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Although essential to fully understand the cycling of mercury at the global scale, mercury species records in the Southern Hemisphere are scarce. Under the framework of the Global Mercury Observation System (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48´ S, 77°34´ E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2-year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 ng m<sup>−3</sup>) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m<sup>−3</sup>, range: < detection limit–4.07 pg m<sup>−3</sup>; and mean: 0.67 pg m<sup>−3</sup>, range: < detection limit–12.67 pg m<sup>−3</sup>, respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets from July to September during the biomass burning season. Low concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique data set provides new baseline GEM concentrations in the Southern Hemisphere midlatitudes while mercury speciation along with upcoming wet deposition data will help to improve our understanding of the mercury cycle in the marine boundary layer.
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Vertical redistribution of HNO<sub>3</sub> through large HNO<sub>3</sub>-containing particles associated with polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. During the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) campaign, apparently very large NAT (nitric acid trihydrate) particles were observed by the airborne in situ probe FSSP-100 (Molleker et al., 2014). Our analysis shows that the FSSP-100 observations associated with the flight on 25 January 2010 cannot easily be explained assuming compact spherical NAT particles due to much too short growing time at temperatures below the existence temperature of NAT (<i>T</i><sub>NAT</sub>). State-of-the-art simulations using CLaMS (Chemical Lagrangian Model of the Stratosphere; Grooß et al., 2014) suggest considerably smaller particles. We consider the hypothesis that the simulation reproduces the NAT particle masses in a realistic way, but that real NAT particles may have larger apparent sizes compared to compact spherical particles, e.g. due to non-compact morphology or aspheric shape. Our study focuses on the consequence that such particles would have reduced settling velocities compared to compact spheres, altering the vertical redistribution of HNO<sub>3</sub>. Utilising CLaMS simulations, we investigate the impact of reduced settling velocities of NAT particles on vertical HNO<sub>3</sub> redistribution and compare the results with observations of gas-phase HNO<sub>3</sub> by the airborne Fourier transform spectrometer MIPAS-STR associated with two RECONCILE flights. The MIPAS-STR observations confirm conditions consistent with denitrification by NAT particles for the flight on 25 January 2010 and show good agreement with the simulations within the limitations of the comparison. Best agreement is found if settling velocities between 100 and 50% relative to compact spherical particles are considered (slight preference for the 70% scenario). In contrast, relative settling velocities of 30% result in too weak vertical HNO<sub>3</sub> redistribution. Sensitivity simulations considering temperature biases of ±1 K and multiplying the simulated nucleation rates by factors of 0.5 and 2.0 affect the comparisons to a similar extent, but result in no effective improvement compared to the reference scenario. Our results show that an accurate knowledge of the settling velocities of NAT particles is important for quantitative simulations of vertical HNO<sub>3</sub> redistribution.
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Smoke aerosols from biomass burning are an important component of the global aerosol system. Analysis of Aerosol Robotic Network (AERONET) retrievals of aerosol microphysical/optical parameters at 10 sites reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke observed at coastal/island AERONET sites also mostly lie within the range of variability at the near-source sites. Differences between sites tend to be larger than variability at an individual site, although optical properties for some sites in different regions can be quite similar. Across the sites, typical midvisible SSA ranges from ~ 0.95–0.97 (sites dominated by boreal forest or peat burning, typically with larger fine-mode particle radius and spread) to ~ 0.88–0.9 (sites most influenced by grass, shrub, or crop burning, typically smaller fine-mode particle radius and spread). The tropical forest site Alta Floresta (Brazil) is closer to this second category, although with intermediate SSA ~ 0.92. The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average midvisible SSA ~ 0.85. Sites with stronger absorption also tend to have stronger spectral gradients in SSA, becoming more absorbing at longer wavelengths. Microphysical/optical models are presented in detail so as to facilitate their use in radiative transfer calculations, including extension to UV (ultraviolet) wavelengths, and lidar ratios. One intended application is to serve as candidate optical models for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean often have insufficient absorption (i.e. too high SSA) to represent these biomass burning aerosols. The underestimates in satellite-retrieved AOD in smoke outflow regions, which have important consequences for applications of these satellite data sets, are consistent with the level of underestimated absorption.
