Saharan dust absorption and refractive index from aircraft-based observations during SAMUM 2006

During the Saharan Mineral Dust Experiment (SAMUM) conducted in summer 2006 in southeast Morocco, the complex refractive index of desert dust was determined from airborne measurements of particle size distributions and aerosol absorption coefficients at three different wavelengths in the blue (467 nm), green (530 nm) and red (660 nm) spectral regions. The vertical structure of the dust layers was analysed by an airborne high spectral resolution lidar (HSRL). The origin of the investigated dust layers was estimated from trajectory analyses, combined with Meteosat 2nd Generation (MSG) scenes and wind field data analyses. The real part n of the dust refractive index was found almost constant with values between 1.55 and 1.56, independent of the wavelength. The values of the imaginary part k varied between the blue and red spectral regions by a factor of three to ten depending on the dust source region. Absolute values of k ranged from 3.1 × 10⁻³ to 5.2 × 10⁻³ at 450 nm and from 0.3 × 10⁻³ to 2.5 × 10⁻³ at 700 nm. Groupings of k values could be attributed to different source regions.     

Broadband extinction method to determine atmospheric aerosol optical properties

The equivalent wavelength ( λ _E), at which the aerosol optical depth (AOD) is equal to broadband AOD (BAOD), can change in a wide range from 0.619 μm to 1.575 μm in the usual aerosol conditions. By using the least squares technique and some empirical corrections, a parameterized relationship of λ _E with BAOD, Ångström wavelength exponent ( α ), solar zenith angle ( θ ₀) and H₂O amount is developed. Using this relationship, and based on the strong sensitivity of BAOD on θ ₀ when θ ₀>70°, the broadband extinction method to derive the spectral AOD and α is further proposed. As shown in comparative simulations to retrieve AOD by the present, Molineaux et al. and Gueymard methods, the present method has the best accuracy in most simulations using Junge, MODTRAN, log‐normal and Deirmendjian aerosol models. A key question of the pyrheliometer method to determine wavelength-dependent AODs is the effect of uncertainty in the aerosol size istribution. It is found that the AOD solution around λ _E is less sensitive to the uncertainty. The wavelength exponent α is derived using an assumption of the stable atmospheric turbidity. If the pyrheliometer data from θ ₀=85° to 70° are used and the change of the turbidity is ±10%, the error of solution α is usually within ±0.32. If the variation of the turbidity is random, the mean value of a lot of the measurements of α would be very reasonable.     

Properties of dust aerosol particles transported to Portugal from the Sahara desert

Aerosol properties of mineral particles in the far field of an African desert dust outbreak were investigated that brought Saharan dust over the Mediterranean in different layers to Portugal. The measurements were performed inside the project Desert Aerosols over Portugal (DARPO) which was linked to the Saharan Mineral Dust Experiment (SAMUM). The maximum particle mass concentration was about 150 μg m⁻³ and the corresponding scattering coefficient was 130 M m⁻¹ which results in a mass scattering efficiency of 0.87 m² g⁻¹. The aerosol optical depth reached values up to 0.53 and the lidar ratio was between 45 and 50 in the whole dust loaded column. A comparison between particle size distributions and refractive indices derived from different instruments and models showed a general good agreement but some minor differences could also be observed. Measurements as well as calculations with a particle transport model suggest that there is a relatively higher concentration of very large particles in the upper region of the dust layer than on the surface which is likely connected with meteorological conditions at the observational site (Évora, Portugal).     

Spatial distribution and optical properties of Saharan dust observed by airborne high spectral resolution lidar during SAMUM 2006

Airborne measurements of pure Saharan dust extinction and backscatter coefficients, the corresponding lidar ratio and the aerosol optical thickness (AOT) have been performed during the Saharan Mineral Dust Experiment 2006, with a high spectral resolution lidar. Dust layers were found to range from ground up to 4–6 km above sea level (asl). Maximum AOT values at 532 nm, encountered within these layers during the DLR Falcon research flights were 0.50–0.55. A significant horizontal variability of the AOT south of the High Atlas mountain range was observed even in cases of a well-mixed dust layer. High vertical variations of the dust lidar ratio of 38–50 sr were observed in cases of stratified dust layers. The variability of the lidar ratio was attributed to dust advection from different source regions. The aerosol depolarization ratio was about 30% at 532 nm during all measurements and showed only marginal vertical variations.     

