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2.
Nature ; 546(7659): 485-491, 2017 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-28640263

RESUMO

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets-consistent with expectations-but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around -0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

3.
Phys Chem Chem Phys ; 23(1): 536-553, 2021 Jan 06.
Artigo em Inglês | MEDLINE | ID: mdl-33325473

RESUMO

Photoacoustic spectroscopy (PAS) is a sensitive technique for the detection of trace gases and aerosols and measurements of their absorption coefficients. The accuracy of such measurements is often governed by the fidelity of the PAS instrument calibration. Gas samples laden with O3 of a known or independently measured absorption coefficient are a convenient and commonplace route to calibration of PAS instruments operating at visible wavelengths (λ), yet the accuracy of such calibrations remains unclear. Importantly, the photoacoustic detection of O3 in the Chappuis band (λ ∼ 400-700 nm) depends strongly on the timescales for energy transfer from the nascent photoproducts O(3P) and O2(X, v > 0) to translational motion of bath gas species. Significant uncertainties remain concerning the dependence of these timescales on both the sample pressure and the bath gas composition. Here, we demonstrate accurate characterisation of microphone response function dependencies on pressure using a speaker transducer to excite resonant acoustic modes of our photoacoustic cells. These corrections enable measurements of photoacoustic response amplitudes (also referred to as PAS sensitivities) and phase shifts with variation in static pressure and bath gas composition, at discrete visible wavelengths spanning the Chappuis band. We develop and fit a photochemical relaxation model to these measurements to retrieve the associated variations in the aforementioned relaxation timescales for O(3P) and O2(X, v > 0). These timescales enable a full assessment of the accuracy of PAS calibrations using O3-laden gas samples, dependent on the sample pressure, bath gas composition and PAS laser modulation frequency.

4.
Sci Adv ; 7(41): eabg9998, 2021 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-34623916

RESUMO

The radiative budget, cloud properties, and precipitation over tropical Africa are influenced by solar absorption by biomass-burning aerosols (BBA) from Central Africa. Recent field campaigns, reinforced by new remote-sensing and aerosol climatology datasets, have highlighted the absorbing nature of the elevated BBA layers over the South-East Atlantic (SEA), indicating that the absorption could be stronger than previously thought. We show that most of the latest generation of general circulation models (GCMs) from the sixth phase of the Coupled Model Intercomparison Project 6 (CMIP6) underestimates the absorption of BBA over the SEA. This underlines why many (~75%) CMIP6 models do not fully capture the intense positive (warming) direct radiative forcing at the top of the atmosphere observed over this region. In addition, underestimating the magnitude of the BBA-induced solar heating could lead to misrepresentations of the low-level cloud responses and fast precipitation feedbacks that are induced by BBA in tropical regions.

5.
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