Items

Advanced search

Impact of very short-lived halogens on stratospheric ozone abundance and UV radiation in a geo-engineered atmosphere

The impact of very short-lived (VSL) halogenated source species on the ozone layer and surface erythemal ultraviolet radiation (UVERY) is investigated in the context of geo-engineering of climate by stratospheric sulfur injection. For a projected 2040 model atmosphere, consideration of VSL halogens at their upper limit results in lower ozone columns and higher UVERY due to geo-engineering for nearly all seasons and latitudes, with UVERY rising by 12% and 6% in southern and northern high latitudes, respectively. When VSL halogen sources are neglected, future UVERY increases due to declines in ozone column are nearly balanced by reductions of UVERY due to scattering by the higher stratospheric aerosol burden in mid-latitudes. Consideration of VSL sources at their upper limit tips the balance, resulting in annual average increases in UVERY of up to 5% in mid and high latitudes. Therefore, VSL halogens should be considered in models that assess the impact of stratospheric sulfur injections on the ozone layer.
Impact of the aging process of black carbon aerosols on their spatial distribution, hygroscopicity, and radiative forcing in a global climate model

Black carbon (BC) absorbs shortwave radiation more strongly than any other type of aerosol, and an accurate simulation of the aging processes of BC-containing particle is required to properly predict aerosol radiative forcing (ARF) and climate change. However, BC aging processes have been simplified in general circulation models (GCMs) due to limited computational resources. In particular, differences in the representation of the mixing states of BC-containing particles between GCMs constitute one of main reasons for the uncertainty in ARF estimates. To understand an impact of the BC aging processes and the mixing state of BC on the spatial distribution of BC and ARF caused by BC (BC-ARF), we implemented three different methods of incorporating BC aging processes into a global aerosol transport model, SPRINTARS: (1) the "AGV" method, using variable conversion rates of BC aging based on a new type of parameterization depending on both BC amount and sulfuric acid; (2) the "AGF" method, using a constant conversion rate used worldwide in GCMs; and (3) the "ORIG" method, which is used in the original SPRINTARS. First, we found that these different methods produced different BC burden within 10% over industrial areas and 50% over remote oceans. Second, a ratio of water-insoluble BC to total BC (WIBC ratio) was very different among the three methods. Near the BC source region, for example, the WIBC ratios were estimated to be 80–90% (AGV and AGF) and 50–60% (ORIG). Third, although the BC aging process in GCMs had small impacts on the BC burden, they had a large impact on BC-ARF through a change in both the WIBC ratio and non-BC compounds coating on BC cores. As a result, possible differences in the treatment of the BC aging process between aerosol modeling studies can produce a difference of approximately 0.3 Wm−2 in the magnitude of BC-ARF, which is comparable to the uncertainty suggested by results from a global aerosol modeling intercomparison project, AeroCom. The surface aerosol forcing efficiencies normalized by aerosol optical thickness and by BC burden varied greatly with region in the AGV method, which allowed for the existence of internally mixed BC and sulfate, whereas these were not varied with region in the AGF method. These results suggest that the efficiencies of BC-ARF obtained by previous studies using the AGF method are significantly underestimated.
The albedo properties of four clean stratocumulus clouds studied during the VOCALS-REX field campaign

The VOCALS-REx field campaign which took place in 2008 used several platforms to investigate the persistent marine stratocumulus cloud deck off the Chilean and Peruvian coasts. VOCALS-UK was the UK component of the experiment, during which the FAAM BAe-146 aircraft gathered data in the stratocumulus cloud. It flew 13 research flights including investigations along 20° S transects. In this paper, the shortwave cloud albedo derived from the Cloud Droplet Probe is compared with the albedo measured from two shortwave radiometers. Four clean cloud segments were selected for investigation. The suitability of the δ-Eddington approximation as a method of calculating shortwave albedo is investigated and it is found to be acceptable (with a R2 of 0.78) for solar zenith angles below 65 degrees.
Process analysis of regional ozone formation over the Yangtze River Delta, China using the Community Multi-scale Air Quality modeling system