Investigation of parameters controlling the soil sink of atmospheric molecular hydrogen

Enclosure measurements have been performed on a bare mineral soil at an experimental field site near Heidelberg, Germany. From observed molecular hydrogen (H₂) mixing ratio changes in the enclosure, deposition velocities were calculated ranging from  8.4 × 10⁻³  to  8.2 × 10⁻² cm s⁻¹  and with an annual mean value of  3.1 × 10⁻² cm s⁻¹  . In the studied range of  2– 27 °C  , the uptake showed a significant temperature dependence. However, this turned out not to be the primary driving mechanism of the uptake flux. Soil moisture content, co-varying with temperature, was identified as the major parameter being responsible for the diffusive permeability of H₂ in the soil and the final rate of H₂ uptake. A simple Millington–Quirk diffusion model approach could largely explain this behaviour and yielded a diffusion path length of H₂ in the studied soil of only 0.2–1.8 cm, suggesting that total H₂ consumption occurs within the first few centimetres of the soil. The diffusion model, when applied to continuous measurements of soil moisture content, atmospheric pressure, temperature and the mixing ratio of H₂ in the atmosphere, could largely reproduce the measured deposition flux densities, assuming a mean thickness of the diffusion path length of 0.7 cm.     

Spectral absorption coefficients and imaginary parts of refractive indices of Saharan dust during SAMUM-1

During the SAMUM-1 experiment, absorption coefficients and imaginary parts of refractive indices of mineral dust particles were investigated in southern Morocco. Main absorbing constituents of airborne samples were identified to be iron oxide and soot. Spectral absorption coefficients were measured using a spectral optical absorption photometer (SOAP) in the wavelength range from 300 to 800 nm with a resolution of 50 nm. A new method that accounts for a loading-dependent correction of fibre filter based absorption photometers, was developed. The imaginary part of the refractive index was determined using Mie calculations from 350 to 800 nm. The spectral absorption coefficient allowed a separation between dust and soot absorption. A correlation analysis showed that the dust absorption coefficient is correlated ( R ² up to 0.55) with the particle number concentration for particle diameters larger than 0.5 μm, whereas the coefficient of determination R ² for smaller particles is below 0.1. Refractive indices were derived for both the total aerosol and a dust aerosol that was corrected for soot absorption. Average imaginary parts of refractive indices of the entire aerosol are 7.4 × 10⁻³, 3.4 × 10⁻³ and 2.0 × 10⁻³ at wavelengths of 450, 550 and 650 nm. After a correction for the soot absorption, imaginary parts of refractive indices are 5.1 × 10⁻³, 1.6 × 10⁻³ and 4.5 × 10⁻⁴.     

Airborne measurements of dust layer properties, particle size distribution and mixing state of Saharan dust during SAMUM 2006

The Saharan Mineral Dust Experiment (SAMUM) was conducted in May/June 2006 in southern Morocco. As part of SAMUM, airborne in situ measurements of the particle size distribution in the diameter range 4 nm < D _p < 100 μm were conducted. The aerosol mixing state was determined below D _p < 2.5 μm. Furthermore, the vertical structure of the dust layers was investigated with a nadir-looking high spectral resolution lidar (HSRL). The desert dust aerosol exhibited two size regimes of different mixing states: below 0.5 μm, the particles had a non-volatile core and a volatile coating; larger particles above 0.5 μm consisted of non-volatile components and contained light absorbing material. In all cases, particles larger than 10 μm were present, and in 80% of the measurements no particles larger than 40 μm were present. The abundance of large particles showed almost no height dependence. The effective diameter D _eff in the dust plumes investigated showed two main ranges: the first range of D _eff peaked around 5 μm and the second range of D _eff around 8 μm. The two ranges of D _eff suggest that it may be inadequate to use one average effective diameter or one parametrization for a typical dust size distribution.     

Spectral surface albedo over Morocco and its impact on radiative forcing of Saharan dust

In May–June 2006, airborne and ground-based solar (0.3–2.2 μm) and thermal infrared (4–42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m⁻² per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m⁻² were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between −19 and +24 W m⁻² for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect.     

