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Simulated 2050 aviation radiative forcing from contrails and aerosols

The radiative forcing from aviation-induced cloudiness is investigated by using the Community Atmosphere Model Version 5 (CAM5) in the present (2006) and the future (through 2050). Global flight distance is projected to increase by a factor of 4 between 2006 and 2050. However, simulated contrail cirrus radiative forcing in 2050 can reach 87 mW m−2, an increase by a factor of 7 from 2006, and thus does not scale linearly with fuel emission mass. This is due to non-uniform regional increase in air traffic and different sensitivities for contrail radiative forcing in different regions. CAM5 simulations indicate that negative radiative forcing induced by the indirect effect of aviation sulfate aerosols on liquid clouds in 2050 can be as large as −160 mW m−2, an increase by a factor of 4 from 2006. As a result, the net 2050 radiative forcing of contrail cirrus and aviation aerosols may have a cooling effect on the planet. Aviation sulfate aerosols emitted at cruise altitude can be transported down to the lower troposphere, increasing the aerosol concentration, thus increasing the cloud drop number concentration and persistence of low-level clouds. Aviation black carbon aerosols produce a negligible net forcing globally in 2006 and 2050 in this model study. Uncertainties in the methodology and the modeling are significant and discussed in detail. Nevertheless, the projected percentage increase in contrail radiative forcing is important for future aviation impacts. In addition, the role of aviation aerosols in the cloud nucleation processes can greatly influence on the simulated radiative forcing from aircraft-induced cloudiness and even change its sign. Future research to confirm these results is necessary.
Tuning of a convective gravity wave source scheme based on HIRDLS observations

Convection as one dominant source of atmospheric gravity waves (GWs) has been the focus of investigation over recent years. However, its spatial and temporal forcing scales are not well known. In this work we address this open issue by a systematic verification of free parameters of the Yonsei convective GW source scheme based on observations from the High Resolution Dynamics Limb Sounder (HIRDLS). The instrument can only see a limited portion of the gravity wave spectrum due to visibility effects and observation geometry. To allow for a meaningful comparison of simulated GWs to observations, a comprehensive filter, which mimics the instrument limitations, is applied to the simulated waves. By this approach, only long horizontal-scale convective GWs are addressed. Results show that spectrum, distribution of momentum flux, and zonal mean forcing of long horizontal-scale convective GWs can be successfully simulated by the superposition of three or four combinations of parameter sets reproducing the observed GW spectrum. These selected parameter sets are different for northern and southern summer. Although long horizontal-scale waves are only part of the full spectrum of convective GWs, the momentum flux of these waves is found to be significant and relevant for the driving of the QBO (quasi-biennial oscillation). The zonal momentum balance is considered in vertical cross sections of GW momentum flux (GWMF) and GW drag (GWD). Global maps of the horizontal distribution of GWMF are considered and consistency between simulated results and HIRDLS observations is found. The latitude dependence of the zonal phase speed spectrum of GWMF and its change with altitude is discussed.
Characteristics of aerosol pollution during heavy haze events in Suzhou, China

Extremely severe haze weather events occurred in many cities in China, especially in the east part of the country, in January 2013. Comprehensive measurements including hourly concentrations of PM2.5 and its major chemical components (water-soluble inorganic ions, organic carbon (OC), and elemental carbon (EC)) and related gas-phase precursors were conducted via an online monitoring system in Suzhou, a medium-sized city in Jiangsu province, just east of Shanghai. PM2.5 (particulate matter with an aerodynamic diameter of 2.5 µm or less) frequently exceeded 150 µg m−3 on hazy days, with the maximum reaching 324 µg m−3 on 14 January 2013. Unfavorable weather conditions (high relative humidity (RH), and low rainfall, wind speed, and atmospheric pressure) were conducive to haze formation. High concentrations of secondary aerosol species (including SO42−, NO3−, NH4+, and SOC) and gaseous precursors were observed during the first two haze events, while elevated primary carbonaceous species emissions were found during the third haze period, pointing to different haze formation mechanisms. Organic matter (OM), (NH4)2SO4, and NH4NO3 were found to be the major contributors to visibility impairment. High concentrations of sulfate and nitrate might be explained by homogeneous gas-phase reactions under low RH conditions and by heterogeneous processes under relatively high RH conditions. Analysis of air mass trajectory clustering and potential source contribution function showed that aerosol pollution in the studied areas was mainly caused by local activities and surrounding sources transported from nearby cities.
Typical synoptic situations and their impacts on the wintertime air pollution in the Guanzhong basin, China

