Aerosol radiative forcing over the Indo-Gangetic plains during major dust storms

Indo-Gangetic (IG) alluvial plains, one of the largest river basins in the world, suffers from the long range transport of mineral dust from the western arid and desert regions of Africa, Arabia and Rajasthan during the summer (pre-monsoon season, April–June). These dust storms influence the aerosol optical depth (AOD) across the IG plains. The Kanpur AERONET (Aerosol Robotic Network) station and Moderate Resolution Imaging Spectro-radiometer (MODIS) data show pronounced effect on the aerosol optical properties and aerosol size distribution during major dust storm events over the IG plains that have significant effect on the aerosol radiative forcing (ARF). The multi-band AOD, from AERONET and MODIS, show contrasting changes in wavelength dependency over dust affected regions. A time collocated (±30 min) validation of AERONET AOD with MODIS Terra (level 2 swath product) over Kanpur, at a common wavelength of 550 nm for the period 2001–2005 show moderate correlation (R²∼0.6) during the summer season. The average surface forcing is found to change by −23 W m⁻² during dust events and the top of the atmosphere (TOA) forcing change by −11 W m⁻² as compared to the non-dusty clear-sky days. A strong correlation is found between AOD at 500 nm and the ARF. At surface, the correlation coefficient between AOD and ARF is found to be high (R²=0.925) and is found to be moderate (R²=0.628) at the TOA. The slope of the regression line gives the aerosol forcing efficiency at 500 nm of about −46±2.6 W m⁻² and −17±2.5 W m⁻² at the surface and the TOA, respectively. The ARF is found to increase with the advance of the dry season in conjunction with the gradual rise in AOD (at 500 nm) from April (0.4–0.5) to June (0.6–0.7) over the IG plains.     

A review of surface ozone in the polar regions

Surface ozone records from ten polar research stations were investigated for the dependencies of ozone on radiative processes, snow-photochemisty, and synoptic and stratospheric transport. A total of 146 annual data records for the Arctic sites Barrow, Alaska; Summit, Greenland; Alert, Canada; Zeppelinfjellet, Norway; and the Antarctic stations Halley, McMurdo, Neumayer, Sanae, Syowa, and South Pole were analyzed. Mean ozone at the Northern Hemisphere (NH) stations (excluding Summit) is ∼5 ppbv higher than in Antarctica. Statistical analysis yielded best estimates for the projected year 2005 median annual ozone mixing ratios, which for the Arctic stations were 33.5 ppbv at Alert, 28.6 ppbv at Barrow, 46.3 ppbv ppb at Summit and 33.7 ppbv at Zeppelinfjellet. For the Antarctic stations the corresponding ozone mixing ratios were 21.6 ppbv at Halley, 27.0 ppbv at McMurdo, 24.9 ppbv at Neumayer, 27.2 ppbv at Sanae, 29.4 ppbv at South Pole, and 25.8 ppbv at Syowa. At both Summit (3212 m asl) and South Pole (2830 m asl), annual mean ozone is higher than at the lower elevation and coastal stations. A trend analysis revealed that all sites in recent years have experienced low to moderate increases in surface ozone ranging from 0.02 to 0.26 ppbv yr⁻¹, albeit none of these changes were found to be statistically significant trends. A seasonal trend analysis showed above-average increases in ozone during the spring and early summer periods for both Arctic (Alert, Zeppelinfjellet) and Antarctic (McMurdo, Neumayer, South Pole) sites. In contrast, at Barrow, springtime ozone has been declining. All coastal stations experience springtime episodes with rapid depletion of ozone in the boundary layer, attributable to photochemically catalyzed ozone depletion from halogen chemistry. This effect is most obvious at Barrow, followed by Alert. Springtime depletion episodes are less pronounced at Antarctic stations. At South Pole, during the Antarctic spring and summer, photochemical ozone production yields frequent episodes with enhanced surface ozone. Other Antarctic stations show similar, though less frequent spring and summertime periods with enhanced ozone. The Antarctic data provide evidence that austral spring and summertime ozone production in Antarctica is widespread, respectively, affects all stations at least through transport events. This ozone production contributes to a several ppbv enhancement in the annual mean ozone over the Antarctic plateau; however, it is not the determining process in the Antarctic seasonal ozone cycle. Although Summit and South Pole have many similarities in their environmental conditions, this ozone production does not appear to be of equal importance at Summit. Amplitudes of diurnal, summertime ozone cycles at these polar sites are weaker than at lower latitude locations. Amplitudes of seasonal ozone changes are larger in the Southern Hemisphere (by ∼5 ppbv), most likely due to less summertime photochemical ozone loss and more transport of ozone-rich air to the Arctic during the NH spring and summer months.     

