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With the rapid growth in population and economic development, emissions of greenhouse gases (GHGs) from the Indian subcontinent have sharply increased during recent decades. However, evaluation of regional fluxes of GHGs and characterization of their spatial and temporal variations by atmospheric inversions remain uncertain due to a sparse regional atmospheric observation network. As a result of an Indo-French collaboration, three new atmospheric stations were established in India at Hanle (HLE), Pondicherry (PON) and Port Blair (PBL), with the objective of monitoring the atmospheric concentrations of GHGs and other trace gases. Here we present the results of the measurements of CO<sub>2</sub>, CH<sub>4</sub>, N<sub>2</sub>O, SF<sub>6</sub>, CO, and H<sub>2</sub> from regular flask sampling at these three stations over the period 2007–2011. For each species, annual means, seasonal cycles and gradients between stations were calculated and related to variations in natural GHG fluxes, anthropogenic emissions, and monsoon circulations. Covariances between species at the synoptic scale were analyzed to investigate the likely source(s) of emissions. The flask measurements of various trace gases at the three stations have the potential to constrain the inversions of fluxes over southern and northeastern India. However, this network of ground stations needs further extension to other parts of India to better constrain the GHG budgets at regional and continental scales.
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High uncertainties affect black carbon (BC) emissions, and, despite its important impact on air pollution and climate, very few BC emissions evaluations are found in the literature. This paper presents a novel approach, based on airborne measurements across the Paris, France, plume, developed in order to evaluate BC and NO<sub><i>x</i></sub> emissions at the scale of a whole agglomeration. The methodology consists in integrating, for each transect, across the plume observed and simulated concentrations above background. This allows for several error sources (e.g., representativeness, chemistry, plume lateral dispersion) to be minimized in the model used. The procedure is applied with the CHIMERE chemistry-transport model to three inventories – the EMEP inventory and the so-called TNO and TNO-MP inventories – over the month of July 2009. Various systematic uncertainty sources both in the model (e.g., boundary layer height, vertical mixing, deposition) and in observations (e.g., BC nature) are discussed and quantified, notably through sensitivity tests. Large uncertainty values are determined in our results, which limits the usefulness of the method to rather strongly erroneous emission inventories. A statistically significant (but moderate) overestimation is obtained for the TNO BC emissions and the EMEP and TNO-MP NO<sub><i>x</i></sub> emissions, as well as for the BC / NO<sub><i>x</i></sub> emission ratio in TNO-MP. The benefit of the airborne approach is discussed through a comparison with the BC / NO<sub><i>x</i></sub> ratio at a ground site in Paris, which additionally suggests a spatially heterogeneous error in BC emissions over the agglomeration.
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To better understand the sources of nitrogenous aerosols, particularly water-soluble organic nitrogen (WSON) and water-insoluble organic nitrogen (WION), in northeastern Asia, we measured total nitrogen (TN) and water-soluble total nitrogen (WSTN) as well as nitrogen isotope ratios (δ<sup>15</sup>N) of TN (δ<sup>15</sup>N<sub>TN</sub>) and WSTN (δ<sup>15</sup>N<sub>WSTN</sub>) in the total suspended particulate (TSP) samples collected from Sapporo, northern Japan, for a 1-year period. In general, WION was more abundant (126 ± 117 ng m<sup>−3</sup>), whereas WSON was 89.7 ± 80.6 ng m<sup>−3</sup>, accounting for 14 ± 11 % and 9.2 ± 7.3 % of TN, respectively. WSON peaked in late autumn to winter (maximum 288 ng m<sup>−3</sup>) and WION peaked in mid-spring to early summer (454 ng m<sup>−3</sup>). δ<sup>15</sup>N<sub>TN</sub> (21.9 ± 4.1 ‰) and δ<sup>15</sup>N<sub>WSTN</sub> (25.8 ± 8.2 ‰) showed peaks in summer with relatively high ratios in late autumn. Based on the seasonal variations in WSON and WION together with organic tracers, fossil fuel combustion and biomass burning are found to be two major sources of WSON, whereas emissions of biological particles and secondary formation by reactions of biogenic secondary organic species (carbonyls) with NH<sub>3</sub> are suggested as an important source of WION. The seasonality of δ<sup>15</sup>N<sub>TN</sub> and δ<sup>15</sup>N<sub>WSTN</sub>, together with the comparisons to literature values, implies that chemical aging (including gas–particle partitioning) and biomass burning are the causes of the enhanced values in summer and autumn, respectively. This study demonstrates that contributions of aerosol N from fossil fuel combustion and biomass burning dominate in autumn and/or winter, whereas emission of terrestrial biological particles and secondary formation from biogenic hydrocarbons and subsequent chemical aging in the atmosphere are important in spring and/or summer in northeastern Asia.