Rapid industrialization and urbanization have caused severe air pollution in the Guanzhong basin, northwestern China, with heavy haze events occurring frequently in recent winters. Using the NCEP reanalysis data, the large-scale synoptic situations influencing the Guanzhong basin during wintertime of 2013 are categorized into six types to evaluate the contribution of synoptic situations to the air pollution, including “north-low”, “southwest-trough”, “southeast-high”, “transition”, “southeast-trough”, and “inland-high”. The FLEXPART model has been utilized to demonstrate the corresponding pollutant transport patterns for the typical synoptic situations in the basin. Except for “southwest-trough” and “southeast-high” (defined as favorable synoptic situations), the other four synoptic conditions (defined as unfavorable synoptic situations) generally facilitate the accumulation of air pollutants, causing heavy air pollution in the basin. In association with the measurement of PM2.5 (particulate matter with aerodynamic diameter less than 2.5 µm) in the basin, the unfavorable synoptic situations correspond to high PM2.5 mass concentrations or poor air quality and vice versa. The same analysis has also been applied to winters of 2008–2012, which shows that the basin was mainly influenced by the unfavorable synoptic situations during wintertime leading to poor air quality. The WRF-CHEM model has further been applied to simulate the selected 6 days representing the typical synoptic situations during the wintertime of 2013, and the results generally show a good agreement between the modeled distributions and variations of PM2.5 and the corresponding synoptic situations, demonstrating reasonable classification for the synoptic situations in the basin. Detailed meteorological conditions, such as temperature inversion, low-level horizontal wind speed, and planetary boundary layer, all contribute to heavy air pollution events in the basin under unfavorable synoptic conditions. Considering the proportion of occurrence of unfavorable synoptic situations during wintertime, reduction of emissions is the optimum approach to mitigate the air pollution in the Guanzhong basin.
Biomass-burning impact on CCN number, hygroscopicity and cloud formation during summertime in the eastern Mediterranean

This study investigates the concentration, cloud condensation nuclei (CCN) activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean and their impacts on cloud droplet formation. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from CCN measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the values of κ, for all particle sizes. Particle sizes smaller than 80 nm exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of condensational growth and cloud processing. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles (having a diameter of ∼  100 nm at dry conditions) sampled. Based on positive matrix factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend as the biomass-burning organic aerosol (BBOA) component, with the former being enhanced between 65 and 150 % (for supersaturations ranging between 0.2 and 0.7 %) with the arrival of the smoke plumes. Using multilinear regression of the PMF factors (BBOA, OOA-BB and OOA) and the observed hygroscopicity parameter, the inferred hygroscopicity of the oxygenated organic aerosol components is determined. We find that the transformation of freshly emitted biomass burning (BBOA) to more oxidized organic aerosol (OOA-BB) can result in a 2-fold increase of the inferred organic hygroscopicity; about 10 % of the total aerosol hygroscopicity is related to the two biomass-burning components (BBOA and OOA-BB), which in turn contribute almost 35 % to the fine-particle organic water of the aerosol. Observation-derived calculations of the cloud droplet concentrations that develop for typical boundary layer cloud conditions suggest that biomass burning increases droplet number, on average by 8.5 %. The strongly sublinear response of clouds to biomass-burning (BB) influences is a result of strong competition of CCN for water vapor, which results in very low maximum supersaturation (0.08 % on average). Attributing droplet number variations to the total aerosol number and the chemical composition variations shows that the importance of chemical composition increases with distance, contributing up to 25 % of the total droplet variability. Therefore, although BB may strongly elevate CCN numbers, the impact on droplet number is limited by water vapor availability and depends on the aerosol particle concentration levels associated with the background.
Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH  ∼  0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ∼  −0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OSC  ∼  2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to higher ages where OA loss dominates. The mass added at low-to-intermediate ages is due primarily to condensation of oxidized species, not heterogeneous oxidation. The OA decrease at high photochemical ages is dominated by heterogeneous oxidation followed by fragmentation/evaporation. A comparison of urban SOA formation in this study with a similar study of vehicle SOA in a tunnel suggests the importance of vehicle emissions for urban SOA. Pre-2007 SOA models underpredict SOA formation by an order of magnitude, while a more recent model performs better but overpredicts at higher ages. These results demonstrate the value of the reactor as a tool for in situ evaluation of the SOA formation potential and OA evolution from ambient air.
Regional emission metrics for short-lived climate forcers from multiple models