A high O3 episode was detected in urban Shanghai, a typical city in the Yangtze River Delta (YRD) region in August 2010. The CMAQ integrated process rate method is applied to account for the contribution of different atmospheric processes during the high pollution episode. The analysis shows that the maximum concentration of ozone occurs due to transport phenomena, including vertical diffusion and horizontal advective transport. Gas-phase chemistry producing O3 mainly occurs at the height of 300–1500 m, causing a strong vertical O3 transport from upper levels to the surface layer. The gas-phase chemistry is an important sink for O3 in the surface layer, coupled with dry deposition. Cloud processes may contribute slightly to the increase of O3 due to convective clouds or to the decrease of O3 due to scavenging. The horizontal diffusion and heterogeneous chemistry contributions are negligible during the whole episode. Modeling results show that the O3 pollution characteristics among the different cities in the YRD region have both similarities and differences. During the buildup period, the O3 starts to appear in the city regions of the YRD and is then transported to the surrounding areas under the prevailing wind conditions. The O3 production from photochemical reaction in Shanghai and the surrounding area is most significant, due to the high emission intensity in the large city; this ozone is then transported out to sea by the westerly wind flow, and later diffuses to rural areas like Chongming island, Wuxi and even to Nanjing. The O3 concentrations start to decrease in the cities after sunset, due to titration of the NO emissions, but ozone can still be transported and maintain a significant concentration in rural areas and even regions outside the YRD region, where the NO emissions are very small.
Thunderstorms and upper troposphere chemistry during the early stages of the 2006 North American Monsoon

To study the meteorology and chemistry that is associated with the early stages of the North American Monsoon, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is applied for the first time at high resolution (4 km grid spacing, allowing for explicit representation of convection) over a large region (continental US and northern Mexico) for a multi-week (15 July to 7 August 2006) integration. Evaluation of model results shows that WRF-Chem reasonably represents the large-scale meteorology and strong convective storms, but tends to overestimate weak convection. In the upper troposphere, the WRF-Chem model predicts ozone (O3) and carbon monoxide (CO) to within 10–20% of aircraft and sonde measurements. Comparison of UT O3 and CO frequency distributions between WRF-Chem and satellite data indicates that WRF-Chem is lofting CO too frequently from the boundary layer (BL). This excessive lofting should also cause biases in the WRF-Chem ozone frequency distribution; however it agrees well with satellite data suggesting that either the chemical production of O3 in the model is overpredicted or there is too much stratosphere to troposphere transport in the model. Analysis of different geographic regions (West Coast, Rocky Mountains, Central Plains, Midwest, and Gulf Coast) reveals that much of the convective transport occurs in the Rocky Mountains, while much of the UT ozone chemical production occurs over the Gulf Coast and Midwest regions where both CO and volatile organic compounds (VOCs) are abundant in the upper troposphere and promote the production of peroxy radicals. In all regions most of the ozone chemical production occurs within 24 h of the air being lofted from the boundary layer. In addition, analysis of the anticyclone and adjacent air indicates that ozone mixing ratios within the anticyclone region associated with the North American Monsoon and just outside the anticyclone are similar. Increases of O3 within the anticyclone are strongly coincident with entrainment of stratospheric air into the anticyclone, but also are from in situ O3 chemical production. In situ O3 production is up to 17% greater within the anticyclone than just outside the anticyclone when the anticyclone is over the southern US indicating that the enhancement of O3 is most pronounced over regions with abundant VOCs.
Dynamic recycling of gaseous elemental mercury in the boundary layer of the Antarctic Plateau