Vertical profiling of Saharan dust with Raman lidars and airborne HSRL in southern Morocco during SAMUM

Three ground-based Raman lidars and an airborne high-spectral-resolution lidar (HSRL) were operated during SAMUM 2006 in southern Morocco to measure height profiles of the volume extinction coefficient, the extinction-to-backscatter ratio and the depolarization ratio of dust particles in the Saharan dust layer at several wavelengths. Aerosol Robotic Network (AERONET) Sun photometer observations and radiosoundings of meteorological parameters complemented the ground-based activities at the SAMUM station of Ouarzazate. Four case studies are presented. Two case studies deal with the comparison of observations of the three ground-based lidars during a heavy dust outbreak and of the ground-based lidars with the airborne lidar. Two further cases show profile observations during satellite overpasses on 19 May and 4 June 2006. The height resolved statistical analysis reveals that the dust layer top typically reaches 4–6 km height above sea level (a.s.l.), sometimes even 7 km a.s.l.. Usually, a vertically inhomogeneous dust plume with internal dust layers was observed in the morning before the evolution of the boundary layer started. The Saharan dust layer was well mixed in the early evening. The 500 nm dust optical depth ranged from 0.2–0.8 at the field site south of the High Atlas mountains, Ångström exponents derived from photometer and lidar data were between 0–0.4. The volume extinction coefficients (355, 532 nm) varied from 30–300 Mm⁻¹ with a mean value of 100 Mm⁻¹ in the lowest 4 km a.s.l.. On average, extinction-to-backscatter ratios of 53–55 sr (±7–13 sr) were obtained at 355, 532 and 1064 nm.     

Boron isotope variations in the atmosphere

We report here the first measurements of boron isotope ratios in the maritime atmosphere together with those of precipitation. The δ¹¹B values of atmospheric condensates in the western North Pacific and Japanese coast and snow in Tokyo range from −12.8 to +5.1‰ and from −0.4 to +0.4‰, respectively, which are significantly lower than those of rainwater (+18.9 to +34.7‰) collected mostly over the North Pacific. Since the ¹¹B/¹⁰B ratios of the atmosphere are lower than those of volcanic emissions (δ¹¹B=+2.3 to +21.4‰), we must seek sources for atmospheric boron other than volcanism. We postulate that the sea may be an important supplier for atmospheric boron under some dynamic conditions and that boron isotope fractionation during evaporation from seawater and removal from the atmosphere may account for the large variations of ¹¹B/¹⁰B ratios observed in the atmosphere and precipitation.     

Vertically resolved dust optical properties during SAMUM: Tinfou compared to Ouarzazate

Vertical profiles of dust key optical properties are presented from measurements during the Saharan Mineral Dust Experiment (SAMUM) by Raman and depolarization lidar at two ground-based sites and by airborne high spectral resolution lidar. One of the sites, Tinfou, is located close to the border of the Sahara in Southern Morocco and was the main in situ site during SAMUM. The other site was Ouarzazate airport, the main lidar site. From the lidar measurements the spatial distribution of the dust between Tinfou and Ouarzazate was derived for 1 d. The retrieved profiles of backscatter and extinction coefficients and particle depolarization ratios show comparable dust optical properties, a similar vertical structure of the dust layer, and a height of about 4 km asl at both sites. The airborne cross-section of the extinction coefficient at the two sites confirms the low variability in dust properties. Although the general picture of the dust layer was similar, the lidar measurements reveal a higher dust load closer to the dust source. Nevertheless, the observed intensive optical properties were the same. These results indicate that the lidar measurements at two sites close to the dust source are both representative for the SAMUM dust conditions.     

Vertical profiles of biospheric and fossil fuel-derived CO2 and fossil fuel CO2 : CO ratios from airborne measurements of Δ14C, CO2 and CO above Colorado, USA

Measurements of  Δ¹⁴C  in atmospheric CO₂ are an effective method of separating CO₂ additions from fossil fuel and biospheric sources or sinks of CO₂. We illustrate this technique with vertical profiles of CO₂ and  Δ¹⁴C  analysed in whole air flask samples collected above Colorado, USA in May and July 2004. Comparison of lower tropospheric composition to cleaner air at higher altitudes (>5 km) revealed considerable additions from respiration in the morning in both urban and rural locations. Afternoon concentrations were mainly governed by fossil fuel emissions and boundary layer depth, also showing net biospheric CO₂ uptake in some cases. We estimate local industrial CO₂:CO emission ratios using in situ measurements of CO concentration. Ratios are found to vary by 100% and average 57 mole CO₂:1 mole CO, higher than expected from emissions inventories. Uncertainty in CO₂ from different sources was ±1.1 to ±4.1 ppm for addition or uptake of −4.6 to 55.8 ppm, limited by  Δ¹⁴C  measurement precision and uncertainty in background  Δ¹⁴C  and CO₂ levels.     

