Dantong Liu

Enhanced light absorption by mixed source black and brown carbon particles in UK winter

Black carbon (BC) and light-absorbing organic carbon (brown carbon, BrC) play key roles in warming the atmosphere, but the magnitude of their effects remains highly uncertain. Theoretical modelling and laboratory experiments demonstrate that coatings on BC can enhance BCs light absorption, therefore many climate models simply assume enhanced BC absorption by a factor of ∼1.5. However, recent field observations show negligible absorption enhancement, implying models may overestimate BCs warming. Here we report direct evidence of substantial field-measured BC absorption enhancement, with the magnitude strongly depending on BC coating amount. Increases in BC coating result from a combination of changing sources and photochemical aging processes. When the influence of BrC is accounted for, observationally constrained model calculations of the BC absorption enhancement can be reconciled with the observations. We conclude that the influence of coatings on BC absorption should be treated as a source and regionally specific parameter in climate models.

The effect of complex black carbon microphysics on the determination of the optical properties of brown carbon

Assessment of the impacts of brown carbon (BrC) requires accurate determination of its physical properties, but a model must be invoked to derive these from instrument data. Ambient measurements were made in London at a site influenced by traffic and solid fuel (principally wood) burning, apportioned by single particle soot photometer data and optical properties measured using multiwavelength photoacoustic spectroscopy. Two models were applied: a commonly used Mie model treating the particles as single-coated spheres and a Rayleigh-Debye-Gans approximation treating them as aggregates of smaller-coated monomers. The derived solid fuel BrC parameters at 405 nm were found to be highly sensitive to the model treatment, with a mass absorption cross section ranging from 0.47 to 1.81 m2/g and imaginary refractive index from 0.013 to 0.062. This demonstrates that a detailed knowledge of particle morphology must be obtained and invoked to accurately parameterize BrC properties based on aerosol phase measurements.

Limited formation of isoprene epoxydiols‐derived secondary organic aerosol under NOx‐rich environments in Eastern China

Secondary organic aerosol (SOA) derived from isoprene epoxydiols (IEPOX) has potential impacts on regional air quality and climate yet is poorly characterized under NOx-rich ambient environments. We report the first real-time characterization of IEPOX-derived SOA (IEPOX-SOA) in Eastern China in summer 2013 using comprehensive ambient measurements, along with model analysis. The ratio of IEPOX-SOA to isoprene high-NOx SOA precursors, e.g., methyl vinyl ketone and methacrolein, and the reactive uptake potential of IEPOX was lower than those generally observed in regions with prevailing biogenic emissions, low NOx levels, and high particle acidity, elucidating the suppression of IEPOX-SOA formation under NOx-rich environments. IEPOX-SOA showed high potential source regions to the south with large biogenic emissions, illustrating that the interactions between biogenic and anthropogenic emissions might have played an important role in affecting the formation of IEPOX-SOA in polluted environments in Eastern China.

Evaluation of ground‐based black carbon measurements by filter‐based photometers at two Arctic sites

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...

The global aerosol synthesis and science project (GASSP): Measurements and modeling to reduce uncertainty

The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in-situ measurements of the particle size distribution, number concentration and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, an extensive global dataset of aerosol in-situ microphysical and chemical measurements, and new ways to assess the uncertainty associated with comparing sparse point measurements with low resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modellers and non-specialist users. Available measurements are extensive, but they biased to polluted regions of the northern hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model-data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.

Summertime Primary and Secondary Contributions to Southern Ocean Cloud Condensation Nuclei

Atmospheric aerosols in clean remote oceanic regions contribute significantly to the global albedo through the formation of haze and cloud layers; however, the relative importance of ‘primary’ wind-produced sea-spray over secondary (gas-to-particle conversion) sulphate in forming marine clouds remains unclear. Here we report on marine aerosols (PM1) over the Southern Ocean around Antarctica, in terms of their physical, chemical, and cloud droplet activation properties. Two predominant pristine air masses and aerosol populations were encountered: modified continental Antarctic (cAA) comprising predominantly sulphate with minimal sea-salt contribution and maritime Polar (mP) comprising sulphate plus sea-salt. We estimate that in cAA air, 75% of the CCN are activated into cloud droplets while in mP air, 37% are activated into droplets, for corresponding peak supersaturation ranges of 0.37–0.45% and 0.19–0.31%, respectively. When realistic marine boundary layer cloud supersaturations are considered (e.g. ~0.2–0.3%), sea-salt CCN contributed 2–13% of the activated nuclei in the cAA air and 8–51% for the marine air for surface-level wind speed < 16 m s−1. At higher wind speeds, primary marine aerosol can even contribute up to 100% of the activated CCN, for corresponding peak supersaturations as high as 0.32%.

