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Representation of the tropical stratospheric zonal wind in global atmospheric reanalyses

This paper reports on a project to compare the representation of the monthly-mean zonal wind in the equatorial stratosphere among major global atmospheric reanalysis data sets. The degree of disagreement among the reanalyses is characterized by the standard deviation (SD) of the monthly-mean zonal wind and this depends on latitude, longitude, height, and the phase of the quasi-biennial oscillation (QBO). At each height the SD displays a prominent equatorial maximum, indicating the particularly challenging nature of the reanalysis problem in the low-latitude stratosphere. At 50–70 hPa the geographical distributions of SD are closely related to the density of radiosonde observations. The largest SD values are over the central Pacific, where few in situ observations are available. At 10–20 hPa the spread among the reanalyses and differences with in situ observations both depend significantly on the QBO phase. Notably the easterly-to-westerly phase transitions in all the reanalyses except MERRA are delayed relative to those directly observed in Singapore. In addition, the timing of the easterly-to-westerly phase transitions displays considerable variability among the different reanalyses and this spread is much larger than for the timing of the westerly-to-easterly phase changes. The eddy component in the monthly-mean zonal wind near the Equator is dominated by zonal wavenumber 1 and 2 quasi-stationary planetary waves propagating from midlatitudes in the westerly phase of the QBO. There generally is considerable disagreement among the reanalyses in the details of the quasi-stationary waves near the Equator. At each level, there is a tendency for the agreement to be best near the longitude of Singapore, suggesting that the Singapore observations act as a strong constraint on all the reanalyses. Our measures of the quality of the reanalysis clearly show systematic improvement over the period considered (1979–2012). The SD among the reanalysis declines significantly over the record, although the geographical pattern of SD remains nearly constant.
Summertime nitrate aerosol in the upper troposphere and lower stratosphere over the Tibetan Plateau and the South Asian summer monsoon region

We use the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to examine the contribution of nitrate aerosol to aerosol concentrations in the upper troposphere and lower stratosphere (UTLS) over the Tibetan Plateau and the South Asian summer monsoon (TP/SASM) region during summertime of year 2005. Simulated surface-layer aerosol concentrations are compared with ground-based observations, and simulated aerosols in the UTLS are evaluated by using the Stratospheric Aerosol and Gas Experiment II satellite data. Simulations show elevated aerosol concentrations of sulfate, nitrate, ammonium, black carbon, organic carbon, and PM2.5 (particles with diameter equal to or less than 2.5 µm, defined as the sum of sulfate, nitrate, ammonium, black carbon, and organic carbon aerosols in this study) in the UTLS over the TP/SASM region throughout the summer. Nitrate aerosol is simulated to be of secondary importance near the surface but the most dominant aerosol species in the UTLS over the studied region. Averaged over summertime and over the TP/SASM region, CNIT (the ratio of nitrate concentration to PM2.5 concentration) values are 5–35 % at the surface, 25–50 % at 200 hPa, and could exceed 60 % at 100 hPa. The mechanisms for the accumulation of nitrate in the UTLS over the TP/SASM region include vertical transport and the gas-to-aerosol conversion of HNO3 to form nitrate. The high relative humidity and low temperature associated with the deep convection over the TP/SASM region are favorable for the gas-to-aerosol conversion of HNO3.
Dimethyl sulfide in the summertime Arctic atmosphere: measurements and source sensitivity simulations

Dimethyl sulfide (DMS) plays a major role in the global sulfur cycle. In addition, its atmospheric oxidation products contribute to the formation and growth of atmospheric aerosol particles, thereby influencing cloud condensation nuclei (CCN) populations and thus cloud formation. The pristine summertime Arctic atmosphere is strongly influenced by DMS. However, atmospheric DMS mixing ratios have only rarely been measured in the summertime Arctic. During July–August, 2014, we conducted the first high time resolution (10 Hz) DMS mixing ratio measurements for the eastern Canadian Archipelago and Baffin Bay as one component of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments (NETCARE). DMS mixing ratios ranged from below the detection limit of 4 to 1155 pptv (median 186 pptv) during the 21-day shipboard campaign. A transfer velocity parameterization from the literature coupled with coincident atmospheric and seawater DMS measurements yielded air–sea DMS flux estimates ranging from 0.02 to 12 µmol m−2 d−1. Air-mass trajectory analysis using FLEXPART-WRF and sensitivity simulations with the GEOS-Chem chemical transport model indicated that local sources (Lancaster Sound and Baffin Bay) were the dominant contributors to the DMS measured along the 21-day ship track, with episodic transport from the Hudson Bay System. After adjusting GEOS-Chem oceanic DMS values in the region to match measurements, GEOS-Chem reproduced the major features of the measured time series but was biased low overall (2–1006 pptv, median 72 pptv), although within the range of uncertainty of the seawater DMS source. However, during some 1–2 day periods the model underpredicted the measurements by more than an order of magnitude. Sensitivity tests indicated that non-marine sources (lakes, biomass burning, melt ponds, and coastal tundra) could make additional episodic contributions to atmospheric DMS in the study region, although local marine sources of DMS dominated. Our results highlight the need for both atmospheric and seawater DMS data sets with greater spatial and temporal resolution, combined with further investigation of non-marine DMS sources for the Arctic.
The aerosol radiative effects of uncontrolled combustion of domestic waste