Temporal trends of black carbon concentrations and regional climate forcing in the southeastern United States

The effect of black carbon (BC) on climate forcing is potentially important, but its estimates have large uncertainties due to a lack of sufficient observational data. The BC mass concentration in the southeastern US was measured at a regionally representative site, Mount Gibbes (35.78°N, 82.29°W, 2006 m MSL). The air mass origin was determined using 48-h back trajectories obtained from the hybrid single-particle Lagrangian integrated trajectory model. The highest average concentration is seen in polluted continental air masses and the lowest in marine air masses. During the winter, the overall average BC value was 74.1 ng m⁻³, whereas the overall summer mean BC value is higher by a factor of 3. The main reason for the seasonal difference may be enhanced thermal convection during summer, which increases transport of air pollutants from the planetary boundary layer of the surrounding urban area to this rural site. In the spring of 1998, abnormally high BC concentrations from the continental sector were measured. These concentrations were originating from a biomass burning plume in Mexico. This was confirmed by the observations of the Earth probe total ozone mapping spectrometer. The BC average concentrations of air masses transported from the polluted continental sector during summer are low on Sunday to Tuesday with a minimum value of 256 ng m⁻³ occurring on Monday, and high on Wednesday to Friday with a maximum value of 379 ng m⁻³ occurring on Friday. The net aerosol radiative forcing (scattering effects plus absorption effects) per unit vertical depth at 2006 m MSL is calculated to be −1.38×10⁻³ W m⁻³ for the southeastern US. The magnitude of direct radiative forcing by aerosol scattering is reduced by 15±7% due to the BC absorption.     

NOX fluxes from three kinds of agricultural lands in the Yangtze Delta,China

Static chamber method was adopted to measure the surface exchanges of NO and NO₂ between three kinds of agricultural lands and the atmosphere during spring–summer period in the Yangtze Delta, China. The average NO fluxes were 20.9, 27.4 and 21.4 ng N m⁻² s⁻¹, respectively, for cabbage (CA, cultivation of celery occurred along with cabbage), potato (PO) and soybean (SY) fields. The average NO₂ fluxes were −1.12, 0.93 and −0.68 ng N m⁻² s⁻¹, respectively, for the cabbage, potato and soybean fields. Apparently, negative linear correlation was found between the NO₂ fluxes from the CK plot (tilled conventionally but did not cultivate any seeds) and its ambient concentrations, and the compensation point was calculated to be 0.92 ppbv. The total NO emission from the vegetable lands and SY land in this region during spring–summer period was roughly estimated to be 15.9 Gg N, which accounted for about 11.2% of the estimated value of total NO emissions in the July of 1999 from Chinese agricultural fields.     

