Refractory black carbon (rBC) aerosol loadings and mass size distributions have been quantified during the HIPPO campaign above the remote Pacific from 80N to 67S. Over 100 vertical profiles of rBC ...loadings, extending from ∼0.3 to ∼14 km were obtained with a Single‐Particle Soot Photometer (SP2) during a two‐week period in January 2009. The dataset provides a striking, and previously unobtainable, pole‐to‐pole snapshot of rBC mass loadings. rBC vertical concentration profiles reveal significant dependences on latitude, while associated rBC mass size distributions were highly uniform. The vertical profiles averaged in five latitude zones were compared to an ensemble of AEROCOM model fields. The model ensemble spread in each zone was over an order of magnitude, while the model average over‐predicted rBC concentrations overall by a factor five. The comparisons suggest that rBC removal in global models may need to be evaluated separately in different latitude regions and perhaps enhanced.
During the ARCPAC (Aerosol, Radiation, and Cloud Processes affecting Arctic Climate) airborne field experiment in April 2008 in northern Alaska, about 50 plumes were encountered with the NOAA WP‐3 ...aircraft between the surface and 6.5 km. Onboard measurements and the transport model FLEXPART showed that most of the plumes were emitted by forest fires in southern Siberia‐Lake Baikal area and by agricultural burning in Kazakhstan‐southern Russia. Unexpectedly, these biomass burning plumes were the dominant aerosol and gas‐phase features encountered in this area during April. The influence on the plumes from sources other than burning was small. The chemical characteristics of plumes from the two source regions were different, with higher enhancements relative to CO for most gas and aerosol species from the agricultural fires. In 2008, the fire season started earlier than usual in Siberia, which may have resulted in unusually efficient transport of biomass burning emissions into the Arctic.
In situ measurements of the mass, mixing state, and optical size of individual black‐carbon (BC) particles in the fine mode (90–600 nm) have been made in fresh emissions from urban and biomass ...burning sources with an airborne single‐particle soot photometer. Contrasts between the two sources are significant and consistent. Urban BC tends to smaller sizes, fewer coated particles, thinner coatings, and less absorption per unit mass than biomass‐burning BC. This suggests that urban BC may have a longer lifetime in the atmosphere and a different impact on BC radiative forcing in the first indirect effect than biomass‐burning BC. These measurements bound the likely variability in the microphysical state of BC emissions from typical continental processes, and provide direct measurements of the size distribution and coating state of fine‐mode BC for use in constraining climate and aerosol models. These results highlight the need for the integration of source‐specific information into such models.
Although laboratory experiments have shown that organic compounds in both gasoline fuel and diesel engine exhaust can form secondary organic aerosol (SOA), the fractional contribution from gasoline ...and diesel exhaust emissions to ambient SOA in urban environments is poorly known. Here we use airborne and ground‐based measurements of organic aerosol (OA) in the Los Angeles (LA) Basin, California made during May and June 2010 to assess the amount of SOA formed from diesel emissions. Diesel emissions in the LA Basin vary between weekdays and weekends, with 54% lower diesel emissions on weekends. Despite this difference in source contributions, in air masses with similar degrees of photochemical processing, formation of OA is the same on weekends and weekdays, within the measurement uncertainties. This result indicates that the contribution from diesel emissions to SOA formation is zero within our uncertainties. Therefore, substantial reductions of SOA mass on local to global scales will be achieved by reducing gasoline vehicle emissions.
Key Points
Diesel emissions contribute significantly to primary organic aerosol
Gasoline exhaust emissions dominate secondary organic aerosol (SOA) formation
Globally, SOA from gasoline exhaust may reach 16% of biogenic SOA
Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of ...BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil-fuel and biomass-burning BC. In addition we develop a global simulation of brown carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of 2. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in absorption aerosol optical depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with the largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 Wm−2 (0.08 Wm−2 from anthropogenic sources and 0.05 Wm−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 Wm−2, with an additional +0.11 Wm−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80%/+140%. Our estimates are at the lower end of the 0.2–1.0 Wm−2 range from previous studies, and substantially less than the +0.6 Wm−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime (including the effect on the vertical profile) and the incorrect attribution of BrC absorption to BC.
The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community ...Earth System Model (CESM) version 1.2. The main focus of this paper is to compare the performance of configurations with internally derived "free running" (FR) meteorology and "specified dynamics" (SD) against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We focus on the representation of aerosols and chemistry. All model configurations reproduce tropospheric ozone for most regions based on in situ and satellite observations. However, shortcomings exist in the representation of ozone precursors and aerosols. Tropospheric ozone in all model configurations agrees for the most part with ozonesondes and satellite observations in the tropics and the Northern Hemisphere within the variability of the observations. Southern hemispheric tropospheric ozone is consistently underestimated by up to 25%. Differences in convection and stratosphere to troposphere exchange processes are mostly responsible for differences in ozone in the different model configurations. Carbon monoxide (CO) and other volatile organic compounds are largely underestimated in Northern Hemisphere mid-latitudes based on satellite and aircraft observations. Nitrogen oxides (NOx) are biased low in the free tropical troposphere, whereas peroxyacetyl nitrate (PAN) is overestimated in particular in high northern latitudes. The present-day methane lifetime estimates are compared among the different model configurations. These range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem and are therefore underestimated compared to observational estimations. We find that differences in tropospheric aerosol surface area between CAM4 and CAM5 play an important role in controlling the burden of the tropical tropospheric hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of NOx from lightning explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss but also by transport and mixing. For future studies, we recommend the use of CAM5-chem configurations, due to improved aerosol description and inclusion of aerosol–cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.
