Spectrally invariant approximation within atmospheric radiative transfer

Certain algebraic combinations of single scattering albedo and solar radiation reflected from, or transmitted through, vegetation canopies do not vary with wavelength. These ‘‘spectrally invariant relationships’’ are the consequence of wavelength independence of the extinction coefficient and scattering phase function in veg- etation. In general, this wavelength independence does not hold in the atmosphere, but in cloud-dominated atmospheres the total extinction and total scattering phase function vary only weakly with wavelength. This paper identifies the atmospheric conditions under which the spectrally invariant approximation can accu- rately describe the extinction and scattering properties of cloudy atmospheres. The validity of the as- sumptions and the accuracy of the approximation are tested with 1D radiative transfer calculations using publicly available radiative transfer models: Discrete Ordinate Radiative Transfer (DISORT) and Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART). It is shown for cloudy atmospheres with cloud optical depth above 3, and for spectral intervals that exclude strong water vapor absorption, that the spectrally invariant relationships found in vegetation canopy radiative transfer are valid to better than 5%. The physics behind this phenomenon, its mathematical basis, and possible applications to remote sensing and climate are discussed.

Aerosol absorption over the clear-sky oceans deduced from POLDER-1 and AERONET observations

We estimate aerosol absorption over the clear-sky oceans using aerosol geophysical products from POLDER-1 space measurements and absorption properties from ground-based AERONET measurements. Our best estimate is 2.5 Wm-2 averaged over the 8-month lifetime of POLDER-1. Low and high absorption estimates are 2.2 and 3.1 Wm-2 based on the variability in aerosol single scattering albedo observed by AERONET. Main sources of uncertainties are the discrimation of the aerosol type from satellite measurements, and potential clear-sky bias induced by the cloud-screening procedure.

In situ and remote-sensing measurements of the mean microphysical and optical properties of industrial pollution aerosol during ADRIEX

We present a summary of the principal physical and optical properties of aerosol particles using the FAAM BAE-146 instrumented aircraft during ADRIEX between 27 August and 6 September 2004, augmented by sunphotometer, lidar and satellite retrievals. Observations of anthropogenic aerosol, principally from industrial sources, were concentrated over the northern Adriatic Sea and over the Po Valley close to the aerosol sources. An additional flight was also carried out over the Black Sea to compare east and west European pollution. Measurements show the single-scattering albedo of dry aerosol particles to vary considerably between 0.89 and 0.97 at a wavelength of 0.55 μm, with a campaign mean within the polluted lower free troposphere of 0.92. Although aerosol concentrations varied significantly from day to day and during individual days, the shape of the aerosol size distribution was relatively consistent through the experiment, with no detectable change observed over land and over sea. There is evidence to suggest that the pollution aerosol within the marine boundary layer was younger than that in the elevated layer. Trends in the aerosol volume distribution show consistency with multiple-site AERONET radiometric observations. The aerosol optical depths derived from aircraft measurements show a consistent bias to lower values than both the AERONET and lidar ground-based radiometric observations, differences which can be explained by local variations in the aerosol column loading and by some aircraft instrumental artefacts. Retrievals of the aerosol optical depth and fine-mode (<0.5 μm radius) fraction contribution to the optical depth using MODIS data from the Terra and Aqua satellites show a reasonable level of agreement with the AERONET and aircraft measurements.

General circulation model estimates of aerosol transport and radiative forcing during the Indian Ocean Experiment

Aerosol sources, transport, and sinks are simulated, and aerosol direct radiative effects are assessed over the Indian Ocean for the Indian Ocean Experiment (INDOEX) Intensive Field Phase during January to March 1999 using the Laboratoire de Me´te´orologie Dynamique (LMDZT) general circulation model. The model reproduces the latitudinal gradient in aerosol mass concentration and optical depth (AOD). The model-predicted aerosol concentrations and AODs agree reasonably well with measurements but are systematically underestimated during high-pollution episodes, especially in the month of March. The largest aerosol loads are found over southwestern China, the Bay of Bengal, and the Indian subcontinent. Aerosol emissions from the Indian subcontinent are transported into the Indian Ocean through either the west coast or the east coast of India. Over the INDOEX region, carbonaceous aerosols are the largest contributor to the estimated AOD, followed by sulfate, dust, sea salt, and fly ash. During the northeast winter monsoon, natural and anthropogenic aerosols reduce the solar flux reaching the surface by 25 W m�2, leading to 10–15% less insolation at the surface. A doubling of black carbon (BC) emissions from Asia results in an aerosol single-scattering albedo that is much smaller than in situ measurements, reflecting the fact that BC emissions are not underestimated in proportion to other (mostly scattering) aerosol types. South Asia is the dominant contributor to sulfate aerosols over the INDOEX region and accounts for 60–70% of the AOD by sulfate. It is also an important but not the dominant contributor to carbonaceous aerosols over the INDOEX region with a contribution of less than 40% to the AOD by this aerosol species. The presence of elevated plumes brings significant quantities of aerosols to the Indian Ocean that are generated over Africa and Southeast and east Asia.

