ALBERT

Description: We present a range of airborne in situ observations of biomass burning carbonaceous aerosol over tropical South America, including a case study of a large tropical forest wildfire and a series of regional survey flights across the Brazilian Amazon and Cerrado. The study forms part of the South American Biomass Burning Analysis (SAMBBA) project, which was conducted during September and October 2012. We find limited evidence for net increases in aerosol mass through atmospheric ageing combined with substantial changes in the chemical properties of organic aerosol (OA). Oxidation of the OA increases significantly and rapidly on the scale of 2.5–3 h based on our case study analysis and is consistent with secondary organic aerosol production. The observations of limited net enhancement in OA coupled with such changes in chemical composition imply that evaporation of OA is also occurring to balance these changes. We observe significant coatings on black carbon particles at source, but with limited changes with ageing in both particle core size and coating thickness. We quantify variability in the ratio of OA to carbon monoxide across our study as a key parameter representing both initial fire conditions and an indicator of net aerosol production with atmospheric ageing. We observe ratios of 0.075–0.13 µgsm-3ppbv-1 in the west of our study region over the Amazon tropical forest in air masses less influenced by precipitation and a value of 0.095 µgsm-3ppbv-1 over the Cerrado environment in the east (where sm−3 refers to standard metre cubed). Such values are consistent with emission factors used by numerical models to represent biomass burning OA emissions. Black carbon particle core sizes typically range from mean mass diameters of 250 to 290 nm, while coating thicknesses range from 40 to 110 nm in air masses less influenced by precipitation. The primary driver of the variability we observe appears to be related to changes at the initial fire source. A key lesson from our study is that simply aggregating our observations as a function of atmospheric ageing would have been misleading due to the complex nature of the regional aerosol and its drivers, due to the many conflating and competing factors that are present. Our study explores and quantifies key uncertainties in the evolution of biomass burning aerosol at both near-field and regional scales. Our results suggest that the initial conditions of the fire are the primary driver of carbonaceous aerosol physical and chemical properties over tropical South America, aside from significant oxidation of OA during atmospheric ageing. Such findings imply that uncertainties in the magnitude of the aerosol burden and its impact on weather, climate, health and natural ecosystems most likely lie in quantifying emission sources, alongside atmospheric dispersion, transport and removal rather than chemical enhancements in mass.

Description: The optical properties of black carbon (BC) are a major source of uncertainty in regional and global climate studies. In the past, detailed investigation of BC absorption has been hampered by systematic biases in the measurement instrumentation. We present airborne measurements of aerosol absorption and black carbon microphysical properties in highly aged biomass burning plumes measured 4–8 d from their source over the southeast Atlantic Ocean during CLARIFY-2017, using a suite of novel photoacoustic spectrometers to measure aerosol absorption at 405, 514, and 655 nm and a single-particle soot photometer to measure the BC mass concentration, size, and mixing state. These measurements are of sufficient quality and detail to provide constraint on optical schemes used in climate models for the first time in biomass burning plumes far from their source – an aerosol environment that is one of the most important climatically. The average absorption Ångström exponents (AAE) were 1.38 over the wavelength range from 405 to 514 nm and 0.88 over the range from 514 to 655 nm, suggesting that brown carbon (BrC) contributed to 11±2 % of absorption at 405 nm. The effective organic aerosol (OA) mass absorption coefficient (MAC) was 0.31±0.09 m2 g−1 at 405 nm. The BC particles were universally thickly coated, and almost no externally mixed BC particles were detected. The average MAC of BC was 20±4, 15±3, and 12±2 m2g−1 at wavelengths of 405, 514, and 655 nm respectively, with equivalent absorption enhancements of around 1.85±0.45 at all three wavelengths, suggesting that the thick coatings acted as a lens that enhanced light absorption by the BC. We compared the measured MAC and AAE values with those calculated using several optical models and absorption parameterisations that took the measured BC mass and mixing state as inputs. Homogeneous grey-sphere Mie models were only able to replicate MAC for some low (real and imaginary) values of the complex BC refractive index (mBC) at the shortest wavelength, but they would have to use unrealistically low values of mBC to accurately replicate the AAE. A core–shell Mie model was able to generate good agreement for MAC in the green–red end of the visible spectrum for most values of mBC. However, there are no possible values of mBC that produce MAC values that agree with our observations at all three wavelengths, due to a wavelength-dependent underestimation of the MAC of the underlying BC core. Four semiempirical parameterisations from the literature were also tested, linking the BC mixing state to either the MAC or absorption enhancement. Two of these schemes produced results that agreed within a few percent with the measured MAC at all three wavelengths, and the AAE agreed well when discounting the effects of BrC. Our results uniquely demonstrate the validity of absorption parameterisations, as well as the failings of Mie calculations, in this highly aged environment. We recommend that future work should conduct similar analyses in environments where BC has different properties; future studies should also investigate the impact of implementing these types of schemes within climate models as well as the impact of developing equivalent schemes for light scattering by soot particles at visible wavelengths.