For short-lived climate forcers (SLCFs), the impact of emissions depends on where and when the emissions take place. Comprehensive new calculations of various emission metrics for SLCFs are presented based on radiative forcing (RF) values calculated in four different (chemical-transport or coupled chemistry–climate) models. We distinguish between emissions during summer (May–October) and winter (November–April) for emissions in Europe and East Asia, as well as from the global shipping sector and global emissions. The species included in this study are aerosols and aerosol precursors (BC, OC, SO2, NH3), as well as ozone precursors (NOx, CO, VOCs), which also influence aerosols to a lesser degree. Emission metrics for global climate responses of these emissions, as well as for CH4, have been calculated using global warming potential (GWP) and global temperature change potential (GTP), based on dedicated RF simulations by four global models. The emission metrics include indirect cloud effects of aerosols and the semi-direct forcing for BC. In addition to the standard emission metrics for pulse and sustained emissions, we have also calculated a new emission metric designed for an emission profile consisting of a ramping period of 15 years followed by sustained emissions, which is more appropriate for a gradual implementation of mitigation policies. For the aerosols, the emission metric values are larger in magnitude for emissions in Europe than East Asia and for summer than winter. A variation is also observed for the ozone precursors, with largest values for emissions in East Asia and winter for CO and in Europe and summer for VOCs. In general, the variations between the emission metrics derived from different models are larger than the variations between regions and seasons, but the regional and seasonal variations for the best estimate also hold for most of the models individually. Further, the estimated climate impact of an illustrative mitigation policy package is robust even when accounting for the fact that the magnitude of emission metrics for different species in a given model is correlated. For the ramping emission metrics, the values are generally larger than for pulse or sustained emissions, which holds for all SLCFs. For SLCFs mitigation policies, the dependency of metric values on the region and season of emission should be considered.
Comparisons of urban and rural PM10−2.5 and PM2.5 mass concentrations and semi-volatile fractions in northeastern Colorado

Coarse (PM10−2.5) and fine (PM2.5) particulate matter in the atmosphere adversely affect human health and influence climate. While PM2.5 is relatively well studied, less is known about the sources and fate of PM10−2.5. The Colorado Coarse Rural-Urban Sources and Health (CCRUSH) study measured PM10−2.5 and PM2.5 mass concentrations, as well as the fraction of semi-volatile material (SVM) in each size regime (SVM2.5, SVM10−2.5), from 2009 to early 2012 in Denver and comparatively rural Greeley, Colorado. Agricultural operations east of Greeley appear to have contributed to the peak PM10−2.5 concentrations there, but concentrations were generally lower in Greeley than in Denver. Traffic-influenced sites in Denver had PM10−2.5 concentrations that averaged from 14.6 to 19.7 µg m−3 and mean PM10−2.5 ∕ PM10 ratios of 0.56 to 0.70, higher than at residential sites in Denver or Greeley. PM10−2.5 concentrations were more temporally variable than PM2.5 concentrations. Concentrations of the two pollutants were not correlated. Spatial correlations of daily averaged PM10−2.5 concentrations ranged from 0.59 to 0.62 for pairs of sites in Denver and from 0.47 to 0.70 between Denver and Greeley. Compared to PM10−2.5, concentrations of PM2.5 were more correlated across sites within Denver and less correlated between Denver and Greeley. PM10−2.5 concentrations were highest during the summer and early fall, while PM2.5 and SVM2.5 concentrations peaked in winter during periodic multi-day inversions. SVM10−2.5 concentrations were low at all sites. Diurnal peaks in PM10−2.5 and PM2.5 concentrations corresponded to morning and afternoon peaks of traffic activity, and were enhanced by boundary layer dynamics. SVM2.5 concentrations peaked around noon on both weekdays and weekends. PM10−2.5 concentrations at sites located near highways generally increased with wind speeds above about 3 m s−1. Little wind speed dependence was observed for the residential sites in Denver and Greeley. The mass concentration data reported here are being used in ongoing epidemiologic studies for PM in northeastern Colorado.
The role of dew as a night-time reservoir and morning source for atmospheric ammonia

