Aerosol Direct Radiative Impact Experiment (ADRIEX) overview

The Aerosol Direct Radiative Experiment (ADRIEX) took place over the Adriatic and Black Seas during August and September 2004 with the aim of characterizing anthropogenic aerosol in these regions in terms of its physical and optical properties and establishing its impact on radiative balance. Eight successful flights of the UK BAE-146 Facility for Atmospheric Airborne Measurements were completed together with surface-based lidar and AERONET measurements, in conjunction with satellite overpasses. This paper outlines the motivation for the campaign, the methodology and instruments used, describes the synoptic situation and provides an overview of the key results. ADRIEX successfully measured a range of aerosol conditions across the northern Adriatic, Po Valley and Black Sea. Generally two layers of aerosol were found in the vertical: in the flights over the Black Sea and the Po Valley these showed differences in chemical and microphysical properties, whilst over the Adriatic the layers were often more similar. Nitrate aerosol was found to be important in the Po Valley region. The use of new instruments to measure the aerosol chemistry and mixing state and to use this information in determining optical properties is demonstrated. These results are described in much more detail in the subsequent papers of this special issue.

Mapping and controlling molecular processes: The application of control theory and system identification algorithms to ASOPS and other fast pulse spectroscopies

Asynchronous Optical Sampling (ASOPS) [1,2] and frequency comb spectrometry [3] based on dual Ti:saphire resonators operated in a master/slave mode have the potential to improve signal to noise ratio in THz transient and IR sperctrometry. The multimode Brownian oscillator time-domain response function described by state-space models is a mathematically robust framework that can be used to describe the dispersive phenomena governed by Lorentzian, Debye and Drude responses. In addition, the optical properties of an arbitrary medium can be expressed as a linear combination of simple multimode Brownian oscillator functions. The suitability of a range of signal processing schemes adopted from the Systems Identification and Control Theory community for further processing the recorded THz transients in the time or frequency domain will be outlined [4,5]. Since a femtosecond duration pulse is capable of persistent excitation of the medium within which it propagates, such approach is perfectly justifiable. Several de-noising routines based on system identification will be shown. Furthermore, specifically developed apodization structures will be discussed. These are necessary because due to dispersion issues, the time-domain background and sample interferograms are non-symmetrical [6-8]. These procedures can lead to a more precise estimation of the complex insertion loss function. The algorithms are applicable to femtosecond spectroscopies across the EM spectrum. Finally, a methodology for femtosecond pulse shaping using genetic algorithms aiming to map and control molecular relaxation processes will be mentioned.

Interference filters and coatings for mid-infrared astronomy (8-30µm)

The VISIR instrument for the European Southern Observatory (ESO) Very Large Telescope (VLT) is a thermal-infrared imager and spectrometer currently being developed by the French Service d'Astrophysique of CEA Saclay, and Dutch NFRA ASTRON Dwingeloo consortium. This cryogenic instrument will employ precision infrared bandpass filters in the N-( =7.5-14µm) and Q-( =16-28µm) band mid-IR atmospheric windows to study interstellar and circumstellar environments crucial for star and planetary formation theories. As the filters in these mid-IR wavelength ranges are of interest to many astronomical cryogenic instruments, a worldwide astronomical filter consortium was set up with participation from 12 differing institutes, each requiring instrument specific filter operating environments and optical metrology. This paper describes the design and fabrication methods used to manufacture these astronomical consortium filters, including the rationale for the selection of multilayer coating designs, temperature-dependant optical properties of the filter materials and FTIR spectral measurements showing the changes in passband and blocking performance on cooling to <50K. We also describe the development of a 7-14µm broadband antireflection coating deposited on Ge lenses and KRS-5 grisms for cryogenic operation at 40K

Exposure to space radiation of high performance infrared multilayer filters and materials technology experiment

Infrared optical-multilayer filters and materials were exposed to the space environment of low Earth orbit on LDEF. This paper summarizes the effects of that environment on the physical and optical properties of the filters and materials flown.

Space exposure of infrared filters and materials on the NASA Long Duration Exposure Facility (LDEF)

Infrared optical-multilayer filters and materials were exposed to the space environment of low Earth for a period of nearly six years on the NASA Long Duration Exposure Facility (LDEF) mission. This report describes the effects of that environment on the physical and optical properties of filters and materials used in an experiment designed by the University of reading Infrared multilayer Laboratory. Results of the experiment comprise IR processed spectra both before (1983), and after (1990) exposure, in conjunction with unexposed control samples.

