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  • Evaluating MODIS cloud retrievals with in situ observations from VOCALS-REx

    Microphysical measurements collected during eleven profiles, by the UK BAe-146 aircraft, through marine stratocumulus as part of the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) are compared to collocated overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Aqua and Terra satellite platforms. The full depth of the cloud is sampled in each case using a Cloud Droplet Probe (CDP) and a Two-Dimensional Stereo Probe (2DS) together sizing cloud and precipitation droplets in the diameter range 2–1260 μm. This allows the total optical depth (&tau;<sub>c</sub>) of the cloud and effective radius (<I>r</I><sub>e</sub>) of the droplet size distribution to be compared to MODIS cloud retrievals of the same quantities along with the secondarily derived total liquid water path. When compared to the effective radius at cloud top, the MODIS retrieved <I>r</I><sub>e</sub> using the 2.1 μm wavelength channel overestimates the in situ measurements on average by 13% with the largest overestimations coinciding with the detection by the 2DS of drizzle sized droplets. We show through consideration of the full vertical profile and penetration depths of the wavelengths used in the retrieval that the expected retrieved values are less than those at cloud top thus increasing the apparent bias in <I>r</I><sub>e</sub> retrievals particularly when using the 1.6 and 2.1 μm channels, with the 3.7 μm channel retrievals displaying the best agreement with in situ values. Retrievals of &tau;<sub>c</sub> also tend to overestimate in situ values which, coupled with a high bias in <I>r</I><sub>e</sub> retrievals, lead to an overestimation of liquid water path. There is little apparent correlation between the variation of the three near-infrared <I>r</I><sub>e</sub> retrievals and the vertical structure of the cloud observed in situ. Retrievals are performed using measured profiles of water vapour and temperature along with an accurate knowledge of the width of the droplet size distribution which improve agreement between in situ and retrieved values but cannot completely explain the observed biases. Additionally we show that cloud heterogeneity and three-dimensional radiative effects may high skew the mean when averaging over comparison domains but cannot explain all of the apparent high bias. An intercomparison between in situ measurements from the BAe-146 and C-130 platforms is also presented, highlighting the uncertainties associated with in situ observations.
  • The Arctic response to remote and local forcing of black carbon

    Recent studies suggest that the Arctic temperature response to black carbon (BC) forcing depend strongly on the location of the forcing. We investigate how atmospheric BC in the mid-latitudes remotely influence the Arctic climate, and compare this with the response to atmospheric BC located in the Arctic itself. In this study, idealized climate simulations are carried out with a fully coupled Earth System Model, which includes a comprehensive treatment of aerosol microphysics. In order to determine how BC transported to the Arctic and BC sources not reaching the Arctic impact the Arctic climate, atmospheric BC concentrations are scaled up in the mid-latitudes (28–60° N) and in the Arctic (60–90° N), respectively. Estimates of the impact on the Arctic energy budget are represented by analyzing radiation fluxes at the top of the atmosphere and at the surface, surface turbulent fluxes, and meridional heat transport in the atmosphere. Our calculations show that increased BC forcing in the Arctic atmosphere reduces the surface air temperature in the Arctic with a corresponding increase in the sea-ice fraction, despite the increased planetary absorption of sunlight. The analysis indicates that this effect is due to a combination of a weakening of the northward heat transport caused by a reduction in the meridional temperature gradient and a dimming at the surface. On the other hand we find that BC forcing at the mid-latitudes warms the Arctic surface significantly and decreases the sea-ice fraction. Our model calculations indicate that atmospheric BC forcing outside the Arctic may be more important for the Arctic climate change than the forcing in the Arctic itself. These results suggest that mitigation strategies for the Arctic climate should also address BC sources in locations outside the Arctic even if they do not contribute much to BC in the Arctic.
  • Fluorescent biological aerosol particles measured with the Waveband Integrated Bioaerosol Sensor WIBS-4: laboratory tests combined with a one year field study