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This study addresses and attempts to mitigate persistent uncertainty and scatter among existing approaches for determining the rate of sea spray aerosol production by breaking waves in the open ocean. The new approach proposed here utilizes passive microwave emissions from the ocean surface, which are known to be sensitive to surface roughness and foam. Direct, simultaneous, and collocated measurements of the aerosol production and microwave emissions were collected aboard the <i>FLoating Instrument Platform</i> (<i>FLIP</i>) in deep water ~ 150 km off the coast of California over a period of ~ 4 days. Vertical profiles of coarse-mode aerosol (0.25–23.5 μm) concentrations were measured with a forward-scattering spectrometer and converted to surface flux using dry deposition and vertical gradient methods. Back-trajectory analysis of eastern North Pacific meteorology verified the clean marine origin of the sampled air mass over at least 5 days prior to measurements. Vertical and horizontal polarization surface brightness temperature were measured with a microwave radiometer at 10.7 GHz frequency. Data analysis revealed a strong sensitivity of the brightness temperature polarization difference to the rate of aerosol production. An existing model of microwave emission from the ocean surface was used to determine the empirical relationship and to attribute its underlying physical basis to microwave emissions from surface roughness and foam within active and passive phases of breaking waves. A possibility of and initial steps towards satellite retrievals of the sea spray aerosol production are briefly discussed in concluding remarks.
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During the July 2011 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field experiment in Maryland, significant enhancements in Aerosol Robotic Network (AERONET) sun–sky radiometer measured aerosol optical depth (AOD) were observed in the immediate vicinity of non-precipitating cumulus clouds on some days. Both measured Ångström exponents and aerosol size distribution retrievals made before, during and after cumulus development often suggest little change in fine mode particle size; therefore, implying possible new particle formation in addition to cloud processing and humidification of existing particles. In addition to sun–sky radiometer measurements of large enhancements of fine mode AOD, lidar measurements made from both ground-based and aircraft-based instruments during the experiment also measured large increases in aerosol signal at altitudes associated with the presence of fair weather cumulus clouds. These data show modifications of the aerosol vertical profile as a result of the aerosol enhancements at and below cloud altitudes. The airborne lidar data were utilized to estimate the spatial extent of these aerosol enhancements, finding increased AOD, backscatter and extinction out to 2.5 km distance from the cloud edge. Furthermore, in situ measurements made from aircraft vertical profiles over an AERONET site during the experiment also showed large increases in aerosol scattering and aerosol volume after cloud formation as compared to before. The 15-year AERONET database of AOD measurements at the Goddard Space Flight Center (GSFC), Maryland site, was investigated in order to obtain a climatological perspective of this phenomenon of AOD enhancement. Analysis of the diurnal cycle of AOD in summer showed significant increases in AOD from morning to late afternoon, corresponding to the diurnal cycle of cumulus development.
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Optical properties of aerosols were measured from the GAW Puy de Dôme station (1465 m) over a seven year period (2006–2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010–2011). The analysis of the spatial and temporal variability of the optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the PBL height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type. At 90% humidity, the scattering factor enhancement (<i>f</i>σ<sub>sca</sub>) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH = 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type.