Direct radiative forcing and atmospheric absorption by boundary layer aerosols in the southeastern US: model estimates on the basis of new observations

In an effort to reduce uncertainties in the quantification of aerosol direct radiative forcing (ADRF) in the southeastern United States (US), a field column experiment was conducted to measure aerosol radiative properties and effects at Mt. Mitchell, North Carolina, and at an adjacent valley site. The experimental period was from June 1995 to mid-December 1995. The aerosol optical properties (single scattering albedo and asymmetry factor) needed to compute ADRF were obtained on the basis of a procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, aerosol optical depth, and diffuse-to-direct solar irradiance ratio. The regional values of ADRF at the surface and top of atmosphere (TOA), and atmospheric aerosol absorption are derived using the obtained aerosol optical properties as inputs to the column radiation model (CRM) of the community climate model (CCM3). The cloud-free instantaneous TOA ADRFs for highly polluted (HP), marine (M) and continental (C) air masses range from 20.3 to −24.8, 1.3 to −10.4, and 1.9 to −13.4 W m⁻², respectively. The mean cloud-free 24-h ADRFs at the TOA (at the surface) for HP, M, and C air masses are estimated to be −8±4 (−33±16), −7±4 (−13±8), and −0.14±0.05 (−8±3) W m⁻², respectively. On the assumption that the fractional coverage of clouds is 0.61, the annual mean ADRFs at the TOA and the surface are −2±1, and −7±2 W m⁻², respectively. This also implies that aerosols currently heat the atmosphere over the southeastern US by 5±3 W m⁻² on annual timescales due to the aerosol absorption in the troposphere.     

Aerosol physical,chemical and optical properties during the Rocky Mountain Airborne Nitrogen and Sulfur study

During the Rocky Mountain Airborne Nitrogen and Sulfur (RoMANS) study, conducted during the spring and summer of 2006, a suite of instruments located near the eastern boundary of Rocky Mountain National Park (RMNP) measured aerosol physical, chemical and optical properties. Three instruments, a differential mobility particle sizer (DMPS), an optical particle counter (OPC), and an aerodynamic particle sizer (APS), measured aerosol size distributions. Aerosols were sampled by an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampler and a URG denuder/filter-pack system for compositional analysis. An Optec integrating nephelometer measured aerosol light scattering. The spring time period had lower aerosol concentrations, with an average volume concentration of 2.2 ± 2.6 μm³ cm^?3 compared to 6.5 ± 3.9 μm³ cm^?3 in the summer. During the spring, soil was the single largest constituent of PM_2.5 mass, accounting for 32%. During the summer, organic carbon accounted for 60% of the PM_2.5 mass. Sulfates and nitrates had higher fractional contributions in the spring than the summer. Variability in aerosol number and volume concentrations and in composition was greater in the spring than in the summer, reflecting differing meteorological conditions. Aerosol scattering coefficients (b_sp) measured by the nephelometer compared well with those calculated from Mie theory using size distributions, composition data and modeled RH dependent water contents.     

Nitric oxide emissions from soils amended with municipal waste biosolids

Land spreading nitrogen-rich municipal waste biosolids (NO₃⁻-N<256 mg N kg⁻¹ dry weight, NH₃-N∼23,080 mg N kg⁻¹ dry weight, Total Kjeldahl N∼41,700 mg N kg⁻¹ dry weight) to human food and non-food chain land is a practice followed throughout the US. This practice may lead to the recovery and utilization of the nitrogen by vegetation, but it may also lead to emissions of biogenic nitric oxide (NO), which may enhance ozone pollution in the lower levels of the troposphere. Recent global estimates of biogenic NO emissions from soils are cited in the literature, which are based on field measurements of NO emissions from various agricultural and non-agricultural fields. However, biogenic emissions of NO from soils amended with biosolids are lacking. Utilizing a state-of-the-art mobile laboratory and a dynamic flow-through chamber system, in-situ concentrations of nitric oxide (NO) were measured during the spring/summer of 1999 and winter/spring of 2000 from an agricultural soil which is routinely amended with municipal waste biosolids. The average NO flux for the late spring/summer time period (10 June 1999–5 August 1999) was 69.4±34.9 ng N m⁻² s⁻¹. Biosolids were applied during September 1999 and the field site was sampled again during winter/spring 2000 (28 February 2000–9 March 2000), during which the average flux was 3.6±1.7 ng N m⁻² s⁻¹. The same field site was sampled again in late spring (2–9 June 2000) and the average flux was 64.8±41.0 ng N m⁻² s⁻¹. An observationally based model, developed as part of this study, found that summer accounted for 60% of the yearly emission while fall, winter and spring accounted for 20%, 4% and 16% respectively. Field experiments were conducted which indicated that the application of biosolids increases the emissions of NO and that techniques to estimate biogenic NO emissions would, on a yearly average, underestimate the NO flux from this field by a factor of 26. Soil temperature and % water filled pore space (%WFPS) were observed to be significant variables for predicting NO emissions, however %WFPS was found to be most significant during high soil temperature conditions. In the range of pH values found at this site (5.8±0.3), pH was not observed to be a significant parameter in predicting NO emissions.     