    In this paper bioaerosol measurements conducted with the Waveband Integrated Bioaerosol Sensor mark 4 (WIBS-4) are presented. The measurements comprise aerosol chamber characterization experiments and a one-year ambient measurement period at a semi-rural site in South Western Germany. This study aims to investigate the sensitivity of WIBS-4 to biological and non-biological aerosols and detection of biological particles in the ambient aerosol. Several types of biological and non-biological aerosol samples, including fungal spores, bacteria, mineral dust, ammonium sulphate, combustion soot, and fluorescent polystyrene spheres, were analyzed by WIBS-4 in the laboratory. The results confirm the sensitivity of the ultraviolet light-induced fluorescence (UV-LIF) method to biological fluorophores and show the good discrimination capabilities of the two excitation wavelengths/detection wavebands method applied in WIBS-4. However, a weak cross-sensitivity to non-biological fluorescent interferers remains and is discussed in this paper. <br><br> All the laboratory studies have been undertaken in order to prepare WIBS-4 for ambient aerosol measurements. According to the one-year ambient aerosol study, number concentration of fluorescent biological aerosol particles (FBAP) show strong seasonal and diurnal variability. The highest number concentration of FBAP was measured during the summer term and decreased towards the winter period when colder and drier conditions prevail. Diurnal FBAP concentrations start to increase after sunset and reach maximum values during the late night and early morning hours. On the other hand, the total aerosol number concentration was almost always higher during daytime than during nighttime and a sharp decrease after sunset was observed. There was no correlation observed between the FBAP concentration and the meteorological parameters temperature, precipitation, wind direction and wind speed. However, a clear correlation was identified between the FBAP number concentration and the relative humidity. Humidity-controlled release mechanisms of some fungal spore species are discussed as a possible explanation.
  • Efficient determination of vehicle emission factors by fuel use category using on-road measurements: downward trends on Los Angeles freight corridor I-710

    To evaluate the success of vehicle emissions regulations, trends in both fleet-wide average emissions as well as high-emitter emissions are needed, but it is challenging to capture the full spread of vehicle emission factors (EFs) with chassis dynamometer or tunnel studies, and remote sensing studies cannot evaluate particulate compounds. We developed an alternative method that links real-time on-road pollutant measurements from a mobile platform with real-time traffic data, and allows efficient calculation of both the average and the spread of EFs for light-duty gasoline-powered vehicles (LDG) and heavy-duty diesel-powered vehicles (HDD). This is the first study in California to report EFs under a full range of real-world driving conditions on multiple freeways. Fleet average LDG EFs were in agreement with most recent studies and an order of magnitude lower than observed HDD EFs. HDD EFs reflected the relatively rapid decreases in diesel emissions that have recently occurred in Los Angeles/California, and on I-710, a primary route used for goods movement and a focus of additional truck fleet turnover incentives, HDD EFs were often lower than on other freeways. When freeway emission rates (ER) were quantified as the product of EF and vehicle miles traveled (VMT) per time per mile of freeway, despite a two- to three-fold difference in HDD fractions between freeways, ERs were found to be generally similar in magnitude. Higher LDG VMT on low HDD fraction freeways largely offset the difference. Therefore, the conventional assumption that freeways with the highest HDD fractions are significantly worse sources of total emissions in Los Angeles may no longer be~true.
  • Optical properties of Saharan dust aerosol and contribution from the coarse mode as measured during the Fennec 2011 aircraft campaign

    New in-situ aircraft measurements of Saharan dust originating from Mali, Mauritania and Algeria taken during the Fennec 2011 aircraft campaign over a remote part of the Sahara Desert are presented. Size distributions extending to 300 μm are shown, representing measurements extending further into the coarse mode than previously published for airborne Saharan dust. A significant coarse mode was present in the size distribution measurements with effective diameter (<i>d</i><sub>eff</sub>) from 2.3 to 19.4 μm and coarse mode volume median diameter (<i>d</i><sub>vc</sub>) from 5.8 to 45.3 μm. The mean size distribution had a larger relative proportion of coarse mode particles than previous aircraft measurements. The largest particles (with <i>d</i><sub>eff</sub> > 12 μm, or <i>d</i><sub>vc</sub> > 25 μm) were only encountered within 1 km of the ground. Number concentration, mass loading and extinction coefficient showed inverse relationships to dust age since uplift. Dust particle size showed a weak exponential relationship to dust age. Two cases of freshly uplifted dust showed quite different characteristics of size distribution and number concentration. <br><br> Single Scattering Albed (SSA) values at 550 nm calculated from the measured size distributions revealed high absorption ranging from 0.70 to 0.97 depending on the refractive index. SSA was found to be strongly related to <i>d</i><sub>eff</sub>. New instrumentation revealed that direct measurements, behind Rosemount inlets, overestimate SSA by up to 0.11 when <i>d</i><sub>eff</sub> is greater than 2 μm. This is caused by aircraft inlet inefficiencies and sampling losses. Previous measurements of SSA from aircraft measurements may also have been overestimates for this reason. Radiative transfer calculations indicate that the range of SSAs during Fennec 2011 can lead to underestimates in shortwave atmospheric heating rates by 2.0 to 3.0 times if the coarse mode is neglected. This will have an impact on Saharan atmospheric dynamics and circulation, which should be taken into account by numerical weather prediction and climate models.
  • Source apportionment of ambient fine particle from combined size distribution and chemical composition data during summertime in Beijing