Reconciliation of excess 14C-constrained global CO2 piston velocity estimates

Oceanic excess radiocarbon data is widely used as a constraint for air–sea gas exchange. However, recent estimates of the global mean piston velocity  〈 k 〉  from Naegler et al., Krakauer et al., Sweeney et al. and Müller et al. differ substantially despite the fact that they all are based on excess radiocarbon data from the GLODAP data base. Here I show that these estimates of  〈 k 〉  can be reconciled if first, the changing oceanic radiocarbon inventory due to net uptake of CO₂ is taken into account; second, if realistic reconstructions of sea surface  Δ¹⁴C  are used and third, if  〈 k 〉  is consistently reported with or without normalization to a Schmidt number of 660. These corrections applied, unnormalized estimates of  〈 k 〉  from these studies range between 15.1 and 18.2 cm h⁻¹. However, none of these estimates can be regarded as the only correct value for  〈 k 〉  . I thus propose to use the 'average' of the corrected values of  〈 k 〉  presented here (16.5 ± 3.2 cm h⁻¹) as the best available estimate of the global mean unnormalized piston velocity  〈 k 〉  , resulting in a gross ocean-to-atmosphere CO₂ flux of 76 ± 15 PgC yr⁻¹ for the mid-1990s.     

In situ measurements of optical properties at Tinfou (Morocco) during the Saharan Mineral Dust Experiment SAMUM 2006

In situ measurements of optical and physical properties of mineral dust were performed at the outskirts of the Saharan Desert in the framework of the Saharan Mineral Dust Experiment part 1 (SAMUM-1). Goals of the field study were to achieve information on the extent and composition of the dust particle size distribution and the optical properties of dust at the ground. For the particle number size distribution, measured with a DMPS/APS, a size dependent dynamic shape factor was considered. The mean refractive index of the particles in this field study is  1.53–4.1 × 10⁻³ i   at 537 nm wavelength and  1.53–3.1 × 10⁻³ i   at 637 nm wavelength derived from measurements of scattering and absorption coefficients, as well as the particle size distribution. Whereas the real part of the refractive index is rather constant, the imaginary part varies depending on the mineral dust concentrations. For high dust concentration the single scattering albedo is primarily influenced by iron oxide and is  0.96 ± 0.02  and  0.98 ± 0.01  at 537 nm and 637 nm wavelength, respectively. During low dust concentration the single scattering albedo is more influenced by a soot-type absorber and is  0.89 ± 0.02  and  0.93 ± 0.01  for the same wavelengths.     

The retrieval of the Asian dust depolarization ratio in Korea with the correction of the polarization-dependent transmission

The linear particle depolarization ratios were retrieved from the observation with a multiwavelength Raman lidar at the Gwangju Institute of Science and Technology (GIST), Korea (35.11°N, 126.54°E). The measurements were carried out in spring (March to May) 2011. The transmission ratio measurements were performed to solve problems of the depolarization-dependent transmission at a receiver of the lidar and applied to correct the retrieved depolarization ratio of Asian dust at first time in Korea. The analyzed data from the GIST multiwavelength Raman lidar were classified into three categories according to the linear particle depolarization ratios, which are pure Asian dust on 21 March, the intermediate case which means Asian dust mixed with urban pollution on 13 May, and haze case on 10 April. The measured transmission ratios were applied to these cases respectively. We found that the transmission ratio is needed to be used to retrieve the accurate depolarization ratio of Asian dust and also would be useful to distinguish the mixed dust particles between intermediate case and haze. The particle depolarization ratios of pure Asian dust were approximately 0.25 at 532 nm and 0.14 at 532 nm for the intermediate case. The linear particle depolarization ratios of pure Asian dust observed with the GIST multiwavelength Raman lidar were compared to the linear particle depolarization ratios of Saharan dust observed in Morocco and Asian dust observed both in Japan and China.     

Diurnal variation of CO2 concentration, Δ14C and δ13C in an urban forest: estimate of the anthropogenic and biogenic CO2 contributions

Diurnal variation in the atmospheric CO₂ concentration and the carbon isotopic composition (Δ¹⁴C and δ¹³C) was measured in a forest in an urban area on 9 February 1999. The carbon isotope approach used in the present study differentiated between the quantitative contributions from anthropogenic and biogenic CO₂ sources in the urban atmosphere. The anthropogenic (fossil fuel) and biogenic (soil respiration) contributions was estimated, and they ranged from 1 to 16% and from 2 to 8% of the total atmospheric CO₂. The diurnal variation of the anthropogenic CO₂ was the major cause of the total atmospheric CO₂ variation, while the biogenic CO₂ remained relatively constant throughout the day. Estimating the contribution of soil respired CO₂ provided the mean residence time of soil respired CO₂ within the forest atmosphere.     