Comparison between the atmospheric boundary layer in Paris and its rural suburbs during the ECLAP experiment

The ECLAP experiment has been performed during the winter of 1995 in order to study the influence of the urban area of Paris on the vertical structure and diurnal evolution of the atmospheric boundary layer, in situations favourable to intense urban heat island and pollution increase. One urban site and one rural site have been instrumented with sodars, lidars and surface measurements. Additional radiosondes, 100 m masts and Eiffel Tower data were also collected. This paper gives a general overview of this experiment, and presents results of the analysis of four selected days, characterized by various wind directions and temperature inversion strengths. This analysis, which consists in a comparison between data obtained in the two sites, has been focused on three parameters of importance to the ABL dynamics: the standard deviation of vertical velocity, the surface sensible heat flux, and the boundary layer height. The vertical component of turbulence is shown to be enhanced by the urban area, the amplitude of this effect strongly depending on the meteorological situation. The sensible heat flux in Paris is generally found larger than in the rural suburbs. The most frequent differences range from 25–65 W m^-2, corresponding to relative differences of 20–60%. The difference of unstable boundary layer height between both sites are most of the time less than 100 m. However, sodar and temperature data show that the urban influence is enhanced during night-time and transitions between stable and unstable regimes.     

Impact of anthropogenic heat on urban climate in Tokyo

This study quantifies the contribution through energy consumption, to the heat island phenomena and discussed how reductions in energy consumption could mitigate impacts on the urban thermal environment. Very detailed maps of anthropogenic heat in Tokyo were drawn with data from energy statistics and a very detailed digital geographic land use data set including the number of stories of building at each grid point. Animated computer graphics of the annual and diurnal variability in Tokyo's anthropogenic heat were also prepared with the same data sources. These outputs characterize scenarios of anthropogenic heat emission and can be applied to a numerical simulation model of the local climate. The anthropogenic heat flux in central Tokyo exceeded 400 W m⁻² in daytime, and the maximum value was 1590 W m⁻² in winter. The hot water supply in offices and hotels contributed 51% of this 1590 W m⁻². The anthropogenic heat flux from the household sector in the suburbs reached about 30 W m⁻² at night. Numerical simulations of urban climate in Tokyo were performed by referring to these maps. A heat island appeared evident in winter because of weakness of the sea breeze from Tokyo Bay. At 8 p.m., several peaks of high-temperature appeared, around Otemachi, Shinjuku and Ikebukuro; the areas with the largest anthropogenic heat fluxes. In summer the shortwave radiation was strong and the influence of anthropogenic heat was relatively small. In winter, on the other hand, the shortwave radiation was weak and the influence of anthropogenic heat was relatively large. The effects of reducing energy consumption, by 50% for hot water supply and 100% for space cooling, on near surface air temperature would be at most −0.5°C.     