The roles of volatile organic compound deposition and oxidation mechanisms in determining secondary organic aerosol production: A global perspective using the UKCA chemistry-climate model (vn8.4)

This work expands the SOA description in the United Kingdom Chemistry and Aerosol (UKCA) chemistry-climate model, and adequately explains why there is need for a more complex description of SOA formation in UKCA. The work also compares UKCA against global observations reasonably well. However, major revisions in the design of the model set-up and interpretation of the results are needed. These changes are

Light Absorption Enhancement of Black Carbon Aerosol Constrained by Particle Morphology

The radiative forcing of black carbon aerosol (BC) is one of the largest sources of uncertainty in climate change assessments. Contrasting results of BC absorption enhancement ( Eabs) after aging are estimated by field measurements and modeling studies, causing ambiguous parametrizations of BC solar absorption in climate models. Here we quantify Eabs using a theoretical model parametrized by the complex particle morphology of BC in different aging scales. We show that Eabs continuously increases with aging and stabilizes with a maximum of ∼3.5, suggesting that previous seemingly contrast results of Eabs can be explicitly described by BC aging with corresponding particle morphology. We also report that current climate models using Mie Core-Shell model may overestimate Eabs at a certain aging stage with a rapid rise of Eabs, which is commonly observed in the ambient. A correction coefficient for this overestimation is suggested to improve model predictions of BC climate impact.

Substantial reductions in ambient PAHs pollution and lives saved as a co-benefit of effective long-term PM2.5 pollution controls

Under great efforts in fighting against serious haze problem of China since 2013, decreasing of air pollutants especially for fine particles (PM2.5) has been revealed for several key regions. This study tried to answer whether the reduction of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) was coincident with PM2.5 because of long-term pollution control measures (PCM), and to assess source-oriented health risks associated with inhalation exposure to PAHs. Field measurements were carried out before and after the publishing of local air pollution protection plan for Nanjing, a mega-city in east China. Results indicated that the air quality was substantially improving, with a significant reduction in annual average PM2.5 by 34%, and moreover, PM2.5-bound PAHs significantly reduced by 63% (p < 0.001). The remarkable reduction was mainly attributable to the change of emission sources, compared to the influence of atmospheric circulation patterns, surface meteorological conditions, and atmospheric chemical reaction. Four PAHs sources including coal combustion (CC), petroleum and oil burning (PO), wood burning (WB) and vehicle emission (VE) were identified. On an annual basis, contributions to ambient PM2.5-PAHs from WB, PO, CC and VE sources in the period before the action of control measures were 2.26, 2.20, 1.96 and 5.62 ng m-3, respectively. They reduced to 1.09, 0.37, 1.31 and 1.77 ng m-3 for the four source types, with the reduction percentages as 51, 83, 33 and 68%, respectively. The estimated reduction in lifetime lung cancer risk was around 61%. The study that firstly assessed the health effects of PAHs reduction as a co-benefit raised by air PCM sustained for a long period is believed to be applicable and referential for other mega-cities around the world for assessing the benefits of PCM.

Mineralogy and mixing state of North African mineral dust by on-line single-particle mass spectrometry

Marsden et al. use laser desorption/ionization single-particle mass spectrometry to analyze source mineral dust particles, and ambient dust-laden aerosol sampled in North Africa. They apply their recently developed mass spectral analysis method to distinguish between different silicate minerals, based on the time delay that the relevant ions are detected in the MS. This time delay relates to the crystal structure of the different mineral phases. Distinguishing between different specific mineral phases or families in individual particles is a serious analytical challenge. The results presented here are quite novel, despite the various issues related to the semi-quantitative nature of the analysis, only being able to identify or distinguish some of the major mineral phases, and not achieving complete separation between different phases (the spread in the