Several field studies have proposed that the volatilization of NH3 from evaporating dew is responsible for an early morning pulse of ammonia frequently observed in the atmospheric boundary layer. Laboratory studies conducted on synthetic dew showed that the fraction of ammonium (NH4+) released as gas-phase ammonia (NH3) during evaporation is dependent on the relative abundances of anions and cations in the dew. Hence, the fraction of NH3 released during dew evaporation (Frac(NH3)) can be predicted given dew composition and pH. Twelve separate ambient dew samples were collected at a remote high-elevation grassland site in Colorado from 28 May to 11 August 2015. Average [NH4+] and pH were 26 µM and 5.2 respectively and were on the lower end of dew [NH4+] and pH observations reported in the literature. Ambient dew mass (in g m−2) was monitored with a dewmeter, which continuously measured the mass of a tray containing artificial turf representative of the grass canopy to track the accumulation and evaporation of dew. Simultaneous measurements of ambient NH3 indicated that a morning increase in NH3 was coincident in time with dew evaporation and that either a plateau or decrease in NH3 occurred once the dew had completely evaporated. This morning increase in NH3 was never observed on mornings without surface wetness (neither dew nor rain, representing one-quarter of mornings during the study period). Dew composition was used to determine an average Frac(NH3) of 0.94, suggesting that nearly all NH4+ is released back to the boundary layer as NH3 during evaporation at this site. An average NH3 emission of 6.2 ng m−2 s−1 during dew evaporation was calculated using total dew volume (Vdew) and evaporation time (tevap) and represents a significant morning flux in a non-fertilized grassland. Assuming a boundary layer height of 150 m, the average mole ratio of NH4+ in dew to NH3 in the boundary layer at sunrise is roughly 1.6 ± 0.7. Furthermore, the observed loss of NH3 during nights with dew is approximately equal to the observed amount of NH4+ sequestered in dew at the onset of evaporation. Hence, there is strong evidence that dew is both a significant night-time reservoir and strong morning source of NH3. The possibility of rain evaporation as a source of NH3, as well as dew evaporation influencing species of similar water solubility (acetic acid, formic acid, and HONO), is also discussed. If release of NH3 from dew and rain evaporation is pervasive in many environments, then estimates of NH3 dry deposition and NHx ( ≡  NH3 + NH4+) wet deposition may be overestimated by models that assume that all NHx deposited in rain and dew remains at the surface.
Fungal spores overwhelm biogenic organic aerosols in a midlatitudinal forest

Both primary biological aerosol particles (PBAPs) and oxidation products of biogenic volatile organic compounds (BVOCs) contribute significantly to organic aerosols (OAs) in forested regions. However, little is known about their relative importance in diurnal timescales. Here, we report biomarkers of PBAP and secondary organic aerosols (SOAs) for their diurnal variability in a temperate coniferous forest in Wakayama, Japan. Tracers of fungal spores, trehalose, arabitol and mannitol, showed significantly higher levels in nighttime than daytime (p < 0.05), resulting from the nocturnal sporulation under near-saturated relative humidity. On the contrary, BVOC oxidation products showed higher levels in daytime than nighttime, indicating substantial photochemical SOA formation. Using tracer-based methods, we estimated that fungal spores account for 45 % of organic carbon (OC) in nighttime and 22 % in daytime, whereas BVOC oxidation products account for 15 and 19 %, respectively. To our knowledge, we present for the first time highly time-resolved results that fungal spores overwhelmed BVOC oxidation products in contributing to OA especially in nighttime. This study emphasizes the importance of both PBAPs and SOAs in forming forest organic aerosols.