Host model uncertainties in aerosol radiative forcing estimates: results from the AeroCom Prescribed intercomparison study

Simulated multi-model “diversity” in aerosol direct radiative forcing estimates is often perceived as a measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated “host-model uncertainties” are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in twelve participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is −4.47Wm−2 and the inter-model standard deviation is 0.55Wm−2, corresponding to a relative standard deviation of 12 %. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.04Wm−2, and the standard deviation increases to 1.01W−2, corresponding to a significant relative standard deviation of 97 %. However, the top-of-atmosphere forcing variability owing to absorption (subtracting the scattering case from the case with scattering and absorption) is low, with absolute (relative) standard deviations of 0.45Wm−2 (8 %) clear-sky and 0.62Wm−2 (11 %) all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the Aero- Com Direct Effect experiment demonstrates that host model uncertainties could explain about 36% of the overall sulfate forcing diversity of 0.11Wm−2 in the AeroCom Direct Radiative Effect experiment.

Synergistic angular and spectral estimation of aerosol properties using CHRIS/PROBA-1 and simulated Sentinel-3~data

A method has been developed to estimate Aerosol Optical Depth (AOD), Fine Mode Fraction (FMF) and Single Scattering Albedo (SSA) over land surfaces using simulated Sentinel-3 data. The method uses inversion of a coupled surface/atmosphere radiative transfer model, and includes a general physical model of angular surface reflectance. An iterative process is used to determine the optimum value of the aerosol properties providing the best fit of the corrected reflectance values for a number of view angles and wavelengths with those provided by the physical model. A method of estimating AOD using only angular retrieval has previously been demonstrated on data from the ENVISAT and PROBA-1 satellite instruments, and is extended here to the synergistic spectral and angular sampling of Sentinel-3 and the additional aerosol properties. The method is tested using hyperspectral, multi-angle Compact High Resolution Imaging Spectrometer (CHRIS) images. The values obtained from these CHRIS observations are validated using ground based sun-photometer measurements. Results from 22 image sets using the synergistic retrieval and improved aerosol models show an RMSE of 0.06 in AOD, reduced to 0.03 over vegetated targets.

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 (deff) from 2.3 to 19.4 μm and coarse mode volume median diameter (dvc) 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 deff >12 μm, or dvc >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. 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 deff. New instrumentation revealed that direct measurements, behind Rosemount inlets, overestimate SSA by up to 0.11 when deff 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.

Impact of atmospheric transport on the evolution of microphysical and optical properties of Saharan dust

Saharan dust affects the climate by altering the radiation balance and by depositing minerals to the Atlantic Ocean. Both are dependent on particle size. We present aircraft measurements comprising 42 profiles of size distribution (0.1–300 µm), representing freshly uplifted dust, regional aged dust, and dust in the Saharan Air Layer (SAL) over the Canary Islands. The mean effective diameter of dust in SAL profiles is 4.5 µm smaller than that in freshly uplifted dust, while the vertical structure changes from a low shallow layer (0–1.5 km) to a well-mixed deep Saharan dust layer (0–5 km). Size distributions show a loss of 60 to 90% of particles larger than 30 µm 12 h after uplift. The single scattering albedo (SSA) increases from 0.92 to 0.94 to 0.95 between fresh, aged, and SAL profiles: this is enough to alter heating rates by 26%. Some fresh dust close to the surface shows SSA as low as 0.85

A new data set of soil mineralogy for dust-cycle modeling

The mineralogy of airborne dust affects the impact of dust particles on direct and indirect radiative forcing, on atmospheric chemistry and on biogeochemical cycling. It is determined partly by the mineralogy of the dust-source regions and partly by size-dependent fractionation during erosion and transport. Here we present a data set that characterizes the clay and silt-sized fractions of global soil units in terms of the abundance of 12 minerals that are important for dust–climate interactions: quartz, feldspars, illite, smectite, kaolinite, chlorite, vermiculite, mica, calcite, gypsum, hematite and goethite. The basic mineralogical information is derived from the literature, and is then expanded following explicit rules, in order to characterize as many soil units as possible. We present three alternative realizations of the mineralogical maps, taking the uncertainties in the mineralogical data into account. We examine the implications of the new database for calculations of the single scattering albedo of airborne dust and thus for dust radiative forcing.