Biogenic nitric oxide emissions from cropland soils

Emissions of nitric oxide (NO) were determined during late spring and summer 1995 and the spring of 1996 from four agricultural soils on which four different crops were grown. These agricultural soils were located at four different sites throughout North Carolina. Emission rates were calculated using a dynamic flow-through chamber system coupled to a mobile laboratory for in-situ analysis. Average NO fluxes during late spring 1995 were: 50.9±47.7 ng N m⁻² s⁻¹ from soil planted with corn in the lower coastal plain. Average NO fluxes during summer 1995 were: 6.4±4.6 and 20.2±19.0 ng N m⁻² s⁻¹, respectively, from soils planted with corn and soybean in the coastal region; 4.2±1.7 ng N m⁻² s⁻¹ from soils planted with tobacco in the piedmont region; and 8.5±4.9 ng N m⁻² s⁻¹ from soils planted with corn in the upper piedmont region. Average NO fluxes for spring 1996 were: 66.7±60.7 ng N m⁻² s⁻¹ from soils planted with wheat in the lower coastal plain; 9.5±2.9 ng N m⁻² s⁻¹ from soils planted with wheat in the coastal plain; 2.7±3.4 ng N m⁻² s⁻¹ from soils planted with wheat in the piedmont region; and 56.1±53.7 ng N m⁻² s⁻¹ from soils planted with corn in the upper piedmont region. An apparent increase in NO flux with soil temperature was present at all of the locations. The composite data from all the research sites revealed a general positive trend of increasing NO flux with soil water content. In general, increases in total extractable nitrogen (TEN) appeared to be related to increased NO emissions within each site, however a consistent trend was not evident across all sites.     

222Rn concentrations,natural flow rate and the radiation exposure levels in the Nerja Cave

²²²Rn concentrations in the air in Nerja Cave (Spain) have been measured over 4 yr and at four sampling points. Concentrations average 168 Bq m^-3 in the spring–summer when the temperature lapse rate provides a stable cave atmosphere. In the autumn–winter, the radon levels decrease to 48 Bq m^-3. ²²²Rn flux has also been measured for soils in the cave, with an average value of 34 × 10^-3 Bq m^-2 s^-1. The average natural flow rate in the spring–summer is about 0.70 m³ s^-1 and the autumn–winter is approximately 3.6 m³ s^-1 determined over 1992–1995. The radiation exposure levels for workers and tourists represent only a low percentage of the exposure guides for the general population.     

Air–land exchanges of CO2, CH4 and N2O measured by FTIR spectrometry and micrometeorological techniques

Micrometeorological flux-gradient and nocturnal boundary layer methods were combined with Fourier transform infrared (FTIR) spectroscopy for high-precision trace gas analysis to measure fluxes of the trace gases CO₂, CH₄ and N₂O between agricultural fields and the atmosphere. The FTIR measurements were fully automated and routinely obtained a precision of 0.1–0.2% for several weeks during a measurement campaign in October 1995. In flux-gradient measurements, vertical profiles of the trace gases were measured every 30 min from the ground to 22 m. When combined with independent micrometeorological measurements of water vapour fluxes, trace gas fluxes from the underlying surface could be determined. In the nocturnal boundary layer method the rate of change in mass storage in the 0–22 m layer was combined with fluxes measured at 22 m to estimate surface fluxes. Daytime fluxes for CO₂ were −0.78±0.40 (1σ) mg CO₂ m⁻² s⁻¹. Daytime fluxes of N₂O and CH₄ were very small and difficult to measure reliably using the flux-gradient technique, despite the high precision of the concentration measurements. Mean daytime flux for N₂O was 17±48 ng N m⁻² s⁻¹, while the corresponding flux for CH₄ was 47±410 ng CH₄ m⁻² s⁻¹. The mean nighttime flux of CO₂ estimated using the nocturnal boundary layer method was +0.15±0.05 mg CO₂ m⁻² s⁻¹, in good agreement with chamber measurements of respiration rates. Nighttime fluxes of CH₄ and N₂O from the nocturnal boundary layer method were 109±69 ng CH₄ m⁻² s⁻¹ and 2±3.2 ng N m⁻² s⁻¹, respectively, in good agreement with chamber measurements and inventory estimates based on the sheep and cattle stocking rates in the region. The suitability of FTIR-based methods for long term monitoring of spatially and temporally averaged flux measurements is discussed.     