Open, uncontrolled combustion of domestic waste is a potentially significant source of aerosol; however, this aerosol source is not generally included in many global emissions inventories. To provide a first estimate of the aerosol radiative impacts from domestic-waste combustion, we incorporate the Wiedinmyer et al. (2014) emissions inventory into GEOS-Chem-TOMAS, a global chemical-transport model with online aerosol microphysics. We find domestic-waste combustion increases global-mean black carbon and organic aerosol concentrations by 8 and 6 %, respectively, and by greater than 40 % in some regions. Due to uncertainties regarding aerosol optical properties, we estimate the globally averaged aerosol direct radiative effect to range from −5 to −20 mW m−2; however, this range increases from −40 to +4 mW m−2 when we consider uncertainties in emission mass and size distribution. In some regions with significant waste combustion, such as India and China, the aerosol direct radiative effect may exceed −0.4 W m−2. Similarly, we estimate a cloud-albedo aerosol indirect effect of −13 mW m−2, with a range of −4 to −49 mW m−2 due to emission uncertainties. In the regions with significant waste combustion, the cloud-albedo aerosol indirect effect may exceed −0.4 W m−2.
Measurements of global distributions of polar mesospheric clouds during 2005–2012 by MIPAS/Envisat

We have analysed MIPAS (Michelson Interferometer for Passive Atmopheric Sounding) infrared measurements of PMCs for the summer seasons in the Northern (NH) and Southern (SH) hemispheres from 2005 to 2012. Measurements of PMCs using this technique are very useful because they are sensitive to the total ice volume and independent of particle size. For the first time, MIPAS has provided coverage of the PMC total ice volume from midlatitudes to the poles. MIPAS measurements indicate the existence of a continuous layer of mesospheric ice, extending from about ∼ 81 km up to about 88–89 km on average and from the poles to about 50–60° in each hemisphere, increasing in concentration with proximity to the poles. We have found that the ice concentration is larger in the Northern Hemisphere than in the Southern Hemisphere. The ratio between the ice water content (IWC) in both hemispheres is also latitude-dependent, varying from a NH ∕ SH ratio of 1.4 close to the poles to a factor of 2.1 around 60°. This also implies that PMCs extend to lower latitudes in the NH. A very clear feature of the MIPAS observations is that PMCs tend to be at higher altitudes with increasing distance from the polar region (in both hemispheres), particularly equatorwards of 70°, and that they are about 1 km higher in the SH than in the NH. The difference between the mean altitude of the PMC layer and the mesopause altitude increases towards the poles and is larger in the NH than in the SH. The PMC layers are denser and wider when the frost-point temperature occurs at lower altitudes. The layered water vapour structure caused by sequestration and sublimation of PMCs is present at latitudes northwards of 70° N and more pronounced towards the pole. Finally, MIPAS observations have also shown a clear impact of the migrating diurnal tide on the diurnal variation of the PMC volume ice density.
Impact of Siberian forest fires on the atmosphere over the Korean Peninsula during summer 2014