Using aircraft observations and transport model calculations we determine the total amounts of various gas‐phase and aerosol species in the Arctic due to distant biomass burning (BB) emissions. We ...find that for many climate‐relevant species, including black carbon (BC) and organic aerosols, fires in Russia that typically occur during the critical springtime snowmelt can more than double the high seasonal Arctic atmospheric background that has built up in the winter months (commonly called “Arctic haze”). Decision makers have targeted BC, because it is expected to cause strong positive forcing over snow‐covered surfaces yet is significantly shorter lived than greenhouse gases. These results demonstrate that BB is more important for the Arctic than previously believed and should be considered in any attempt to mitigate impacts.
Results for the solar heating rates in ambient air due to absorption by black-carbon (BC) containing particles and ozone are presented as calculated from airborne observations made in the tropical ...tropopause layer (TTL) in January-February 2006. The method uses airborne in situ observations of BC particles, ozone and actinic flux. Total BC mass is obtained along the flight track by summing the masses of individually detected BC particles in the range 90 to 600-nm volume-equivalent diameter, which includes most of the BC mass. Ozone mixing ratios and upwelling and partial downwelling solar actinic fluxes were measured concurrently with BC mass. Two estimates used for the BC wavelength-dependent absorption cross section yielded similar heating rates. For mean altitudes of 16.5, 17.5, and 18.5 km (0.5 km) in the tropics, average BC heating rates were near 0.0002 K/d. Observed BC coatings on individual particles approximately double derived BC heating rates. Ozone heating rates exceeded BC heating rates by approximately a factor of 100 on average and at least a factor of 4, suggesting that BC heating rates in this region are negligible in comparison.
Evaluation of the aerosol schemes in current climate models is dependent upon the available observational data. In-situ observations from flight campaigns can provide valuable data about the vertical ...distribution of aerosol that is difficult to obtain from satellite or ground-based platforms, although they are localised in space and time. Using single-particle soot-photometer (SP2) measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign, which consists of many vertical profiles over a large region of the Pacific, we evaluate the meridional and vertical distribution of black carbon (BC) aerosol simulated by the HadGEM3-UKCA and ECHAM5-HAM2 models. Both models show a similar pattern of overestimating the BC column burden compared to that derived from the observations, in many areas by an order of magnitude. However, by sampling the simulated BC mass mixing ratio along the flight track and comparing to the observations, we show that this discrepancy has a rather different vertical structure in the two models: in HadGEM3-UKCA the discrepancy is dominated by excess aerosol in the tropical upper troposphere, while in ECHAM5-HAM2 areas of discrepancy are spread across many different latitudes and altitudes. Using this methodology, we conduct sensitivity tests on two specific elements of the models: biomass-burning emissions and scavenging by convective precipitation. We show that, by coupling the convective scavenging more tightly with convective transport, both the column burden and vertical distribution of BC in HadGEM3-UKCA are much improved with respect to the observations, with a substantial and statistically significant increase in correlation - this demonstrates the importance of a realistic representation of this process. In contrast, updating from GFED2 to GFED3.1 biomass-burning emissions makes a more modest improvement in both models, which is not statistically significant. By comparing our results with a more traditional approach using regional- and monthly-mean vertical profile curves, we show that the point-by-point analysis allows the model improvements to be demonstrated more clearly. We also demonstrate the important role that nudged simulations (where the large-scale model dynamics are continuously relaxed towards a reanalysis) can play in this type of evaluation, allowing statistically significant differences between configurations of the aerosol scheme to be seen where the differences between the corresponding free-running simulations would not be significant.
The variability of precipitation and water supply along the U.S. West Coast creates major challenges to the region’s economy and environment, as evidenced by the recent California drought. This ...variability is strongly influenced by atmospheric rivers (ARs), which deliver much of the precipitation along the U.S. West Coast and can cause flooding, and by aerosols (from local sources and transported from remote continents and oceans) that modulate clouds and precipitation. A better understanding of these processes is needed to reduce uncertainties in weather predictions and climate projections of droughts and floods, both now and under changing climate conditions.
To address these gaps, a group of meteorologists, hydrologists, climate scientists, atmospheric chemists, and oceanographers have created an interdisciplinary research effort, with support from multiple agencies. From 2009 to 2011 a series of field campaigns California Water Service (CalWater) 1 collected atmospheric chemistry, cloud microphysics, and meteorological measurements in California and associated modeling and diagnostic studies were carried out. Based on the remaining gaps, a vision was developed to extend these studies offshore over the eastern North Pacific and to enhance land-based measurements from 2014 to 2018 (CalWater-2). The dataset and selected results from CalWater-1 are summarized here. The goals of CalWater-2, and measurements to date, are then described.
CalWater is producing new findings and exploring new technologies to evaluate and improve global climate models and their regional performance and to develop tools supporting water and hydropower management. These advances also have potential to enhance hazard mitigation by improving near-term weather prediction and subseasonal and seasonal outlooks.
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