Durability assessment of PbTe/II-IV infrared filters (Space Shuttle 1st LDEF)

Residual stress having been further reduced, selected infrared coatings composed of thin films of (PbTe/ ZnS (or ZnSe) can now be made which comply with the durability requirements of MIL-48616 whilst retaining transparency. Such improved durability is due to the sequence:- i) controlled deposition, followed by ii) immediate exposure to air, followed by iii) annealing in vacuo to relieve stress. (At the time of writing we assume the empiric procedure "exposure to air/annealing in vacuo" acts to relieve the inherent stresses of deposition). As part of their testing, representative sample filters prepared by the procedure are being assembled for the shuttle's 1st Long Duration Exposure Facility (to be placed in earth orbit for a considerable period and then recovered for analysis). The sample filters comprise various narrowband-designs to permit deduction of the constituent thin film optical properties. The Reading assembly also contains representative sample of the infrared crystals, glasses, thin-film absorbers and bulk absorbers, and samples of shorter-wavelength filters prepared similarly but made with Ge/SiO. Findings on durability and transparency after exposure will be reported.

Motivation, rationale and key results from the GERBILS Saharan dust measurement campaign

The Geostationary Earth Radiation Budget Intercomparison of Longwave and Shortwave radiation (GERBILS) was an observational field experiment over North Africa during June 2007. The campaign involved 10 flights by the FAAM BAe-146 research aircraft over southwestern parts of the Sahara Desert and coastal stretches of the Atlantic Ocean. Objectives of the GERBILS campaign included characterisation of mineral dust geographic distribution and physical and optical properties, assessment of the impact upon radiation, validation of satellite remote sensing retrievals, and validation of numerical weather prediction model forecasts of aerosol optical depths (AODs) and size distributions. We provide the motivation behind GERBILS and the experimental design and report the progress made in each of the objectives. We show that mineral dust in the region is relatively non-absorbing (mean single scattering albedo at 550 nm of 0.97) owing to the relatively small fraction of iron oxides present (1–3%), and that detailed spectral radiances are most accurately modelled using irregularly shaped particles. Satellite retrievals over bright desert surfaces are challenging owing to the lack of spectral contrast between the dust and the underlying surface. However, new techniques have been developed which are shown to be in relatively good agreement with AERONET estimates of AOD and with each other. This encouraging result enables relatively robust validation of numerical models which treat the production, transport, and deposition of mineral dust. The dust models themselves are able to represent large-scale synoptically driven dust events to a reasonable degree, but some deficiencies remain both in the Sahara and over the Sahelian region, where cold pool outflow from convective cells associated with the intertropical convergence zone can lead to significant dust production.

Determining the contribution of volcanic ash and boundary layer aerosol in backscatter lidar returns: a three‐component atmosphere approach

A solution of the lidar equation is discussed, that permits combining backscatter and depolarization measurements to quantitatively distinguish two different aerosol types with different depolarization properties. The method has been successfully applied to simultaneous observations of volcanic ash and boundary layer aerosol obtained in Exeter, United Kingdom, on 16 and 18 April 2010, permitting the contribution of the two aerosols to be quantified separately. First a subset of the atmospheric profiles is used where the two aerosol types belong to clearly distinguished layers, for the purpose of characterizing the ash in terms of lidar ratio and depolarization. These quantities are then used in a three‐component atmosphere solution scheme of the lidar equation applied to the full data set, in order to compute the optical properties of both aerosol types separately. On 16 April a thin ash layer, 100–400 m deep, is observed (average and maximum estimated ash optical depth: 0.11 and 0.2); it descends from ∼2800 to ∼1400 m altitude over a 6‐hour period. On 18 April a double ash layer, ∼400 m deep, is observed just above the morning boundary layer (average and maximum estimated ash optical depth: 0.19 and 0.27). In the afternoon the ash is entrained into the boundary layer, and the latter reaches a depth of ∼1800 m (average and maximum estimated ash optical depth: 0.1 and 0.15). An additional ash layer, with a very small optical depth, was observed on 18 April at an altitude of 3500–4000 m. By converting the lidar optical measurements using estimates of volcanic ash specific extinction, derived from other works, the observations seem to suggest approximate peak ash concentrations of ∼1500 and ∼1000 mg/m3,respectively, on the two observations dates.