Seasonal variation of black carbon aerosols over a tropical urban city of Pune,India

Black carbon (BC) aerosols were monitored continuously at Pune, a tropical urban location in southwest India, using aethalometer AE-42 model. Results of the data for the 1-year period (January to December 2005) have been discussed here. Seasonal and diurnal variations of BC in relation to changes in the regional meteorological conditions and local boundary layer characteristics have been studied along with the mass fraction of BC to the total suspended particulates (TSP) in different months. Also, using the Hysplit model, back-trajectories are studied to assess the sources for transported BC particles. The data collected during January to December 2005 indicated that annual average BC concentration (4.1 μg m⁻³) at Pune was comparable to that reported for other urban locations in southern Indian region. During winter season, BC concentrations were maximum (about 80% more than annual mean), mainly due to prevailing meteorological conditions like low wind speeds and low ventilation coefficients; as well as due to the transport from northeast regions. Minimum BC concentrations were observed during monsoon season (about 68% less than annual mean), which could be attributed to the wash-out effects due to precipitation as well as due to southwesterly winds coming from marine areas. Diurnal variation of BC showed two peaks, one in morning and another in the evening, which are mostly related to the daily changes in the local boundary layer. However, the intensity of local traffic emissions could have some impact on the magnitude of these peaks. BC aerosols formed about 2.3% of the total aerosol mass fraction at Pune.     

Measurements of GEM fluxes and atmospheric mercury concentrations (GEM,RGM and Hgp) from an agricultural field amended with biosolids in Southern Ont., Canada (October 2004–November 2004)

Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hg^p) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g⁻¹±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m⁻² h⁻¹(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m⁻² h⁻¹ and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m⁻² h⁻¹. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m⁻³), Hg^p (3.0±6.2 pg m⁻³) and GEM (1.8±0.2 ng m⁻³) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hg^p (25.8 pg m⁻³) and RGM (21.7 pg m⁻³) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hg^p but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hg^p at Maryhill.     

Black carbon concentrations in precipitation and near surface air in and near Halifax,Nova Scotia

Black carbon (soot) concentrations have been measured in rain water, snow samples and near surface air at several locations in Nova Scotia, Canada. The average black carbon concentration in near surface air in summer was found to be 0.54 μg m^-3 compared to 1.74 μg m^-3 in the winter season. These values are comparable to black carbon concentrations found in other mid-size urban areas. The black carbon concentration in rain water and snow samples varied between an undetectable amount to about 20 μg kg^-1 of rain (or melt) water. The relatively low concentrations of black carbon in precipitation are attributed to extratropical cyclones that often develop off-shore to the east and south of Nova Scotia in relatively clean conditions of the marine boundary layer.     

Annual evolution and generation mechanisms of particulate nitrate in Madrid

During the course of one year (March 2004–March 2005), PM_2.5 particulate nitrate concentrations were semi-continuously measured every 10 min at a Madrid suburban site using the Rupprecht and Patashnick Series 8400N Ambient Particulate Nitrate Monitor (8400N). Gaseous pollutants (NO, NO₂, O₃, HCHO, HNO₂) were simultaneously measured with a DOAS spectrometer (OPSIS AR-500) and complementary meteorological information was obtained by a permanent tower. The particulate nitrate concentrations ranged from the instrumental detection limit of around 0.2 μg m⁻³, up to a maximum of about 25 μg m⁻³. The minimum monthly average was reached during August (0.32 μg m⁻³) and the maximum during November (3.0 μg m⁻³). Due to the semi-volatile nature of ammonium nitrate, peaks were hardly present during summer air pollution episodes. A typical pattern during days with low dispersive conditions was characterized by a steep rise of particulate nitrate in the morning, reaching maximum values between 9 and 14 UTC, followed by a decrease during the evening. On some occasions a light increase was observed at nighttime. During spring episodes, brief diurnal nitrate peaks were recorded, while during the autumn and winter episodes, later and broader nitrate peaks were registered. Analysis of particulate nitrate and related gaseous species indicated the photo-chemical origin of the morning maxima, delayed with respect to NO and closely associated with secondary NO₂ maximum values. The reverse evolution of nitrate and nitrous acid was observed after sunrise, suggesting a major contribution from HNO₂ photolysis to OH formation at this time of the day, which would rapidly produce nitrate in both gaseous and particulate phase. Some nocturnal nitrate maxima appeared under high humidity conditions, and a discussion about their origin involving different possible mechanisms is presented, i.e. the possibility that these nocturnal maximum values could be related to the heterogeneous formation of nitrous and nitric acid by the hydrolysis of NO₂ on wet aerosols.     