Extensive forest fires occurred during late July 2014 across the forested region of Siberia, Russia. Smoke plumes emitted from Siberian forest fires underwent long-range transport over Mongolia and northeast China to the Korean Peninsula, which is located ∼  3000 km south of the Siberian forest. A notably high aerosol optical depth of ∼  4 was observed at a wavelength of 500 nm near the source of the Siberian forest fires. Smoke plumes reached 3–5 km in height near the source and fell below 2 km over the Korean Peninsula. Elevated concentrations of levoglucosan were observed (119.7 ± 6.0 ng m−3), which were ∼  4.5 times higher than those observed during non-event periods in July 2014. During the middle of July 2014, a haze episode occurred that was primarily caused by the long-range transport of emission plumes originating from urban and industrial complexes in East China. Sharp increases in SO42− concentrations (23.1 ± 2.1 µg m−3) were observed during this episode. The haze caused by the long-range transport of Siberian forest fire emissions was clearly identified by relatively high organic carbon (OC) ∕ elemental carbon (EC) ratios (7.18 ± 0.2) and OC ∕ SO42− ratios (1.31 ± 0.07) compared with those of the Chinese haze episode (OC ∕ EC ratio: 2.4 ± 0.4; OC ∕ SO42− ratio: 0.21 ± 0.05). Remote measurement techniques and chemical analyses of the haze plumes clearly show that the haze episode that occurred during late July 2014 was caused mainly by the long-range transport of smoke plumes emitted from Siberian forest fires.
Analysis of the potential of near-ground measurements of CO2 and CH4 in London, UK, for the monitoring of city-scale emissions using an atmospheric transport model

Carbon dioxide (CO2) and methane (CH4) mole fractions were measured at four near-ground sites located in and around London during the summer of 2012 with a view to investigating the potential of assimilating such measurements in an atmospheric inversion system for the monitoring of the CO2 and CH4 emissions in the London area. These data were analysed and compared with simulations using a modelling framework suited to building an inversion system: a 2 km horizontal resolution south of England configuration of the transport model CHIMERE driven by European Centre for Medium-Range Weather Forecasts (ECMWF) meteorological forcing, coupled to a 1 km horizontal resolution emission inventory (the UK National Atmospheric Emission Inventory). First comparisons reveal that local sources, which cannot be represented in the model at a 2 km resolution, have a large impact on measurements. We evaluate methods to filter out the impact of some of the other critical sources of discrepancies between the measurements and the model simulation except that of the errors in the emission inventory, which we attempt to isolate. Such a separation of the impact of errors in the emission inventory should make it easier to identify the corrections that should be applied to the inventory. Analysis is supported by observations from meteorological sites around the city and a 3-week period of atmospheric mixing layer height estimations from lidar measurements. The difficulties of modelling the mixing layer depth and thus CO2 and CH4 concentrations during the night, morning and late afternoon lead to focusing on the afternoon period for all further analyses. The discrepancies between observations and model simulations are high for both CO2 and CH4 (i.e. their root mean square (RMS) is between 8 and 12 parts per million (ppm) for CO2 and between 30 and 55 parts per billion (ppb) for CH4 at a given site). By analysing the gradients between the urban sites and a suburban or rural reference site, we are able to decrease the impact of uncertainties in the fluxes and transport outside the London area and in the model domain boundary conditions. We are thus able to better focus attention on the signature of London urban CO2 and CH4 emissions in the atmospheric CO2 and CH4 concentrations. This considerably improves the statistical agreement between the model and observations for CO2 (with model–data RMS discrepancies that are between 3 and 7 ppm) and to a lesser degree for CH4 (with model–data RMS discrepancies that are between 29 and 38 ppb). Between one of the urban sites and either the rural or suburban reference site, selecting the gradients during periods wherein the reference site is upwind of the urban site further decreases the statistics of the discrepancies in general, though not systematically. In a further attempt to focus on the signature of the city anthropogenic emission in the mole fraction measurements, we use a theoretical ratio of gradients of carbon monoxide (CO) to gradients of CO2 from fossil fuel emissions in the London area to diagnose observation-based fossil fuel CO2 gradients, and compare them with the fossil fuel CO2 gradients simulated with CHIMERE. This estimate increases the consistency between the model and the measurements when considering only one of the two urban sites, even though the two sites are relatively close to each other within the city. While this study evaluates and highlights the merit of different approaches for increasing the consistency between the mesoscale model and the near-ground data, and while it manages to decrease the random component of the analysed model–data discrepancies to an extent that should not be prohibitive to extracting the signal from the London urban emissions, large biases, the sign of which depends on the measurement sites, remain in the final model–data discrepancies. Such biases are likely related to local emissions to which the urban near-ground sites are highly sensitive. This questions our current ability to exploit urban near-ground data for the atmospheric inversion of city emissions based on models at spatial resolution coarser than 2 km. Several measurement and modelling concepts are discussed to overcome this challenge.
Substantial secondary organic aerosol formation in a coniferous forest: observations of both day- and nighttime chemistry