Gaseous elemental mercury (Hg0) was investigated in the troposphere and in the interstitial air extracted from the snow at Dome Concordia station (alt. 3320 m) on the Antarctic Plateau during January 2009. Measurements and modeling studies showed evidence of a very dynamic and daily cycling of Hg0 inside the mixing layer with a range of values from 0.2 ng m−3 up to 2.3 ng m−3. During low solar irradiation periods, fast Hg0 oxidation processes in a confined layer were suspected. Unexpectedly high Hg0 concentrations for such a remote place were measured under higher solar irradiation due to snow photochemistry. We suggest that a daily cycling of reemission/oxidation occurs during summer within the mixing layer at Dome Concordia. Hg0 concentrations showed a negative correlation with ozone mixing ratios, which contrasts with atmospheric mercury depletion events observed during the Arctic spring. Unlike previous Antarctic studies, we think that atmospheric Hg0 removal may not be the result of advection processes. The daily and dramatic Hg0 losses could be a consequence of surface or snow induced oxidation pathways. It remains however unclear whether halogens are involved. The cycling of other oxidants should be investigated together with Hg species in order to clarify the complex reactivity on the Antarctic plateau.
The mixing state of carbonaceous aerosol particles in northern and southern California measured during CARES and CalNex 2010

Carbonaceous aerosols impact climate directly by scattering and absorbing radiation, and hence play a major, although highly uncertain, role in global radiative forcing. Commonly, ambient carbonaceous aerosols are internally mixed with secondary species such as nitrate, sulfate, and ammonium, which influences their optical properties, hygroscopicity, and atmospheric lifetime, thus impacting climate forcing. Aircraft-aerosol time-of-flight mass spectrometry (A-ATOFMS), which measures single-particle mixing state, was used to determine the fraction of organic and soot aerosols that are internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosols and Radiative Effects Study (CARES) and the Research at the Nexus of Air Quality and Climate Change (CalNex) field campaigns in the late spring and early summer of 2010. Nearly 88% of all A-ATOFMS measured particles (100–1000 nm in diameter) were internally mixed with secondary species, with 96% and 75% of particles internally mixed with nitrate and/or sulfate in southern and northern California, respectively. Even though atmospheric particle composition in both regions was primarily influenced by urban sources, the mixing state was found to vary greatly, with nitrate and soot being the dominant species in southern California, and sulfate and organic carbon in northern California. Furthermore, mixing state varied temporally in northern California, with soot becoming the prevalent particle type towards the end of the study as regional pollution levels increased. The results from these studies demonstrate that the majority of ambient carbonaceous particles in California are internally mixed and are heavily influenced by secondary species that are most prevalent in the particular region. Based on these findings, considerations of regionally dominant sources and secondary species, as well as temporal variations of aerosol physical and optical properties, will be required to obtain more accurate predictions of the climate impacts of aerosol in California.
An analysis of atmospheric CH4 concentrations from 1984 to 2008 with a single box atmospheric chemistry model

We present a single box atmospheric chemistry model involving atmospheric methane (CH4), carbon monoxide (CO) and radical hydroxyl (OH) to analyze atmospheric CH4 concentrations from 1984 to 2008. When OH is allowed to vary, the modeled CH4 is 20 ppb higher than observations from the NOAA/ESRL and AGAGE networks for the end of 2008. However, when the OH concentration is held constant at 106 molecule cm−3, the simulated CH4 shows a trend approximately equal to observations. Both simulations show a clear slowdown in the CH4 growth rate during recent decades, from about 13 ppb yr−1 in 1984 to less than 5 ppb yr−1 in 2003. Furthermore, if the constant OH assumption is credible, we think that this slowdown is mainly due to a pause in the growth of wetland methane emissions. In simulations run for the Northern and Southern Hemispheres separately, we find that the Northern Hemisphere is more sensitive to wetland emissions, whereas the southern tends to be more perturbed by CH4 transportation, dramatic OH change, and biomass burning. When measured CO values from NOAA/ESRL are used to drive the model, changes in the CH4 growth rate become more consistent with observations, but the long-term increase in CH4 is underestimated. This shows that CO is a good indicator of short-term variations in oxidizing power in the atmosphere. The simulation results also indicate the significant drop in OH concentrations in 1998 (about 5% lower than the previous year) was probably due to an abrupt increase in wetland methane emissions during an intense EI Niño event. Using a fixed-lag Kalman smoother, we estimate the mean wetland methane flux is about 128 Tg yr−1 through the period 1984–2008. This study demonstrates the effectiveness in examining the role of OH and CO in affecting CH4.
Heterogeneous chlorine activation on stratospheric aerosols and clouds in the Arctic polar vortex

