Abstract. Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003). An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE) method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths) with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities), even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal) size distributions naturally differ from the correct bimodal values, the associated surface area (A) and volume densities (V) are, nevertheless, fairly accurately retrieved, except at values larger than 1.0 μm2 cm−3 (A) and 0.05 μm3 cm−3 (V), where they tend to underestimate the true bimodal values. Due to the limited information content in the SAGE II spectral extinction measurements this kind of forward model error cannot be avoided here. Nevertheless, the retrieved uncertainties are a good estimate of the true errors in the retrieved integrated properties, except where the surface area density exceeds the 1.0 μm2 cm−3 threshold. When applied to near-global SAGE II satellite extinction measured in 1999 the retrieved OE surface area and volume densities are observed to be larger by, respectively, 20–50% and 10–40% compared to those estimates obtained by the SAGE~II operational retrieval algorithm. An examination of the OE algorithm biases with in situ data indicates that the new OE aerosol property estimates tend to be more realistic than previous estimates obtained from remotely sensed data through other retrieval techniques. Based on the results of this study we therefore suggest that the new Optimal Estimation retrieval algorithm is able to contribute to an advancement in aerosol research by considerably improving current estimates of aerosol properties in the lower stratosphere under low aerosol loading conditions.
Steady-state aerosol distributions in the extra-tropical, lower stratosphere and the processes that maintain them