Description: The vertical distribution in the physical and chemical properties of submicron aerosol has been characterised across northern India for the first time using airborne in situ measurements. This study focusses primarily on the Indo-Gangetic Plain, a low-lying area in the north of India which commonly experiences high aerosol mass concentrations prior to the monsoon season. Data presented are from the UK Facility for Airborne Atmospheric Measurements BAe-146 research aircraft that performed flights in the region during the 2016 pre-monsoon (11 and 12 June) and monsoon (30 June to 11 July) seasons. Inside the Indo-Gangetic Plain boundary layer, organic matter dominated the submicron aerosol mass (43 %) followed by sulfate (29 %), ammonium (14 %), nitrate (7 %) and black carbon (7 %). However, outside the Indo-Gangetic Plain, sulfate was the dominant species, contributing 44 % to the total submicron aerosol mass in the boundary layer, followed by organic matter (30 %), ammonium (14 %), nitrate (6 %) and black carbon (6 %). Chlorine mass concentrations were negligible throughout the campaign. Black carbon mass concentrations were higher inside the Indo-Gangetic Plain (2 µg m−3) compared to outside (1 µg m−3). Nitrate appeared to be controlled by thermodynamic processes, with increased mass concentration in conditions of lower temperature and higher relative humidity. Increased mass and number concentrations were observed inside the Indo-Gangetic Plain and the aerosol was more absorbing in this region, whereas outside the Indo-Gangetic Plain the aerosol was larger in size and more scattered in nature, suggesting greater dust presence, especially in north-western India. The aerosol composition remained largely similar as the monsoon season progressed, but the total aerosol mass concentrations decreased by ∼50 % as the rainfall arrived; the pre-monsoon average total mass concentration was 30 µg m−3 compared to a monsoon average total mass concentration of 10–20 µg m−3. However, this mass concentration decrease was less noteworthy (∼20 %–30 %) over the Indo-Gangetic Plain, likely due to the strength of emission sources in this region. Decreases occurred in coarse mode aerosol, with the fine mode fraction increasing with monsoon arrival. In the aerosol vertical profile, inside the Indo-Gangetic Plain during the pre-monsoon, organic aerosol and absorbing aerosol species dominated in the lower atmosphere (〈1.5 km), with sulfate, dust and other scattering aerosol species enhanced in an elevated aerosol layer above 1.5 km with maximum aerosol height ∼6 km. The elevated concentration of dust at altitudes 〉1.5 km is a clear indication of dust transport from the Great Indian Desert, also called the Thar Desert, in north-western India. As the monsoon progressed into this region, the elevated aerosol layer diminished, the aerosol maximum height reduced to ∼2 km. The dust and sulfate-dominated aerosol layer aloft was removed upon monsoon arrival, highlighted by an increase in fine mode fraction throughout the profile.