Synergistic angular and spectral estimation of aerosol properties using CHRIS/PROBA-1 and simulated Sentinel-3 data

We develop a method to derive aerosol properties over land surfaces using combined spectral and angular information, such as available from ESA Sentinel-3 mission, to be launched in 2015. A method of estimating aerosol optical depth (AOD) using only angular retrieval has previously been demonstrated on data from the ENVISAT and PROBA-1 satellite instruments, and is extended here to the synergistic spectral and angular sampling of Sentinel-3. The method aims to improve the estimation of AOD, and to explore the estimation of fine mode fraction (FMF) and single scattering albedo (SSA) over land surfaces by inversion of a coupled surface/atmosphere radiative transfer model. The surface model includes a general physical model of angular and spectral surface reflectance. An iterative process is used to determine the optimum value of the aerosol properties providing the best fit of the corrected reflectance values to the physical model. The method is tested using hyperspectral, multi-angle Compact High Resolution Imaging Spectrometer (CHRIS) images. The values obtained from these CHRIS observations are validated using ground-based sun photometer measurements. Results from 22 image sets using the synergistic retrieval and improved aerosol models show an RMSE of 0.06 in AOD, reduced to 0.03 over vegetated targets.

Airborne measurements of trace gases and aerosols over the London metropolitan region

The Emissions around the M25 motorway (EM25) campaign took place over the megacity of London in the United Kingdom in June 2009 with the aim of characterising trace gas and aerosol composition and properties entering and emitted from the urban region. It featured two mobile platforms, the UK BAe-146 Facility for Airborne Atmospheric Measurements (FAAM) research aircraft and a ground-based mobile lidar van, both travelling in circuits around London, roughly following the path of the M25 motorway circling the city. We present an overview of findings from the project, which took place during typical UK summertime pollution conditions. Emission ratios of volatile organic compounds (VOCs) to acetylene and carbon monoxide emitted from the London region were consistent with measurements in and downwind of other large urban areas and indicated traffic and associated fuel evaporation were major sources. Sub-micron aerosol composition was dominated by secondary species including sulphate (24% of sub-micron mass in the London plume and 29% in the non-plume regional aerosol), nitrate (24% plume; 20% regional) and organic aerosol (29% plume; 31% regional). The primary sub-micron aerosol emissions from London were minor compared to the larger regional background, with only limited increases in aerosol mass in the urban plume compared to the background (~12% mass increase on average). Black carbon mass was the major exception and more than doubled in the urban plume, leading to a decrease in the single scattering albedo from 0.91 in the regional aerosol to 0.86 in the London plume, on average. Our observations indicated that regional aerosol plays a major role on aerosol concentrations around London, at least during typical summertime conditions, meaning future efforts to reduce PM levels in London must account for regional as well as local aerosol sources.

Comparison of aerosol optical properties above clouds between POLDER and AeroCom models over the South East Atlantic Ocean during the fire season

Aerosol properties above clouds have been retrieved over the South East Atlantic Ocean during the fire season 2006 using satellite observations from POLDER (Polarization and Directionality of Earth Reflectances). From June to October, POLDER has observed a mean Above-Cloud Aerosol Optical Thickness (ACAOT) of 0.28 and a mean Above-Clouds Single Scattering Albedo (ACSSA) of 0.87 at 550 nm. These results have been used to evaluate the simulation of aerosols above clouds in 5 AeroCom (Aerosol Comparisons between Observations and Models) models (GOCART, HadGEM3, ECHAM5-HAM2, OsloCTM2 and SPRINTARS). Most models do not reproduce the observed large aerosol load episodes. The comparison highlights the importance of the injection height and the vertical transport parameterizations to simulate the large ACAOT observed by POLDER. Furthermore, POLDER ACSSA is best reproduced by models with a high imaginary part of black carbon refractive index, in accordance with recent recommendations.

