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<p>This study explores the potential to retrieve aerosol properties with the GRASP algorithm (Generalized Retrieval of Atmosphere and Surface Properties) using as input measurements of zenith sky radiance (ZSR), which are sky radiance values measured in the zenith direction, recorded at four wavelengths by a ZEN-R52 radiometer. To this end, the ZSR measured at 440, 500, 675 and 870 nm by a ZEN-R52 (ZSR<span class="inline-formula">_ZEN</span>), installed in Valladolid (Spain), is employed. This instrument is calibrated by intercomparing the signal of each channel with coincident ZSR values simulated (ZSR<span class="inline-formula">_SIM</span>) at the same wavelengths with a radiative transfer model (RTM). These simulations are carried out using the GRASP forward module as RTM and the aerosol information from a co-located CE318 photometer belonging to AERONET (AErosol RObotic NETwork) as input. The dark signal and the signal dependence on temperature are characterized and included in the calibration process. The uncertainties for each channel are quantified by an intercomparison with a co-located CE318 photometer, obtaining lower values for shorter wavelengths; they are between 3 % for 440 nm and 21 % for 870 nm. The proposed inversion strategy for the aerosol retrieval using the ZSR<span class="inline-formula">_ZEN</span> measurements as input, i.e. so-called GRASP-ZEN, assumes the aerosol as an external mixture of five pre-calculated aerosol types. A sensitivity analysis is conducted using synthetic ZSR<span class="inline-formula">_ZEN</span> measurements, pointing out that these measurements are sensitive to aerosol load and type. It also assesses that the retrieved aerosol optical depth (AOD) values in general overestimate the reference ones by 0.03, 0.02, 0.02 and 0.01 for 440, 500, 675 and 870 nm, respectively. The calibrated ZSR<span class="inline-formula">_ZEN</span> measurements, recorded during 2.5 years at Valladolid, are inverted by the GRASP-ZEN strategy to retrieve some aerosol properties like AOD. The retrieved AOD shows a high correlation with respect to independent values obtained from a co-located AERONET CE318 photometer, with determination coefficients (<span class="inline-formula"><i>r</i>²</span>) of 0.86, 0.85, 0.79 and 0.72 for 440, 500, 675 and 870 nm, respectively, and finding uncertainties between 0.02 and 0.03 with respect to the AERONET values. Finally, the retrieval of other aerosol properties, like aerosol volume concentration for total, fine and coarse modes (VCT, VCF and VCC, respectively), is also explored. The comparison against independent values from AERONET presents <span class="inline-formula"><i>r</i>²</span> values of 0.57, 0.56 and 0.66 and uncertainties of 0.009, 0.016 and 0.02 <span class="inline-formula">µm³ µm⁻²</span> for VCT, VCF and VCC, respectively.</p>