Aerosol effects on clouds are concealed by natural cloud heterogeneity and satellite retrieval errors.

One major source of uncertainty in the cloud-mediated aerosol forcing arises from the magnitude of the cloud liquid water path (LWP) adjustment to aerosol-cloud interactions, which is poorly constrained by observations. Many of the recent satellite-based studies have observed a decreasing LWP as a function of cloud droplet number concentration (CDNC) as the dominating behavior. Estimating the LWP response to the CDNC changes is a complex task since various confounding factors need to be isolated. However, an important aspect has not been sufficiently considered: the propagation of natural spatial variability and errors in satellite retrievals of cloud optical depth and cloud effective radius to estimates of CDNC and LWP. Here we use satellite and simulated measurements to demonstrate that, because of this propagation, even a positive LWP adjustment is likely to be misinterpreted as negative. This biasing effect therefore leads to an underestimate of the aerosol-cloud-climate cooling and must be properly considered in future studies.

Correction: Lamy et al. Monitoring Solar Radiation UV Exposure in the Comoros. Int. J. Environ. Res. Public Health 2021, 18, 10475.

Text Correction [...].

Monitoring Solar Radiation UV Exposure in the Comoros.

As part of the UV-Indien project, a station for measuring ultraviolet radiation and the cloud fraction was installed in December 2019 in Moroni, the capital of the Comoros, situated on the west coast of the island of Ngazidja. A ground measurement campaign was also carried out on 12 January 2020 during the ascent of Mount Karthala, located in the center of the island of Ngazidja. In addition, satellite estimates (Ozone Monitoring Instrument and TROPOspheric Monitoring Instrument) and model outputs (Copernicus Atmospheric Monitoring Service and Tropospheric Ultraviolet Model) were combined for this same region. On the one hand, these different measurements and estimates make it possible to quantify, evaluate, and monitor the health risk linked to exposure to ultraviolet radiation in this region, and, on the other, they help to understand how cloud cover influences the variability of UV-radiation on the ground. The measurements of the Ozone Monitoring Instrument onboard the EOS-AURA satellite, being the longest timeseries of ultraviolet measurements available in this region, make it possible to quantify the meteorological conditions in Moroni and to show that more than 80% of the ultraviolet indices are classified as high and that 60% of these are classified as extreme. The cloud cover measured in Moroni by an All Sky Camera was used to distinguish between the cases of UV index measurements taken under clear or cloudy sky conditions. The ground-based measurements thus made it possible to describe the variability of the diurnal cycle of the UV index and the influence of cloud cover on this parameter. They also permitted the satellite measurements and the results of the simulations to be validated. In clear sky conditions, a relative difference of between 6 and 11% was obtained between satellite or model estimates and ground measurements. The ultraviolet index measurement campaign on Mount Karthala showed maximum one-minute standard erythemal doses at 0.3 SED and very high daily cumulative erythemal doses at more than 80 SED. These very high levels are also observed throughout the year and all skin phototypes can exceed the daily erythemal dose threshold at more than 20 SED.

Significance of the organic aerosol driven climate feedback in the boreal area.

Aerosol particles cool the climate by scattering solar radiation and by acting as cloud condensation nuclei. Higher temperatures resulting from increased greenhouse gas levels have been suggested to lead to increased biogenic secondary organic aerosol and cloud condensation nuclei concentrations creating a negative climate feedback mechanism. Here, we present direct observations on this feedback mechanism utilizing collocated long term aerosol chemical composition measurements and remote sensing observations on aerosol and cloud properties. Summer time organic aerosol loadings showed a clear increase with temperature, with simultaneous increase in cloud condensation nuclei concentration in a boreal forest environment. Remote sensing observations revealed a change in cloud properties with an increase in cloud reflectivity in concert with increasing organic aerosol loadings in the area. The results provide direct observational evidence on the significance of this negative climate feedback mechanism.

Impacts of brown carbon from biomass burning on surface UV and ozone photochemistry in the Amazon Basin.

The spectral dependence of light absorption by atmospheric particulate matter has major implications for air quality and climate forcing, but remains uncertain especially in tropical areas with extensive biomass burning. In the September-October 2007 biomass-burning season in Santa Cruz, Bolivia, we studied light absorbing (chromophoric) organic or "brown" carbon (BrC) with surface and space-based remote sensing. We found that BrC has negligible absorption at visible wavelengths, but significant absorption and strong spectral dependence at UV wavelengths. Using the ground-based inversion of column effective imaginary refractive index in the range 305-368 nm, we quantified a strong spectral dependence of absorption by BrC in the UV and diminished ultraviolet B (UV-B) radiation reaching the surface. Reduced UV-B means less erythema, plant damage, and slower photolysis rates. We use a photochemical box model to show that relative to black carbon (BC) alone, the combined optical properties of BrC and BC slow the net rate of production of ozone by up to 18% and lead to reduced concentrations of radicals OH, HO2, and RO2 by up to 17%, 15%, and 14%, respectively. The optical properties of BrC aerosol change in subtle ways the generally adverse effects of smoke from biomass burning.

Contribution of Brown Carbon to Direct Radiative Forcing over the Indo-Gangetic Plain.

The Indo-Gangetic Plain is a region of known high aerosol loading with substantial amounts of carbonaceous aerosols from a variety of sources, often dominated by biomass burning. Although black carbon has been shown to play an important role in the absorption of solar energy and hence direct radiative forcing (DRF), little is known regarding the influence of light absorbing brown carbon (BrC) on the radiative balance in the region. With this in mind, a study was conducted for a one month period during the winter-spring season of 2013 in Kanpur, India that measured aerosol chemical and physical properties that were used to estimate the sources of carbonaceous aerosols, as well as parameters necessary to estimate direct forcing by aerosols and the contribution of BrC absorption to the atmospheric energy balance. Positive matrix factorization analyses, based on aerosol mass spectrometer measurements, resolved organic carbon into four factors including low-volatile oxygenated organic aerosols, semivolatile oxygenated organic aerosols, biomass burning, and hydrocarbon like organic aerosols. Three-wavelength absorption and scattering coefficient measurements from a Photo Acoustic Soot Spectrometer were used to estimate aerosol optical properties and estimate the relative contribution of BrC to atmospheric absorption. Mean ± standard deviation values of short-wave cloud free clear sky DRF exerted by total aerosols at the top of atmosphere, surface and within the atmospheric column are -6.1 ± 3.2, -31.6 ± 11, and 25.5 ± 10.2 W/m(2), respectively. During days dominated by biomass burning the absorption of solar energy by aerosols within the atmosphere increased by ∼35%, accompanied by a 25% increase in negative surface DRF. DRF at the top of atmosphere during biomass burning days decreased in negative magnitude by several W/m(2) due to enhanced atmospheric absorption by biomass aerosols, including BrC. The contribution of BrC to atmospheric absorption is estimated to range from on average 2.6 W/m(2) for typical ambient conditions to 3.6 W/m(2) during biomass burning days. This suggests that BrC accounts for 10-15% of the total aerosol absorption in the atmosphere, indicating that BrC likely plays an important role in surface and boundary temperature as well as climate.