FTS. The second instrument was the Portable Atmospheric Research Interferometric Spectrometer for the Infrared (PARIS-IR), the ground-based version of the satellite-borne FTS on the ACE satellite (ACE-FTS). From the measurements collected by these two ground-based instruments, total column densities of seven stratospheric trace gases (O3, HCl, ClONO2, HF, HNO3, NO2, and NO) were retrieved using the optimal estimation method and these results were compared. Since the two instruments sampled the same portions of atmosphere by synchronizing observations during the campaign and used consistent retrieval parameters, the biases in retrieved columns from the two spectrometers represent the instrumental differences. Mean differences in total column densities of O3, HCl, ClONO2, HF, HNO3, and NO2 from the observations between PARIS-IR and the DA8 FTS are 2.8 %, −3.2 %, −4.3 %, −1.5 %, −1.9 %, and −0.1 %, respectively. Partial column results from the ground-based spectrometers were also compared with partial columns derived from ACE-FTS version 2.2 (including updates for O3) profiles. Mean differences in partial column densities of O3, HCl, ClONO2, HF, HNO3, NO2, and NO from the measurements between ACE-FTS and the DA8 FTS are −5.9 %, −8.5 %, −11.8 %, −0.9 %, −6.6 %, −21.6 % and −7.6 % respectively. Mean differences in partial column densities of O3, HCl, ClONO2, HF, HNO3, NO2 from the measurements between ACE-FTS and the PARIS-IR are −5.2 %, −4.6 %, −2.3 %, −4.7 %, 5.7 % and −11.9 %, respectively. This work provides further evidence of the reliability of ACE-FTS measurements from the first three years of on-orbit observations. Column densities of O3, HCl, ClONO2, and HNO3 from the three FTSs were normalized with respect to HF and used to compare the time evolution of the chemical constituents in the atmosphere over Eureka during spring 2006.
Sensing Hadley cell with space lidar

This letter shows that the extent of the Hadley cell could reliably be estimated by measuring the height of the uppermost super-thin clouds in the troposphere with space-borne lidar. Through consecutive multi-year measurements of the height of the uppermost super-thin clouds, a good estimation of the expansion of the Hadley cell could be obtained.
Ultraviolet actinic flux in clear and cloudy atmospheres: model calculations and aircraft-based measurements

Ultraviolet (UV) actinic fluxes measured with two Scanning Actinic Flux Spectroradiometers (SAFS) aboard the NASA DC-8 aircraft are compared with the Tropospheric Ultraviolet-Visible (TUV) model. The observations from 17 days in July-August 2004 (INTEX-NA field campaign) span a wide range of latitudes (28° N–53° N), longitudes (45° W–140° W), altitudes (0.1–11.9 km), ozone columns (285–353 DU), and solar zenith angles (2°–85°). Both cloudy and cloud-free conditions were encountered. For cloud-free conditions, the ratio of observed to clear-sky-model actinic flux (integrated from 298 to 422 nm) was 1.01±0.04, i.e. in good agreement with observations. The agreement improved to 1.00±0.03 for the down-welling component under clear sky conditions. In the presence of clouds and depending on their position relative to the aircraft, the up-welling component was frequently enhanced (by as much as a factor of 8 relative to cloud-free values) while the down-welling component showed both reductions and enhancements of up to a few tens of percent. Including all conditions, the ratio of the observed actinic flux to the cloud-free model value was 1.1±0.3 for the total, or separately 1.0±0.2 for the down-welling and 1.5±0.8 for the up-welling components. The correlations between up-welling and down-welling deviations are well reproduced with sensitivity studies using the TUV model, and are understood qualitatively with a simple conceptual model. This analysis of actinic flux observations illustrates opportunities for future evaluations of photolysis rates in three-dimensional chemistry-transport models.
Seasonal variations and vertical features of aerosol particles in the Antarctic troposphere