Ozone and meteorological boundary-layer conditions at Summit,Greenland, during 3–21 June 2000

The temporal and spatial distributions of boundary-layer ozone were studied during June 2000 at Summit, Greenland, using surface-level measurements and vertical profiling from a tethered balloon platform. Three weeks of continuous ozone surface data, 133 meteorological vertical profile data and 82 ozone vertical profile data sets were collected from the surface to a maximum altitude of 1400 m above ground.The lower atmosphere at Summit was characterized by the prevalence of strong stable conditions with strong surface temperature inversions. These inversions reversed to neutral to slightly unstable conditions between ∼9.00 and 18.00 h local time with the formation of shallow mixing heights of ∼70–250 m above the surface.The surface ozone mixing ratio ranged from 39 to 68 ppbv and occasionally had rapid changes of up to 20 ppb in 12 h. The diurnal mean ozone mixing ratio showed diurnal trends indicating meteorological and photochemical controls of surface ozone. Vertical profiles were within the range of 37–76 ppb and showed strong stratification in the lower troposphere. A high correlation of high ozone/low water vapor air masses indicated the transport of high tropospheric/low stratospheric air into the lower boundary layer. A ∼0.1–3 ppb decline of the ozone mixing ratio towards the surface was frequently observed within the neutrally stable mixed layer during midday hours. These data suggest that the boundary-layer ozone mixing ratio and ozone depletion and deposition to the snowpack are influenced by photochemical processes and/or transport phenomena that follow diurnal dependencies. With 37 ppb of ozone being the lowest mixing ratio measured in all data no evidence was seen for the occurrence of ozone depletion episodes similar to those that have been reported within the boundary layer at coastal Arctic sites during springtime.     

Vertical mixing above Summit,Greenland: Insights into seasonal and high frequency variability from the radionuclide tracers 7Be and 210Pb

The activity of the natural radionuclide tracers ⁷Be and ²¹⁰Pb has been determined in bulk aerosol samples collected over 2-day intervals for nearly five full years at Summit, Greenland. Year-round sampling was conducted in three campaigns; summer 1997 to summer 1998, summer 2000 to summer 2002, and summer 2003 to present. As in previous summer campaigns at Summit, and a year-round investigation at Dye 3, variations in the activities of the tracers on short time scales were strongly correlated despite the upper troposphere/lower stratosphere source of ⁷Be and the continental surface source of ²²²Rn (precursor of ²¹⁰Pb). This behavior is attributed to boundary layer dynamics exerting the dominant control on activities in air just above the ice sheet. Aerosols and associated species are depleted from the boundary layer above the snow when a strong inversion limits exchange with the free troposphere. Episodic weakening of the inversion allows ventilation of the boundary layer. This cycle drives simultaneous decreases and increases in the radionuclide tracers. The correlation between ⁷Be and ²¹⁰Pb on seasonal and annual bases was found to be stronger than at Dye 3, and the average activity of ⁷Be was lower at Summit despite the higher elevation (3.0 versus 2.5 km). These observations indicate that the boundary layer at Summit is more effectively isolated than at Dye 3. The activity of ⁷Be at Summit peaked in June or July all 5 years, closely following the seasonality of stratospheric injection of ⁷Be into the Arctic troposphere (based on seasonality of the ¹⁰Be/⁷Be ratio previously measured at Alert, NWT). This suggests that when the boundary layer at Summit is replenished by ventilation, it receives air reflecting the composition of the mid and upper troposphere.     

