Climate models and remote sensing retrievals generally assume that dust aerosols are spherical or spheroidal. However, measurements show that dust aerosols deviate substantially from spherical and spheroidal shapes, as ratios of particle length to width (the aspect ratio) and height to width (height‐to‐width ratio) deviate substantially from unity. Here, we quantify dust asphericity by compiling dozens of measurements of aspect ratio and height‐to‐width ratio across the globe. We find that the length is on average 5 times larger than the height and that climate models and remote sensing retrievals underestimate this asphericity by a factor of ~3–5. Compiled measurements further suggest that North African dust becomes more aspherical during transport, whereas Asian dust might become less aspherical. We obtain globally‐averaged shape distributions, from which we find that accounting for dust asphericity increases gravitational settling lifetime by ~20%. This increased lifetime helps explain the underestimation of coarse dust transport by models.
24 November 2015 in Atmospheric Chemistry and Physics
The seasonal cycle accounts for a dominant mode of total column CO2 (XCO2) annual variability and is connected to CO2 uptake and release; it thus represents an important quantity to test the accuracy of the measurements from space. We quantitatively evaluate the XCO2 seasonal cycle of the Greenhouse Gases Observing Satellite (GOSAT) observations from the Atmospheric CO2 Observations from Space (ACOS) retrieval system and compare average regional seasonal cycle features to those directly measured by the Total Carbon Column Observing Network (TCCON). We analyse the mean seasonal cycle amplitude, dates of maximum and minimum XCO2, as well as the regional growth rates in XCO2 through the fitted trend over several years. We find that GOSAT/ACOS captures the seasonal cycle amplitude within 1.0 ppm accuracy compared to TCCON, except in Europe, where the difference exceeds 1.0 ppm at two sites, and the amplitude captured by GOSAT/ACOS is generally shallower compared to TCCON. This bias over Europe is not as large for the other GOSAT retrieval algorithms (NIES v02.21, RemoTeC v2.35, UoL v5.1, and NIES PPDF-S v.02.11), although they have significant biases at other sites. We find that the ACOS bias correction partially explains the shallow amplitude over Europe. The impact of the co-location method and aerosol changes in the ACOS algorithm were also tested and found to be few tenths of a ppm and mostly non-systematic. We find generally good agreement in the date of minimum XCO2 between ACOS and TCCON, but ACOS generally infers a date of maximum XCO2 2–3 weeks later than TCCON. We further analyse the latitudinal dependence of the seasonal cycle amplitude throughout the Northern Hemisphere and compare the dependence to that predicted by current optimized models that assimilate in situ measurements of CO2. In the zonal averages, models are consistent with the GOSAT amplitude to within 1.4 ppm, depending on the model and latitude. We also show that the seasonal cycle of XCO2 depends on longitude especially at the mid-latitudes: the amplitude of GOSAT XCO2 doubles from western USA to East Asia at 45–50° N, which is only partially shown by the models. In general, we find that model-to-model differences can be larger than GOSAT-to-model differences. These results suggest that GOSAT/ACOS retrievals of the XCO2 seasonal cycle may be sufficiently accurate to evaluate land surface models in regions with significant discrepancies between the models.
Light scattering by light absorbing carbon (LAC) aggregates encapsulated into sulfate shells is computed by use of the discrete dipole method. Computations are performed for a UV, visible, and IR wavelength, different particle sizes, and volume fractions. Reference computations are compared to three classes of simplified model particles that have been proposed for climate modeling purposes. Neither model matches the reference results sufficiently well. Remarkably, more realistic core-shell geometries fall behind homogeneous mixture models. An extended model based on a core-shell-shell geometry is proposed and tested. Good agreement is found for total optical cross sections and the asymmetry parameter.
Optical properties of light absorbing carbon (LAC) aggregates encapsulated in a shell of sulfate are computed for realistic model geometries based on field measurements. Computations are performed for wavelengths from the UV-C to the mid-IR. Both climate- and remote sensing-relevant optical properties are considered. The results are compared to commonly used simplified model geometries, none of which gives a realistic representation of the distribution of the LAC mass within the host material and, as a consequence, fail to predict the optical properties accurately. A new core-gray shell model is introduced, which accurately reproduces the size- and wavelength dependence of the integrated and differential optical properties.
30 September 2011 in Journal of Quantitative Spectroscopy and Radiative Transfer