Description: In recent years, photoacoustic spectroscopy has emerged as an invaluable tool for the accurate measurement of light absorption by atmospheric aerosol. Photoacoustic instruments require calibration, which can be achieved by measuring the photoacoustic signal generated by known quantities of gaseous ozone. Recent work has questioned the validity of this approach at short visible wavelengths (404 nm), indicating systematic calibration errors of the order of a factor of 2. We revisit this result and test the validity of the ozone calibration method using a suite of multipass photoacoustic cells operating at wavelengths 405, 514 and 658 nm. Using aerosolised nigrosin with mobility-selected diameters in the range 250–425 nm, we demonstrate excellent agreement between measured and modelled ensemble absorption cross sections at all wavelengths, thus demonstrating the validity of the ozone-based calibration method for aerosol photoacoustic spectroscopy at visible wavelengths.

Description: On 15–16 October 2017, ex-hurricane Ophelia passed to the west of the British Isles, bringing dust from the Sahara and smoke from Portuguese forest fires that was observable to the naked eye and reported in the UK's national press. We report here detailed observations of this event using the UK operational lidar and sun-photometer network, established for the early detection of aviation hazards, including volcanic ash. We also use ECMWF ERA5 wind field data and MODIS imagery to examine the aerosol transport. The observations, taken continuously over a period of 30 h, show a complex picture, dominated by several different aerosol layers at different times and clearly correlated with the passage of different air masses associated with the intense cyclonic system. A similar evolution was observed at several sites, with a time delay between them explained by their different location with respect to the storm and associated meteorological features. The event commenced with a shallow dust layer at 1–2 km in altitude and culminated in a deep and complex structure that lasted ∼12 h at each site over the UK, correlated with the storm's warm sector. For most of the time, the aerosol detected was dominated by mineral dust mixtures, as highlighted by depolarisation measurements, but an intense biomass burning aerosol (BBA) layer was observed towards the end of the event, lasting around 3 h at each site. The aerosol optical depth at 355 nm (AOD355) during the whole event ranged from 0.2 to 2.9, with the larger AOD correlated to the intense BBA layer. Such a large AOD is unprecedented in the UK according to AERONET records for the last 20 years. The Raman lidars permitted the measurement of the aerosol extinction coefficient at 355 nm, the particle linear depolarisation ratio (PLDR), and the lidar ratio (LR) and made the separation of the dust (depolarising) aerosol from other aerosol types possible. A specific extinction has also been computed to provide an estimate of the atmospheric concentration of both aerosol types separately, which peaked at 420±200 µg m−3 for the dust and 558±232 µg m−3 for the biomass burning aerosols. Back trajectories computed using the Numerical Atmospheric-dispersion Modelling Environment (NAME) were used to identify the sources and strengthen the conclusions drawn from the observations. The UK network represents a significant expansion of the observing capability in northern Europe, with instruments evenly distributed across Great Britain, from Camborne in Cornwall to Lerwick in the Shetland Islands, and this study represents the first attempt to demonstrate its capability and validate the methods in use. Its ultimate purpose will be the detection and quantification of volcanic plumes, but the present study clearly demonstrates the advanced capabilities of the network.

Description: Here we show results from Earth system model simulations from the marine cloud brightening experiment G4cdnc of the Geoengineering Model Intercomparison Project (GeoMIP). The nine contributing models prescribe a 50 % increase in the cloud droplet number concentration (CDNC) of low clouds over the global oceans in an experiment dubbed G4cdnc, with the purpose of counteracting the radiative forcing due to anthropogenic greenhouse gases under the RCP4.5 scenario. The model ensemble median effective radiative forcing (ERF) amounts to −1.9 W m−2, with a substantial inter-model spread of −0.6 to −2.5 W m−2. The large spread is partly related to the considerable differences in clouds and their representation between the models, with an underestimation of low clouds in several of the models. All models predict a statistically significant temperature decrease with a median of (for years 2020–2069) −0.96 [−0.17 to −1.21] K relative to the RCP4.5 scenario, with particularly strong cooling over low-latitude continents. Globally averaged there is a weak but significant precipitation decrease of −2.35 [−0.57 to −2.96] % due to a colder climate, but at low latitudes there is a 1.19 % increase over land. This increase is part of a circulation change where a strong negative top-of-atmosphere (TOA) shortwave forcing over subtropical oceans, caused by increased albedo associated with the increasing CDNC, is compensated for by rising motion and positive TOA longwave signals over adjacent land regions.