Substantial biogenic secondary organic aerosol (BSOA) formation was investigated in a coniferous forest mountain region in Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment with limited influence from anthropogenic emissions. Positive matrix factorization of aerosol mass spectrometry (AMS) measurement identified two types of BSOA (BSOA-1 and BSOA-2), which were primarily generated by gas-phase oxidation of monoterpenes and perhaps sesquiterpenes. The temporal variations of BSOA-1 and BSOA-2 can be explained by gas–particle partitioning in response to ambient temperature and the relative importance of different oxidation mechanisms between day and night. While BSOA-1 arises from gas-phase ozonolysis and nitrate radical chemistry at night, BSOA-2 is likely less volatile than BSOA-1 and consists of products formed via gas-phase oxidation by OH radical and ozone during the day. Organic nitrates produced through nitrate radical chemistry can account for 22–33 % of BSOA-1 mass at night. The mass spectra of BSOA-1 and BSOA-2 have higher values of the mass fraction of m/z 91 (f91) compared to the background organic aerosol. Using f91 to evaluate BSOA formation pathways in this unpolluted, forested region, heterogeneous oxidation of BSOA-1 is a minor production pathway of BSOA-2.
Near-surface and columnar measurements with a micro pulse lidar of atmospheric pollen in Barcelona, Spain

We present for the first time continuous hourly measurements of pollen near-surface concentration and lidar-derived profiles of particle backscatter coefficients and of volume and particle depolarization ratios during a 5-day pollination event observed in Barcelona, Spain, between 27 and 31 March 2015. Daily average concentrations ranged from 1082 to 2830 pollen m−3. Platanus and Pinus pollen types represented together more than 80 % of the total pollen. Maximum hourly pollen concentrations of 4700 and 1200 m−3 were found for Platanus and Pinus, respectively. Every day a clear diurnal cycle caused by the vertical transport of the airborne pollen was visible on the lidar-derived profiles with maxima usually reached between 12:00 and 15:00 UT. A method based on the lidar polarization capabilities was used to retrieve the contribution of the pollen to the total aerosol optical depth (AOD). On average the diurnal (09:00–17:00 UT) pollen AOD was 0.05, which represented 29 % of the total AOD. Maximum values of the pollen AOD and its contribution to the total AOD reached 0.12 and 78 %, respectively. The diurnal means of the volume and particle depolarization ratios in the pollen plume were 0.08 and 0.14, with hourly maxima of 0.18 and 0.33, respectively. The diurnal mean of the height of the pollen plume was found at 1.24 km with maxima varying in the range of 1.47–1.78 km. A correlation study is performed (1) between the depolarization ratios and the pollen near-surface concentration to evaluate the ability of the former parameter to monitor pollen release and (2) between the depolarization ratios as well as pollen AOD and surface downward solar fluxes, which cause the atmospheric turbulences responsible for the particle vertical motion, to examine the dependency of the depolarization ratios and the pollen AOD upon solar fluxes. For the volume depolarization ratio the first correlation study yields to correlation coefficients ranging 0.00–0.81 and the second to correlation coefficients ranging 0.49–0.86.
Spatial distribution of the persistent organic pollutants across the Tibetan Plateau and its linkage with the climate systems: a 5-year air monitoring study

The Tibetan Plateau (TP) has been contaminated by persistent organic pollutants (POPs), including legacy organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) through atmospheric transport. The exact source regions, transport pathways and time trends of POPs to the TP are not well understood. Here polystyrene–divinylbenzene copolymer resin (XAD)-based passive air samplers (PASs) were deployed at 16 Tibetan background sites from 2007 to 2012 to gain further insight into spatial patterns and temporal trends of OCPs and PCBs. The southeastern TP was characterized by dichlorodiphenyltrichloroethane (DDT)-related chemicals delivered by Indian monsoon air masses. The northern and northwestern TP displayed the greatest absolute concentration and relative abundance of hexachlorobenzene (HCB) in the atmosphere, caused by the westerly-driven European air masses. The interactions between the DDT polluted Indian monsoon air and the clean westerly winds formed a transition zone in central Tibet, where both DDT and HCB were the dominant chemicals. Based on 5 years of continuous sampling, our data indicated declining concentrations of HCB and hexachlorocyclohexanes (HCHs) across the Tibetan region. Inter-annual trends of DDT class chemicals, however, showed less variation during this 5-year sampling period, which may be due to the ongoing usage of DDT in India. This paper demonstrates the possibility of using POP fingerprints to investigate the climate interactions and the validity of using PAS to derive inter-annual atmospheric POP time trends.