Aqueous-phase reactive uptake of dicarbonyls as a source of organic aerosol over eastern North America

We use a global 3-D atmospheric chemistry model (GEOS-Chem) to simulate surface and aircraft measurements of organic carbon (OC) aerosol over eastern North America during summer 2004 (ICARTT aircraft campaign), with the goal of evaluating the potential importance of a new secondary organic aerosol (SOA) formation pathway via irreversible uptake of dicarbonyl gases (glyoxal and methylglyoxal) by aqueous particles. Both dicarbonyls are predominantly produced in the atmosphere by isoprene, with minor contributions from other biogenic and anthropogenic precursors. Dicarbonyl SOA formation is represented by a reactive uptake coefficient γ = 2.9 × 10^?3 and takes place mainly in clouds. Surface measurements of OC aerosol at the IMPROVE network in the eastern U.S. average 2.2 ± 0.7 μg C m^?3 for July–August 2004 with little regional structure. The corresponding model concentration is 2.8 ± 0.8 μg C m^?3, also with little regional structure due to compensating spatial patterns of biogenic, anthropogenic, and fire contributions. Aircraft measurements of water-soluble organic carbon (WSOC) aerosol average 2.2 ± 1.2 μg C m^?3 in the boundary layer (<2 km) and 0.9 ± 0.8 μg C m^?3 in the free troposphere (2–6 km), consistent with the model (2.0 ± 1.2 μg C m^?3 in the boundary layer and 1.1 ± 1.0 μg C m^?3 in the free troposphere). Source attribution for the WSOC aerosol in the model boundary layer is 27% anthropogenic, 18% fire, 28% semi-volatile SOA, and 27% dicarbonyl SOA. In the free troposphere it is 13% anthropogenic, 37% fire, 23% semi-volatile SOA, and 27% dicarbonyl SOA. Inclusion of dicarbonyl SOA doubles the SOA contribution to WSOC aerosol at all altitudes. Observed and simulated correlations of WSOC aerosol with other chemical variables measured aboard the aircraft suggest a major SOA source in the free troposphere compatible with the dicarbonyl mechanism.     

An analysis of seasonal surface dust aerosol concentrations in the western US (2001–2004): Observations and model predictions

Long-term surface observations indicate that soil dust represents over 30% of the annual fine (particle diameter less than 2.5 μm) particulate mass in many areas of the western US; in spring and summer, it represents an even larger fraction. There are numerous dust-producing playas in the western US, but surface dust aerosol concentrations in this region are also influenced by dust of Asian origin. This study examines the seasonality of surface soil dust concentrations at 15 western US sites using observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network from 2001 to 2004. Average soil concentrations in particulate matter less than 10 μm in diameter (PM₁₀) were lowest in winter and peaked during the summer months at these sites; however, episodic higher-concentration events (>10 μg m⁻³) occurred in the spring, the time of maximum Asian dust transport to the western US. Simulated surface dust concentrations from the Navy Aerosol Analysis and Prediction System (NAAPS) suggested that long-range transport from Asia dominates surface dust concentrations in the western US in the spring, and that, although some long-range transport does occur throughout the year (1–2 μg m⁻³), locally generated dust plays a larger role in the region in summer and fall. However, NAAPS simulated some anomalously high concentrations (>50 μg m⁻³) of local dust in the fall and winter months over portions of the western US. Differences between modeled and observed dust concentrations were attributed to overestimation of total observed soil dust concentrations by the assumptions used to convert IMPROVE measurements into PM₁₀ soil concentrations, lack of inhibition of model dust production in snow-covered regions, and lack of seasonal agricultural sources in the model.