Impact of melt ponds on Arctic sea ice simulations from 1990 to 2007

The extent and thickness of the Arctic sea ice cover has decreased dramatically in the past few decades with minima in sea ice extent in September 2007 and 2011 and climate models did not predict this decline. One of the processes poorly represented in sea ice models is the formation and evolution of melt ponds. Melt ponds form on Arctic sea ice during the melting season and their presence affects the heat and mass balances of the ice cover, mainly by decreasing the value of the surface albedo by up to 20%. We have developed a melt pond model suitable for forecasting the presence of melt ponds based on sea ice conditions. This model has been incorporated into the Los Alamos CICE sea ice model, the sea ice component of several IPCC climate models. Simulations for the period 1990 to 2007 are in good agreement with observed ice concentration. In comparison to simulations without ponds, the September ice volume is nearly 40% lower. Sensitivity studies within the range of uncertainty reveal that, of the parameters pertinent to the present melt pond parameterization and for our prescribed atmospheric and oceanic forcing, variations of optical properties and the amount of snowfall have the strongest impact on sea ice extent and volume. We conclude that melt ponds will play an increasingly important role in the melting of the Arctic ice cover and their incorporation in the sea ice component of Global Circulation Models is essential for accurate future sea ice forecasts.

The global distribution of phytoplankton size spectrum and size classes from their light-absorption spectra derived from satellite data

The absorption spectra of phytoplankton in the visible domain hold implicit information on the phytoplankton community structure. Here we use this information to retrieve quantitative information on phytoplankton size structure by developing a novel method to compute the exponent of an assumed power-law for their particle-size spectrum. This quantity, in combination with total chlorophyll-a concentration, can be used to estimate the fractional concentration of chlorophyll in any arbitrarily-defined size class of phytoplankton. We further define and derive expressions for two distinct measures of cell size of mixed populations, namely, the average spherical diameter of a bio-optically equivalent homogeneous population of cells of equal size, and the average equivalent spherical diameter of a population of cells that follow a power-law particle-size distribution. The method relies on measurements of two quantities of a phytoplankton sample: the concentration of chlorophyll-a, which is an operational index of phytoplankton biomass, and the total absorption coefficient of phytoplankton in the red peak of visible spectrum at 676 nm. A sensitivity analysis confirms that the relative errors in the estimates of the exponent of particle size spectra are reasonably low. The exponents of phytoplankton size spectra, estimated for a large set of in situ data from a variety of oceanic environments (~ 2400 samples), are within a reasonable range; and the estimated fractions of chlorophyll in pico-, nano- and micro-phytoplankton are generally consistent with those obtained by an independent, indirect method based on diagnostic pigments determined using high-performance liquid chromatography. The estimates of cell size for in situ samples dominated by different phytoplankton types (diatoms, prymnesiophytes, Prochlorococcus, other cyanobacteria and green algae) yield nominal sizes consistent with the taxonomic classification. To estimate the same quantities from satellite-derived ocean-colour data, we combine our method with algorithms for obtaining inherent optical properties from remote sensing. The spatial distribution of the size-spectrum exponent and the chlorophyll fractions of pico-, nano- and micro-phytoplankton estimated from satellite remote sensing are in agreement with the current understanding of the biogeography of phytoplankton functional types in the global oceans. This study contributes to our understanding of the distribution and time evolution of phytoplankton size structure in the global oceans.

A model of melt pond evolution on sea ice

A one-dimensional, thermodynamic, and radiative model of a melt pond on sea ice is presented that explicitly treats the melt pond as an extra phase. A two-stream radiation model, which allows albedo to be determined from bulk optical properties, and a parameterization of the summertime evolution of optical properties, is used. Heat transport within the sea ice is described using an equation describing heat transport in a mushy layer of a binary alloy (salt water). The model is tested by comparison of numerical simulations with SHEBA data and previous modeling. The presence of melt ponds on the sea ice surface is demonstrated to have a significant effect on the heat and mass balance. Sensitivity tests indicate that the maximum melt pond depth is highly sensitive to optical parameters and drainage. INDEX TERMS: 4207 Oceanography: General: Arctic and Antarctic oceanography; 4255 Oceanography: General: Numerical modeling; 4299 Oceanography: General: General or miscellaneous; KEYWORDS: sea ice, melt pond, albedo, Arctic Ocean, radiation model, thermodynamic

Sensitivity of direct radiative forcing by mineral dust to particle characteristics