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The quasi 2-day wave (QTDW) at 82–97 km altitude over Collm (51° N, 13° E) has been observed using a VHF meteor radar. The long-term mean amplitudes calculated using data between September 2004 and August 2014 show a strong summer maximum and a much weaker winter maximum. In summer, the meridional amplitude is slightly larger than the zonal one with about 15 m s<sup>−1</sup> at 91 km height. Phase differences are slightly greater than 90° on an average. The periods of the summer QTDW vary between 43 and 52 h during strong bursts, while in winter the periods tend to be more diffuse. On average, the summer QTDW is amplified after a maximum of zonal wind shear which is connected with the summer mesospheric jet and there is a possible correlation of the summer mean amplitudes with the background wind shear. QTDW amplitudes exhibit considerable inter-annual variability; however, a relationship between the 11-year solar cycle and the QTDW is not found.
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We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over central and eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS) Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and was most notable in June in any given year. Similar seasonal variations were observed throughout the 9-year OMI measurement period of 2005 to 2013. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from industrial activities and automobiles, and possibly from open crop residue burning (OCRB) after the winter wheat harvest. The ozone distribution presented in this study is also consistent with some model studies. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.
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The response of the Indian summer monsoon (ISM) circulation and precipitation to Middle East dust aerosols on sub-seasonal timescales is studied using observations and the Weather Research and Forecasting model coupled with online chemistry (WRF-Chem). Satellite data show that the ISM rainfall in coastal southwest India, central and northern India, and Pakistan is closely associated with the Middle East dust aerosols. The physical mechanism behind this dust–ISM rainfall connection is examined through ensemble simulations with and without dust emissions. Each ensemble includes 16 members with various physical and chemical schemes to consider the model uncertainties in parameterizing short-wave radiation, the planetary boundary layer, and aerosol chemical mixing rules. Experiments show that dust aerosols increase rainfall by about 0.44 mm day<sup>−1</sup> (~10 % of the climatology) in coastal southwest India, central and northern India, and north Pakistan, a pattern consistent with the observed relationship. The ensemble mean rainfall response over India shows a much stronger spatial correlation with the observed rainfall response than any other ensemble members. The largest modeling uncertainties are from the boundary layer schemes, followed by short-wave radiation schemes. In WRF-Chem, the dust aerosol optical depth (AOD) over the Middle East shows the strongest correlation with the ISM rainfall response when dust AOD leads rainfall response by about 11 days. Further analyses show that increased ISM rainfall is related to enhanced southwesterly monsoon flow and moisture transport from the Arabian Sea to the Indian subcontinent, which are associated with the development of an anomalous low-pressure system over the Arabian Sea, the southern Arabian Peninsula, and the Iranian Plateau due to dust-induced heating in the troposphere. The dust-induced heating in the mid-upper troposphere is mainly located in the Iranian Plateau rather than the Tibetan Plateau. This study demonstrates a thermodynamic mechanism that links remote desert dust emissions in the Middle East to ISM circulation and precipitation variability on sub-seasonal timescales, which may have implications for ISM rainfall forecasts.
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A merged time series of stratospheric water vapour built from the Halogen Occultation Instrument (HALOE) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) data between 60° S and 60° N and 15 to 30 km and covering the years 1992 to 2012 was analysed by multivariate linear regression, including an 11-year solar cycle proxy. Lower stratospheric water vapour was found to reveal a phase-shifted anti-correlation with the solar cycle, with lowest water vapour after solar maximum. The phase shift is composed of an inherent constant time lag of about 2 years and a second component following the stratospheric age of air. The amplitudes of the water vapour response are largest close to the tropical tropopause (up to 0.35 ppmv) and decrease with altitude and latitude. Including the solar cycle proxy in the regression results in linear trends of water vapour being negative over the full altitude/latitude range, while without the solar proxy, positive water vapour trends in the lower stratosphere were found. We conclude from these results that a solar signal seems to be generated at the tropical tropopause which is most likely imprinted on the stratospheric water vapour abundances and transported to higher altitudes and latitudes via the Brewer–Dobson circulation. Hence it is concluded that the tropical tropopause temperature at the final dehydration point of air may also be governed to some degree by the solar cycle. The negative water vapour trends obtained when considering the solar cycle impact on water vapour abundances can possibly solve the "water vapour conundrum" of increasing stratospheric water vapour abundances despite constant or even decreasing tropopause temperatures.