    Continuous particle number concentration and chemical composition data were collected over one month during summertime in Beijing to investigate the source apportionment of ambient fine particles. Particle size distributions from 15 nm to 2.5 μm in diameter and composition data, such as organic matter, sulfate, nitrate, ammonium, chlorine, and gaseous pollutants, were analyzed using positive matrix factorisation (PMF) which indentified eight factors: cooking, solid mode exhaust, nucleation mode exhaust, accumulation mode, secondary nitrate, secondary sulfate, coal-fired power plant and road dust. Nearly two-thirds of particle number concentrations were attributed to cooking (22.8%) and motor vehicle (37.5%), whereas road dust, coal-fired power plant and regional sources contributed 69.0% to particle volume concentrations. Local and remote sources were distinguished using size distributions associated with each factor. Local sources were generally characterised by unimodal or bimodal number distributions, consisting mostly of particles less 0.1 μm in diameter, and regional sources were defined by mostly accumulation mode particles. Nearly one third of secondary nitrate and secondary sulfate was transported from the surrounding areas of Beijing during study period. Overall the introduction of combination of particle number concentration and chemical composition in PMF model is successful at separating the components and quantifying relative contributions to the particle number and volume population in a complex urban atmosphere.
  • New particle formation in the western Yangtze River Delta: first data from SORPES-station

    Aerosols and new particle formation were studied in the western part of the Yangtze River Delta (YRD), at the SORPES station of Nanjing University. Air ions between 0.8 and 42 nm were measured using an air ion spectrometer; a DMPS provided particle size distributions between 6 and 800 nm. Additionally, meteorological data, trace gas concentrations, and PM<sub>2.5</sub> values were recorded. During the measurement period from 18 November 2011 to 31 March 2012, the mean total particle concentration was found to be 23 000 cm<sup>&minus;3</sup>. The mean PM<sub>2.5</sub> value was 90 &mu; g m<sup>&minus;3</sup>, well above national limits. During the observations, 26 new particle formation events occurred, typically producing 6 nm particles at a rate of 1 cm<sup>&minus;3</sup> s<sup>&minus;1</sup>, resulting in over 4000 cm<sup>&minus;3</sup> new CCN per event. Typical growth rates were between 6 and 7 nm h<sup>&minus;1</sup>. Ion measurements showed the typical cluster band below 2 nm, with total ion concentrations roughly between 600 and 1000 cm<sup>&minus;3</sup>. A peculiar feature of the ion measurements were the heightened ion cluster concentrations during the nights before event days. The highly polluted air of the YRD provides both the potential source (SO<sub>2</sub>) and the sink (particulate matter) for sulfuric acid, leaving radiation as the determining force behind new particle formation. Accordingly, a good correlation was found between new particle formation rate and radiation values.
  • Regional and monthly and clear-sky aerosol direct radiative effect (and forcing) derived from the GlobAEROSOL-AATSR satellite aerosol product