Downwelling solar irradiance in the biomass burning region of the southern Amazon: Dependence on aerosol intensive optical properties and role of water vapor

The sensitivity of solar irradiance at the surface to the variability of aerosol intensive optical properties is investigated for a site (Alta Floresta) in the southern portion of the Amazon basin using detailed comparisons between measured and modeled irradiances. Apart from aerosol intensive optical properties, specifically single scattering albedo (omega(o lambda)) and asymmetry parameter (g(lambda)), which were assumed constant, all other relevant input to the model were prescribed based on observation. For clean conditions, the differences between observed and modeled irradiances were consistent with instrumental uncertainty. For polluted conditions, the agreement was significantly worse, with a root mean square difference three times larger (23.5 Wm(-2)). Analysis revealed a noteworthy correlation between the irradiance differences (observed minus modeled) and the column water vapor (CWV) for polluted conditions. Positive differences occurred mostly in wet conditions, while the differences became more negative as the atmosphere dried. To explore the hypothesis that the irradiance differences might be linked to the modulation of omega(o lambda) and g(lambda) by humidity, AERONET retrievals of aerosol properties and CWV over the same site were analyzed. The results highlight the potential role of humidity in modifying omega(o lambda) and g(lambda) and suggest that to explain the relationship seen between irradiances differences via aerosols properties the focus has to be on humidity-dependent processes that affect particles chemical composition. Undoubtedly, there is a need to better understand the role of humidity in modifying the properties of smoke aerosols in the southern portion of the Amazon basin.

Characterization of the optical properties of atmospheric aerosols in Amazonia from long-term AERONET monitoring (1993-1995 and 1999-2006)

We present a new climatology of atmospheric aerosols (primarily pyrogenic and biogenic) for the Brazilian tropics on the basis of a high-quality data set of spectral aerosol optical depth and directional sky radiance measurements from Aerosol Robotic Network (AERONET) Cimel Sun-sky radiometers at more than 15 sites distributed across the Amazon basin and adjacent Cerrado region. This network is the only long-term project (with a record including observations from more than 11 years at some locations) ever to have provided ground-based remotely-sensed column aerosol properties for this critical region. Distinctive features of the Amazonian area aerosol are presented by partitioning the region into three aerosol regimes: southern Amazonian forest, Cerrado, and northern Amazonian forest. The monitoring sites generally include measurements from the interval 1999-2006, but some sites have measurement records that date back to the initial days of the AERONET program in 1993. Seasonal time series of aerosol optical depth (AOD), angstrom ngstrom exponent, and columnar-averaged microphysical properties of the aerosol derived from sky radiance inversion techniques (single-scattering albedo, volume size distribution, fine mode fraction of AOD, etc.) are described and contrasted for the defined regions. During the wet season, occurrences of mineral dust penetrating deep into the interior were observed.

MODIS aerosol optical depth Retrievals with high spatial resolution over an urban area using the critical reflectance

[1] The retrieval of aerosol optical depth (Ta) over land by satellite remote sensing is still a challenge when a high spatial resolution is required. This study presents a tool that uses satellite measurements to dynamically identify the aerosol optical model that best represents the optical properties of the aerosol present in the atmosphere. We use aerosol critical reflectance to identify the single scattering albedo of the aerosol layer. Two case studies show that the Sao Paulo region can have different aerosol properties and demonstrates how the dynamic methodology works to identify those differences to obtain a better T a retrieval. The methodology assigned the high single scattering albedo aerosol model (pi o( lambda = 0.55) = 0.90) to the case where the aerosol source was dominated by biomass burning and the lower pi(o) model (pi(o) (lambda = 0.55) = 0.85) to the case where the local urban aerosol had the dominant influence on the region, as expected. The dynamic methodology was applied using cloud-free data from 2002 to 2005 in order to retrieve Ta with Moderate Resolution Imaging Spectroradiometer ( MODIS). These results were compared with collocated data measured by AERONET in Sao Paulo. The comparison shows better results when the dynamic methodology using two aerosol optical models is applied (slope 1.06 +/- 0.08 offset 0.01 +/- 0.02 r(2) 0.6) than when a single and fixed aerosol model is used (slope 1.48 +/- 0.11 and offset - 0.03 +/- 0.03 r(2) 0.6). In conclusion the dynamical methodology is shown to work well with two aerosol models. Further studies are necessary to evaluate the methodology in other regions and under different conditions.