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We present a detailed budget of the changes in atmospheric aerosol mass and numbers due to various processes: emission (including instant condensation of soluble biogenic emissions), nucleation, coagulation, H<sub>2</sub>SO<sub>4</sub> condensation and in-cloud production, aging and deposition. The budget is created from monthly averaged tracer tendencies calculated by the global aerosol model ECHAM5.5-HAM2 and allows us to investigate process contributions at various length-scales and timescales. As a result, we show in unprecedented detail what processes drive the evolution of aerosol. In particular, we show that the processes that affect aerosol masses are quite different from those that affect aerosol numbers. Condensation of H<sub>2</sub>SO<sub>4</sub> gas onto pre-existing particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the aging of hydrophobic matter. Together with in-cloud production of H<sub>2</sub>SO<sub>4</sub>, it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. As expected, the coarse mode is dominated by primary emissions and mostly decoupled from the smaller modes. Our analysis also suggests that coagulation serves mainly as a loss process for number densities and that, relative to other processes, it is a rather unimportant contributor to composition changes of aerosol. The analysis is extended with sensitivity studies where the impact of a lower model resolution or pre-industrial emissions is shown to be small. We discuss the use of the current budget for model simplification, prioritization of model improvements, identification of potential structural model errors and model evaluation against observations.
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Vertical profiles of aerosol extinction coefficients were measured by a micro-pulse lidar at Naqu (31.5° N, 92.1° E; 4508 m a.m.s.l.), a meteorological station located on the central part of the Tibetan Plateau during summer 2011. Observations show a persistent maximum in aerosol extinction coefficients in the upper troposphere–lower stratosphere (UTLS). These aerosol layers were generally located at an altitude of 18–19 km a.m.s.l., 1–2 km higher than the tropopause, with broad layer depth ranging approximately 3–4 km and scattering ratio of 4–9. Daily averaged aerosol optical depths (AODs) of the enhanced aerosol layers in UTLS over the Tibetan Plateau varied from 0.007 to 0.030, in agreement with globally averaged levels of 0.018 ± 0.009 at 532 nm from previous observations, but the percentage contributions of the enhanced aerosol layers to the total AOD over the Tibetan Plateau are higher than those observed elsewhere. The aerosol layers in UTLS wore off gradually with the reducing intensity of the Asian monsoon over the Tibetan Plateau at the end of August. The eruption of Nabro volcano on 13 June 2011 is considered an important factor to explain the enhancement of tropopause aerosols observed this summer over the Tibetan Plateau.
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This work describes improvements in the regional aerosol–climate model REMO-HAM in order to simulate more realistically the process of atmospheric new particle formation (NPF). A new scheme was implemented to simulate OH radical concentrations using a proxy approach based on observations and also accounting for the effects of clouds upon OH concentrations. Second, the nucleation rate calculation was modified to directly simulate the formation rates of 3 nm particles, which removes some unnecessary steps in the formation rate calculations used earlier in the model. Using the updated model version, NPF over Europe was simulated for the periods 2003–2004 and 2008–2009. The statistics of the simulated particle formation events were subsequently compared to observations from 13 ground-based measurement sites. The new model shows improved agreement with the observed NPF rates compared to former versions and can simulate the event statistics realistically for most parts of Europe.
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Black carbon (BC) in snow lowers its albedo, increasing the absorption of sunlight, leading to positive radiative forcing, climate warming and earlier snowmelt. A series of recent studies have used prescribed-aerosol deposition flux fields in climate model runs to assess the forcing by black carbon in snow. In these studies, the prescribed mass deposition flux of BC to surface snow is decoupled from the mass deposition flux of snow water to the surface. Here we compare prognostic- and prescribed-aerosol runs and use a series of offline calculations to show that the prescribed-aerosol approach results, on average, in a factor of about 1.5–2.5 high bias in annual-mean surface snow BC mixing ratios in three key regions for snow albedo forcing by BC: Greenland, Eurasia and North America. These biases will propagate directly to positive biases in snow and surface albedo reduction by BC. The bias is shown be due to coupling snowfall that varies on meteorological timescales (daily or shorter) with prescribed BC mass deposition fluxes that are more temporally and spatially smooth. The result is physically non-realistic mixing ratios of BC in surface snow. We suggest that an alternative approach would be to prescribe BC mass mixing ratios in snowfall, rather than BC mass fluxes, and we show that this produces more physically realistic BC mixing ratios in snowfall and in the surface snow layer.