Physical characterization of aerosol particles during nucleation events

Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm⁻³ and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm⁻³. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm⁻³, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm⁻³, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.     

Assessment of the soil CO2 gradient method for soil CO2 efflux measurements: comparison of six models in the calculation of the relative gas diffusion coefficient

This paper uses a refined soil gradient method to estimate soil CO₂ efflux. Six different models are used to determine the relative gas diffusion coefficient (ξ). A weighted harmonic averaging is used to estimate the soil CO₂ diffusion coefficient, yielding a better estimate of soil CO₂ efflux. The resulting soil CO₂ efflux results are then compared to the soil CO₂ efflux measured with a soil chamber. Depending on the choice of ξ model used, the estimated soil CO₂ efflux using the gradient method reasonably approximates the efflux obtained using the soil chamber method. In addition, the estimated soil CO₂ efflux obtained by this improved method is well described by an exponential function of soil temperature at a depth of 0.05 m with the temperature sensitivity ( Q ₁₀) of 1.81 and a linear function of soil moisture at a depth of 0.12 m, in general agreement with previous findings. These results suggest that the gradient method is a practical cost-effective means to measure soil CO₂ emissions. Results from the present study suggest that the gradient method can be used successfully to measure soil CO₂ efflux provided that proper attention is paid to the judicious use of the proper diffusion coefficient.     

Vertical profiles and storage fluxes of CO2, heat and water in a tropical rainforest at Pasoh, Peninsular Malaysia

Ambient CO₂ concentration, air temperature and relative humidity were measured intermittently for a 3-year period from the floor to the canopy top of a tropical rainforest in Pasoh, Peninsular Malaysia. Mean diurnal CO₂ storage flux ( S _c; μmol m⁻² s⁻¹) and sensible and latent heat storage fluxes ( Q _a and Q _w; W m⁻²) ranged from −12.7 to 3.2 μmol m⁻² s⁻¹, −15 to 27 W m⁻² and −10 to 20 W m⁻², respectively. Small differences in diurnal changes were observed in S _c and Q _a between the driest and wettest periods. Compared with the ranges of mean diurnal CO₂ eddy flux (−14.7 to 4.9 μmol m⁻² s⁻¹), sensible eddy flux (−12 to 169 W m⁻²) and latent eddy flux (0 to 250 W m⁻²), the contribution of CO₂ storage flux was especially large. Comparison with summertime data from a temperate Japanese cypress forest suggested a higher contribution of S _c in the tropical rainforest, probably mainly due to the difference in nighttime friction velocity at the sites. On the other hand, differences in Q _a and Q _w were smaller than the difference in S _c, probably because of the smaller nighttime sinks/sources of heat and water vapour.     

Chemical effect of carbonaceous aerosols on the diurnal cycle of MBL ozone at a tropical site: measurements and simulations

During late austral summer and winter 1998, black carbon (BC) aerosols were monitored with an Aethalometer at 2 sites of La Réunion Island (Indian Ocean): Saint‐Denis, the main city and Sainte‐Rose, a quite uninhabited region situated at the east coast. BC concentration data at Saint‐Denis show a marked diurnal cycle, which may be primarily attributed to traffic. The background data found at night‐time display average BC concentrations, ranging from about 80 to 250 ng/m³ whereas during the day, BC concentrations increase by a factor of at least 4. In comparison, BC concentrations vary in the range of 10 to 60 ng/m³ at Sainte‐Rose. Ozone concentration was also measured at Saint‐Denis using a Dasibi photometer and found to be at significant levels (means: 16.5–23 ppbv in April and 28.5–34 ppbv in September). A noticeable increase of ozone concentrations during the day points out the build‐up of pollutants enhancing photochemical transformations. However, during traffic pollution peaks, ozone concentration displays systematic depletion. The comparison of ozone and BC measurements at both seasons points to some possible effects of heterogeneous interaction of ozone and its precursors with BC particles. These interactions were also simulated with a 0D time‐dependent chemistry model using conditions of a polluted site. The measured ozone concentration characteristics (mean concentration and range of variation) are well simulated in the presence of BC. Our model results show that at La Réunion Island adsorption of ozone and its precursors onto BC aerosol particles could be one of the important steps determining ozone concentration characteristics, especially in absence of photochemistry during night‐time.