Description: Geoengineering, or climate intervention, describes methods of deliberately altering the climate system to offset anthropogenic climate change. As an idealized representation of near-surface solar geoengineering over the ocean, such as marine cloud brightening, this paper discusses experiment G1ocean-albedo of the Geoengineering Model Intercomparison Project (GeoMIP), involving an abrupt quadrupling of the CO2 concentration and an instantaneous increase in ocean albedo to maintain approximate net top-of-atmosphere radiative flux balance. A total of 11 Earth system models are relatively consistent in their temperature, radiative flux, and hydrological cycle responses to this experiment. Due to the imposed forcing, air over the land surface warms by a model average of 1.14 K, while air over most of the ocean cools. Some parts of the near-surface air temperature over ocean warm due to heat transport from land to ocean. These changes generally resolve within a few years, indicating that changes in ocean heat content play at most a small role in the warming over the oceans. The hydrological cycle response is a general slowing down, with high heterogeneity in the response, particularly in the tropics. While idealized, these results have important implications for marine cloud brightening, or other methods of geoengineering involving spatially heterogeneous forcing, or other general forcings with a strong land–ocean contrast. It also reinforces previous findings that keeping top-of-atmosphere net radiative flux constant is not sufficient for preventing changes in global mean temperature.

Description: Photoacoustic spectroscopy is a sensitive in situ technique for measuring the absorption coefficient for gas and aerosol samples. Photoacoustic spectrometer (PAS) instruments require accurate calibration by comparing the measured photoacoustic response with a known level of absorption for a calibrant. Ozone is a common calibrant of PAS instruments, yet recent work by Bluvshtein et al. (2017) has cast uncertainty on the validity of ozone as a calibrant at a wavelength of 405 nm. Moreover, Fischer and Smith (2018) demonstrate that a low O2 mass fraction in the bath gas can bias the measured PAS calibration coefficient to lower values for wavelengths in the range 532–780 nm. In this contribution, we present PAS sensitivity measurements at wavelengths of 405, 514 and 658 nm using ozone-based calibrations with variation in the relative concentrations of O2 and N2 bath gases. We find excellent agreement with the results of Fischer and Smith at the 658 nm wavelength. However, the PAS sensitivity decreases significantly as the bath gas composition tends to pure oxygen for wavelengths of 405 and 514 nm, which cannot be rationalised using arguments presented in previous studies. To address this, we develop a model to describe the variation in PAS sensitivity with both wavelength and bath gas composition that considers Chappuis band photodynamics and recognises that the photoexcitation of O3 leads rapidly to the photodissociation products O(3P) and O2(X, v 〉 0). We show that the rates of two processes are required to model the PAS sensitivity correctly. The first process involves the formation of vibrationally excited O3(X̃) through the reaction of the nascent O(3P) with bath gas O2. The second process involves the quenching of vibrational energy from the nascent O2(X, v 〉 0) to translational modes of the bath gas. Both of these processes proceed at different rates in collisions with N2 or O2 bath gas species. Importantly, we show that the PAS sensitivity is optimised for our PAS instruments when the ozone-based calibration is performed in a bath gas with a similar composition to ambient air and conclude that our methods for measuring aerosol absorption using an ozone-calibrated PAS are accurate and without detectable bias. We emphasise that the dependence of PAS sensitivity on bath gas composition is wavelength-dependent, and we recommend strongly that researchers characterise the optimal bath gas composition for their particular instrument.