    Using the GlobAEROSOL-AATSR dataset, estimates of the instantaneous, clear-sky, direct aerosol radiative effect and radiative forcing have been produced for the year 2006. Aerosol Robotic Network sun-photometer measurements have been used to characterise the random and systematic error in the GlobAEROSOL product for 22 regions covering the globe. Representative aerosol properties for each region were derived from the results of a wide range of literature sources and, along with the de-biased GlobAEROSOL AODs, were used to drive an offline version of the Met Office unified model radiation scheme. In addition to the mean AOD, best-estimate run of the radiation scheme, a range of additional calculations were done to propagate uncertainty estimates in the AOD, optical properties, surface albedo and errors due to the temporal and spatial averaging of the AOD fields. This analysis produced monthly, regional estimates of the clear-sky aerosol radiative effect and its uncertainty, which were combined to produce annual, global mean values of (−6.7 ± 3.9) W m<sup>−2</sup> at the top of atmosphere (TOA) and (−12 ± 6) W m<sup>−2</sup> at the surface. These results were then used to give estimates of regional, clear-sky aerosol direct radiative forcing, using modelled pre-industrial AOD fields for the year 1750 calculated for the AEROCOM PRE experiment. However, as it was not possible to quantify the uncertainty in the pre-industrial aerosol loading, these figures can only be taken as indicative and their uncertainties as lower bounds on the likely errors. Although the uncertainty on aerosol radiative effect presented here is considerably larger than most previous estimates, the explicit inclusion of the major sources of error in the calculations suggest that they are closer to the true constraint on this figure from similar methodologies, and point to the need for more, improved estimates of both global aerosol loading and aerosol optical properties.
  • Using measurements of the aerosol charging state in determination of the particle growth rate and the proportion of ion-induced nucleation

    The fraction of charged nucleation mode particles as a function of particle diameter depends on the particle growth rate and the proportion of particles formed via ion-induced nucleation. In this study we have tested the applicability of recent data analysis methods to determine the growth rate and the proportion of ion-induced nucleation from the measured charged fractions. For this purpose we have conducted a series of aerosol dynamic simulations covering a wide range of atmospheric conditions. The growth rate and initial fraction of charged particles were estimated from simulated data using these methods and compared with the values obtained directly from the simulations. We found that the data analysis methods used in this study should not be used when the nuclei growth rate is less than ~3 nm h<sup>−1</sup>, or when charged particles grow much more rapidly than neutral ones. Furthermore, we found that the difference in removal rates of neutral and charged particles should be taken into account when estimating the proportion of ion-induced nucleation. Neglecting the higher removal rate of charged particles compared with that of neutral ones could result in an underestimation of the proportion of ion-induced nucleation by up to a factor of 2. This underestimation is further increased if charged particles grow more rapidly than neutral ones. We also provided a simple way of assessing whether these methods are suitable for analyzing data measured under specific conditions. The assessment procedure was illustrated using a few examples of actual measurement sites with a more detailed examination of the typical conditions observed at the SMEAR II station in Hyytiälä, Finland.
  • Idealized WRF model sensitivity simulations of sea breeze types and their effects on offshore windfields

    The behaviour and characteristics of the marine component of sea breeze cells have received little attention relative to their onshore counterparts. Yet there is a growing interest and dependence on the offshore wind climate from, for example, a wind energy perspective. Using idealized model experiments, we investigate the sea breeze circulation at scales which approximate to those of the southern North Sea, a region of major ongoing offshore wind farm development. We also contrast the scales and characteristics of the <i>pure</i> and the little known <i>corkscrew</i> and <i>backdoor</i> sea breeze types, where the type is pre-defined by the orientation of the synoptic scale flow relative to the shoreline. We find, crucially, that <i>pure</i> sea breezes, in contrast to <i>corkscrew</i> and <i>backdoor</i> types, can lead to substantial wind speed reductions offshore and that the addition of a second eastern coastline emphasises this effect through generation of offshore "calm zones". The offshore extent of all sea breeze types is found to be sensitive to both the influence of Coriolis acceleration and to the boundary layer scheme selected. These extents range, for example for a <i>pure</i> sea breeze produced in a 2 m s<sup>&minus;1</sup> offshore gradient wind, from 0 km to 21 km between the Mellor-Yamada-Nakanishi-Niino and the Yonsei State University schemes respectively. The <i>corkscrew</i> type restricts the development of a <i>backdoor</i> sea breeze on the opposite coast and is also capable of traversing a 100 km offshore domain even under high along-shore gradient wind speed (>15 m s<sup>&minus;1</sup>) conditions. Realistic variations in sea surface skin temperature and initializing vertical thermodynamic profile do not significantly alter the resulting circulation, though the strengths of the simulated sea breezes are modulated if the effective land-sea thermal contrast is altered. We highlight how sea breeze impacts on circulation need to be considered in order to improve the accuracy of both assessments of the offshore wind energy climate and forecasts of wind energy output.
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