Tethered balloon-borne aerosol measurements were conducted at Syowa Station, Antarctica during the 46th Japanese Antarctic expedition (2005–2006). The CN concentration reached a maximum in the summer, although the number concentrations of fine particles (Dp>0.3 μm) and coarse particles (Dp>2.0 μm) increased during the winter–spring. The CN concentration was 30–2200 cm−3 near the surface (surface – 500 m) and 7–7250 cm−3 in the lower free troposphere (>1500 m). During the austral summer, higher CN concentration was often observed in the lower free troposphere, where the number concentrations in fine and coarse modes were remarkably lower. The frequent appearance of higher CN concentrations in the free troposphere relative to continuous aerosol measurements at the ground strongly suggests that new particle formation is more likely to occur in the lower free troposphere in Antarctic regions. Seasonal variations of size distribution of fine-coarse particles show that the contribution of the coarse mode was greater in the winter–spring than in summer because of the dominance of sea-salt particles in the winter–spring. The number concentrations of fine and coarse particles were high in air masses from the ocean and mid-latitudes. Particularly, aerosol enhancement was observed not only in the boundary layer, but also in the lower free troposphere during and immediately after Antarctic haze events occurring in May, July and September.
The fluorescence properties of aerosol larger than 0.8 μm in urban and tropical rainforest locations

UV-LIF measurements were performed on ambient aerosol in Manchester, UK (urban city centre, winter) and Borneo, Malaysia (remote, tropical) using a Wide Issue Bioaerosol Spectrometer, version 3 (WIBS3). These sites are taken to represent environments with minor and significant primary biological aerosol (PBA) influences respectively, and the urban dataset describes the fluorescent background aerosol against which PBA must be identified by researchers using LIF. The ensemble aerosol at both sites was characterised over 2–3 weeks by measuring the fluorescence intensity and optical equivalent diameter (DP) of single particles sized 0.8 ≤ DP ≤ 20 μm. Filter samples were also collected for a subset of the Manchester campaign and analysed using energy dispersive X-Ray (EDX) spectroscopy and environmental scanning electron microscopy (ESEM), which revealed mostly non-PBA at D ≤ 1 μm. The WIBS3 features three fluorescence channels: the emission following a 280 nm excitation is recorded at 310–400 nm (channel F1) and 400–600 nm (F2), and fluorescence excited at 350 nm is detected at 400–600 nm (F3). In Manchester the primary size mode of fluorescent and non-fluorescent material was present at 0.8–1.2 μm, with a secondary fluorescent mode at 2–4 μm. In Borneo non-fluorescent material peaked at 0.8–1.2 μm and fluorescent at 3–4 μm. Agreement between fluorescent number concentrations in each channel differed at the two sites, with F1 and F3 reporting similar concentrations in Borneo but F3 outnumbering F1 by a factor of 2–3 across the size spectrum in Manchester. The fluorescence intensity in each channel generally rose with DP at both sites with the exception of F1 intensity in Manchester, which peaked at DP = 4 μm, causing a divergence between F1 and F3 intensity at larger DP. This divergence and the differing fluorescent particle concentrations demonstrate the additional discrimination provided by the F1 channel in Manchester. The relationships between fluorescence intensities in different pairs of channels were also investigated as a function of DP. Differences between these metrics were apparent at each site and provide some distinction between the two datasets. Finally, particle selection criteria based on the Borneo dataset were applied to identify a median concentration of 10 "Borneo-like" fluorescent particles per litre in Manchester.
Tropopause height at 78° N 16° E: average seasonal variation 2007–2010

We present a seasonal climatology of tropopause altitude for 78° N 16° E derived from observations 2007–2010 by the SOUSY VHF radar on Svalbard. The spring minimum occurs one month later than that of surface air temperature and instead coincides with the maximum in ozone column density. This confirms similar studies based on radiosonde measurements in the arctic and demonstrates downward control by the stratosphere. If one is to exploit the potential of tropopause height as a metric for climate change at high latitude and elsewhere, it is imperative to observe and understand the processes which establish the tropopause – an understanding to which this study contributes.