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Chemical composition data obtained from the Microwave Limb Sounder (MLS) and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instruments onboard EOS-Aura and ENVISAT satellites are used to investigate the variation of ozone (O<sub>3</sub>), water vapor (H<sub>2</sub>O) and methane (CH<sub>4</sub>) volume mixing ratios (VMRs) in the height range 20–60 km over the equatorial region during the sudden stratospheric warmings (SSWs) of 2004, 2009 and 2012, the occurrence of which are identified using the ERA (European Center for Medium Range Weather Forecasting Reanalysis) Interim temperature and zonal wind data sets. It is found that the O<sub>3</sub> VMR shows increment whereas H<sub>2</sub>O VMR shows decrement during the SSW event and the possible reasons for these changes in the VMRs are investigated. In the upper stratosphere, the source of water vapor is oxidation of CH<sub>4</sub> which takes place either by hydroxyl (OH) or by atomic oxygen (O). However, the OH VMR available for the year 2009 SSW event does not show any significant variation. The decrease of zonal mean MLS temperature over the equator during the SSW suggests that the rate of the reaction of ozone production (O + O<sub>2</sub> ⟶ O</sub>3</sub> + M), which increases with decreasing temperature, shifts the O/O<sub>3</sub> ratio towards O<sub>3</sub>, resulting in the decrease of CH<sub>4</sub> oxidation and consequent decrease in water vapor.
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The ergodic hypothesis is a basic hypothesis typically invoked in atmospheric surface layer (ASL) experiments. The ergodic theorem of stationary random processes is introduced to analyse and verify the ergodicity of atmospheric turbulence measured using the eddy-covariance technique with two sets of field observational data. The results show that the ergodicity of atmospheric turbulence in atmospheric boundary layer (ABL) is relative not only to the atmospheric stratification but also to the eddy scale of atmospheric turbulence. The eddies of atmospheric turbulence, of which the scale is smaller than the scale of the ABL (i.e. the spatial scale is less than 1000 m and temporal scale is shorter than 10 min), effectively satisfy the ergodic theorems. Under these restrictions, a finite time average can be used as a substitute for the ensemble average of atmospheric turbulence, whereas eddies that are larger than ABL scale dissatisfy the mean ergodic theorem. Consequently, when a finite time average is used to substitute for the ensemble average, the eddy-covariance technique incurs large errors due to the loss of low-frequency information associated with larger eddies. A multi-station observation is compared with a single-station observation, and then the scope that satisfies the ergodic theorem is extended from scales smaller than the ABL, approximately 1000 m to scales greater than about 2000 m. Therefore, substituting the finite time average for the ensemble average of atmospheric turbulence is more faithfully approximate the actual values. Regardless of vertical velocity or temperature, the variance of eddies at different scales follows Monin–Obukhov similarity theory (MOST) better if the ergodic theorem can be satisfied; if not it deviates from MOST. The exploration of ergodicity in atmospheric turbulence is doubtlessly helpful in understanding the issues in atmospheric turbulent observations and provides a theoretical basis for overcoming related difficulties.
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This study explores our ability to simulate the atmospheric chemistry stemming from isoprene emissions in pristine and polluted regions of the Amazon basin. We confront two atmospheric chemistry models – a global, Eulerian chemistry-climate model (UM-UKCA) and a trajectory-based Lagrangian model (CiTTyCAT) – with recent airborne measurements of atmospheric composition above the Amazon made during the SAMBBA campaign of 2012. The simulations with the two models prove relatively insensitive to the chemical mechanism employed; we explore one based on the Mainz Isoprene Mechanism, and an updated one that includes changes to the chemistry of first generation isoprene nitrates (ISON) and the regeneration of hydroxyl radicals via the formation of hydroperoxy-aldehydes (HPALDS) from hydroperoxy radicals (ISO<sub>2</sub>). In the Lagrangian model, the impact of increasing the spatial resolution of trace gas emissions employed from 3.75° × 2.5° to 0.1° × 0.1° varies from one flight to another, and from one chemical species to another. What consistently proves highly influential on our simulations, however, is the model framework itself – how the treatment of transport, and consequently mixing, differs between the two models. The lack of explicit mixing in the Lagrangian model yields variability in atmospheric composition more reminiscent of that exhibited by the measurements. In contrast, the combination of explicit (and implicit) mixing in the Eulerian model removes much of this variability but yields better agreement with the measurements overall. We therefore explore a simple treatment of mixing in the Lagrangian model that, drawing on output from the Eulerian model, offers a compromise between the two models. We use this Lagrangian/Eulerian combination, in addition to the separate Eulerian and Lagrangian models, to simulate ozone at a site in the boundary layer downwind of Manaus, Brazil. The Lagrangian/Eulerian combination predicts a value for an AOT40-like accumulated exposure metric of around 1000 ppbv h, compared to just 20 ppbv h with the Eulerian model. The model framework therefore has considerable bearing on our understanding of the frequency at which, and the duration for which, the rainforest is exposed to damaging ground-level ozone concentrations.