Chlorine activation in the Arctic is investigated by examining different parameterizations for uptake coefficients on stratospheric aerosols, high-resolution in-situ measurements and vortex-wide satellite observations. The parameterizations for heterogeneous chemistry on liquid aerosols are most sensitive to temperature with the reaction rates doubling for every 1 K increase in temperature. However, differences between the currently available parameterizations are negligible. For Nitric Acid Trihydrate particles (NAT) the major factors of uncertainty are the number density of nucleated particles and different parameterizations for heterogeneous chemistry. These two factors induce an uncertainty that covers several orders of magnitude on the reaction rate. Nonetheless, since predicted reaction rates on liquid aerosols always exceed those on NAT, the overall uncertainty for chlorine activation is small. In-situ observations of ClOx from Arctic winters in 2005 and 2010 are used to evaluate the heterogeneous chemistry parameterizations. The conditions for these measurements proved to be very different between those two winters with HCl being the limiting reacting partner for the 2005 measurements and ClONO2 for the 2010 measurements. Modeled levels of chlorine activation are in very good agreement with the in-situ observations and the surface area provided by Polar Stratospheric Clouds (PSCs) has only a limited impact on modeled chlorine activation. This indicates that the parameterizations give a good representation of the processes in the atmosphere. Back-trajectories started on the location of the observations in 2005 indicate temperatures on the threshold for PSC formation, hence the surface area is mainly provided by the background aerosol. Still, the model shows additional chlorine activation during this time-frame, providing cautionary evidence for chlorine activation even in the absence of PSCs. Vortex-averaged satellite observations by the MLS instrument also show no definite connection between chlorine activation and PSC formation. The inter -and intra-annual variability of vortex-average HCl and HNO3 based on MLS observations is examined for the Arctic winters 2004/2005 to 2010/2011. These observations show that removal of HCl and HNO3 from the gas-phase are not correlated. HNO3 loss exhibits great inter-annual variability depending on prevailing temperatures while HCl loss is continuous through December without considerable inter- or intra-annual variability. Only the recovery of HCl in late winter depends on the level of denitrification. Hence, the occurrence of HNO3 containing PSC particles does not seem to have a significant effect on the speed of initial chlorine activation on a vortex-wide scale.
Initial MST radar observations of upper tropospheric-lower stratospheric duct-like structures over Jicamarca, Peru

Persistent wind jet structures along zonal and meridional fields, believed to be caused by stationary gravity waves, were detected in February 1999 in mesosphere-stratosphere-troposphere (MST) radar wind measurements of the troposphere and lower stratosphere over Jicamarca, Peru. Over a continuous seven day span of MST-data analyzed in this study, two days of observations showed signatures of wave-like structures in the upper troposphere/lower stratosphere wind jets associated with the phases of the stationary gravity waves. We believe these wave-like structures are ducted gravity waves. We present these initial observations, their characteristics, and the results of simple numerical simulations used in an attempt to mimic these observed features. Although a fair replication of the observed ducted structure in the numerical model is found, the observed period of ~90 min is nonetheless much longer than what is traditionally observed. As a result, the specific physical nature of the observed structures is not fully established. Nevertheless, given the high quality of the observations, we demonstrate here that continued analysis of this data set and concurrent modeling efforts will allow for a better understanding of Doppler ducts at high spatial and temporal resolution, and the results presented here can ultimately be applied to studies of middle atmospheric fronts, ducts, and bores.