Airborne dust affects the Earth's energy balance — an impact that is measured in terms of the implied change in net radiation (or radiative forcing, in W m-2) at the top of the atmosphere. There remains considerable uncertainty in the magnitude and sign of direct forcing by airborne dust under current climate. Much of this uncertainty stems from simplified assumptions about mineral dust-particle size, composition and shape, which are applied in remote sensing retrievals of dust characteristics and dust-cycle models. Improved estimates of direct radiative forcing by dust will require improved characterization of the spatial variability in particle characteristics to provide reliable information dust optical properties. This includes constraints on: (1) particle-size distribution, including discrimination of particle subpopulations and quantification of the amount of dust in the sub-10 µm to <0.1 µm mass fraction; (2) particle composition, specifically the abundance of iron oxides, and whether particles consist of single or multi-mineral grains; (3) particle shape, including degree of sphericity and surface roughness, as a function of size and mineralogy; and (4) the degree to which dust particles are aggregated together. The use of techniques that measure the size, composition and shape of individual particles will provide a better basis for optical modelling.

Radiative forcing effect of ice-age dust

During glacial periods, dust deposition rates and inferred atmospheric concentrations were globally much higher than present. According to recent model results, the large enhancement of atmospheric dust content at the last glacial maximum (LGM) can be explained only if increases in the potential dust source areas are taken into account. Such increases are to be expected, due to effects of low precipitation and low atmospheric (CO2) on plant growth. Here the modelled three-dimensional dust fields from Mahowald et al. and modelled seasonally varying surface-albedo fields derived in a parallel manner, are used to quantify the mean radiative forcing due to modern (non-anthropogenic) and LGM dust. The effect of mineralogical provenance on the radiative properties of the dust is taken into account, as is the range of optical properties associated with uncertainties about the mixing state of the dust particles. The high-latitude (poleward of 45°) mean change in forcing (LGM minus modern) is estimated to be small (–0.9 to +0.2 W m–2), especially when compared to nearly –20 W m–2 due to reflection from the extended ice sheets. Although the net effect of dust over ice sheets is a positive forcing (warming), much of the simulated high-latitude dust was not over the ice sheets, but over unglaciated regions close to the expanded dust source region in central Asia. In the tropics the change in forcing is estimated to be overall negative, and of similarly large magnitude (–2.2 to –3.2 W m–2) to the radiative cooling effect of low atmospheric (CO2). Thus, the largest long-term climatic effect of the LGM dust is likely to have been a cooling of the tropics. Low tropical sea-surface temperatures, low atmospheric (CO2) and high atmospheric dust loading may be mutually reinforcing due to multiple positive feedbacks, including the negative radiative forcing effect of dust.

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)Wm−2 at the top of atmosphere (TOA) and (−12±6)Wm−2 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.

Aerosol scattering and absorption during the EUCAARI-LONGREX flights of the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146: can measurements and models agree?

Scattering and absorption by aerosol in anthropogenically perturbed air masses over Europe has been measured using instrumentation flown on the UK’s BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM) on 14 flights during the EUCAARI-LONGREX campaign in May 2008. The geographical and temporal variations of the derived shortwave optical properties of aerosol are presented. Values of single scattering albedo of dry aerosol at 550 nm varied considerably from 0.86 to near unity, with a campaign average of 0.93 ± 0.03. Dry aerosol optical depths ranged from 0.030 ± 0.009 to 0.24 ± 0.07. An optical properties closure study comparing calculations from composition data and Mie scattering code with the measured properties is presented. Agreement to within measurement uncertainties of 30% can be achieved for both scattering and absorption,but the latter is shown to be sensitive to the refractive indices chosen for organic aerosols, and to a lesser extent black carbon, as well as being highly dependent on the accuracy of the absorption measurements. Agreement with the measured absorption can be achieved either if organic carbon is assumed to be weakly absorbing, or if the organic aerosol is purely scattering and the absorption measurement is an overestimate due to the presence of large amounts of organic carbon. Refractive indices could not be inferred conclusively due to this uncertainty, despite the enhancement in methodology compared to previous studies that derived from the use of the black carbon measurements. Hygroscopic growth curves derived from the wet nephelometer indicate moderate water uptake by the aerosol with a campaign mean f (RH) value (ratio in scattering) of 1.5 (range from 1.23 to 1.63) at 80% relative humidity. This value is qualitatively consistent with the major chemical components of the aerosol measured by the aerosol mass spectrometer, which are primarily mixed organics and nitrate and some sulphate.