CO2 Mixing Ratios Research Articles

Simulation of the Air Quality in Southern California, USA in July and October of the Year 2018

A numerical investigation of the air quality in Southern California, USA in the year 2018 is presented using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). In July, a heat wave occurred, and in October, Santa Ana conditions prevailed; these conditions and their impact on air quality are the scope of the present numerical study.The high spatial resolution in the simulation includes two nested domains of 1 km and 3 km, respectively. Local climate zones land use categories are combined with the complex urban model building effect parameterization coupled with the building energy model (BEP+BEM) and the detailed MOZCART-T1 chemical reaction mechanism, which is the MOZART-T1 mechanism for trace gases with GOCART aerosols. Thus, the model is suitable to compare simulation results to in situ and satellite measurements of O3, NO2, CH4, and CO. The meteorology is captured well by the model. Comparison of simulation results with observations shows a good agreement of NO2 and ozone, whereas CO mixing ratios are generally underestimated. This hints at missing emissions in the 2017 National Emissions Inventory (NEI) dataset. Both the heat wave and the Santa Ana winds increase the air pollution with gas-phase species in Los Angeles. In both cases, nighttime boundary layer heights are small, which causes emissions to reside near the ground. During Santa Ana winds, NOx removal on aerosols is reduced. Methane mixing ratios are modeled very well at most stations in Los Angeles, but predictions of low emissions near the University of California cause inaccuracies at that location. Modeled and observed PM2.5 agree well on low-pollution days, but high-pollution events are generally missed by the model. During the heat wave, both modeled and observed PM2.5 concentrations exceed the recommended NAAQS National Ambient Air Quality Standards value of 12.5 g/m3. The present modeling approach serves as a base for the study and prediction of special weather events and their impact on air pollution.

Surface ozone in southeast Tibet: variations and implications of tropospheric ozone sink over a highland

Environment context One-year-long on-line measurements of surface O3 and CO mixing ratios were performed on the southeast Tibetan Plateau to examine O3 behaviour. During the daytime, the O3 mixing ratio was strongly affected by vertical air exchange. The O3 mixing ratio was high in the afternoon and decreased at night, indicating a sink of tropospheric O3. The upper limit of the tropospheric O3 sink averaged from 4.5 to 5.5 ppb h−1. Rationale Ozone (O3) behaviour over the Tibetan Plateau has attracted attention in recent decades. However, few long-term measurements have been performed in the region. Methodology Field observations were conducted at a mountain site on the southeastern Tibetan Plateau from June 2014 to July 2015 in order to understand the behaviour of surface O3 and its influencing factors. Backward trajectory cluster analysis was applied to understand long-range transport sources and their relative contributions. Results The monthly average O3 ranged from 22.1 to 48.6 ppb with a common high spring ozone concentration phenomenon. The O3 diurnal variation exhibited a similar pattern to those in polluted areas but the cause was different. The O3 mixing ratio was significantly positively correlated with mixed-layer depth and wind speed, and negatively with temperature and relative humidity, indicating strong vertical air exchange. Approximately 50% of air mass trajectories originated from the northeastern Bengal Bay region, with fairly low O3 (CO) mixing ratios and high humidity. Others originated from the north Indian subcontinent (28%) and the Middle East (18%), with fairly high O3 (and CO) and low humidity. Discussion The average relative contributions of different air masses to surface O3 and CO were small and scattered but large for trajectories arriving at 14:00 hours when vertical air exchange was close to its strongest for the day. The tropospheric O3 sink may be common in the highlands, indicating a negative greenhouse effect there. The O3 sink at Linzhi was estimated in the range of 4.5–5.5 ppb h−1 at maximum.

Evolving CO2 Rather Than SST Leads to a Factor of Ten Decrease in GCM Convergence Time.

The high computational cost of Global Climate Models (GCMs) is a problem that limits their use in many areas. Recently an inverse climate modeling (InvCM) method, which fixes the global mean sea surface temperature (SST) and evolves the CO2 mixing ratio to equilibrate climate, has been implemented in a cloud‐resolving model. In this article, we apply InvCM to ExoCAM GCM aquaplanet simulations, allowing the SST pattern to evolve while maintaining a fixed global‐mean SST. We find that InvCM produces the same climate as normal slab‐ocean simulations but converges an order of magnitude faster. We then use InvCM to calculate the equilibrium CO2 for SSTs ranging from 290 to 340 K at 1 K intervals and reproduce the large increase in climate sensitivity at an SST of about 315 K at much higher temperature resolution. The speedup provided by InvCM could be used to equilibrate GCMs at higher spatial resolution or to perform broader parameter space exploration in order to gain new insight into the climate system. Additionally, InvCM could be used to find unstable and hidden climate states, and to find climate states close to bifurcations such as the runaway greenhouse transition.

Analysis of atmospheric greenhouse gases in north Xinjiang

Flask air samples were collected weekly at the Akedala (AKD) regional atmosphere station in north Xinjiang, China, and atmospheric carbon dioxide (CO2) and methane (CH4) mole fractions were measured using cavity-ring down spectroscopy. AKD station is under a typical temperate continental semiarid and arid monsoon climate with westerly air flow. This paper presents the long-term trends and seasonal variations in atmospheric CO2 and CH4 concentrations for the first time and discusses the possible influencing mechanisms. The CO2 and CH4 background mixing ratios were 412.1 ± 0.36 ppm and 1968.9 ± 0.95 ppb, respectively, in 2018. The growth rates were 2.62 ppm y−1 and 9.67 ppb y−1 for CO2 and CH4, respectively, during 2010–2018, which were higher than the surface measurements at Waliguan Baseline Observatory at similar latitudes. The averaged CO2 seasonal cycle showed a minimum in summer and a maximum in winter, and the annual amplitude was high at 18.7 ppm. The CH4 seasonal cycle showed a rapid recovery in summer during July and August. Back-trajectory analysis showed that the atmospheric information at AKD station can provide some implications for uptake from Kazakhstan and Russia, as well as information about natural and anthropogenic emissions in northern Xinjiang. This study revealed that the long-term upward trend of the CO2 concentration in AKD might be attributed to emissions from energy consumption of heavy industry. The comprehensive effects of livestock, geological micro seepage and oil and gas production, and vertical transport also enhanced the atmospheric CH4 concentrations. The results of this study may improve our basic understanding of observed atmospheric CO2 and CH4 in China and Central Asia and the underlying fluxes to be used in atmospheric inversion models.

Nitrous acid production and uptake by Zea mays plants in growth chambers in the presence of nitrogen dioxide

Nitrous acid (HONO) photolysis is an important atmospheric reaction that leads to the formation of hydroxyl radicals (OH), the main diurnal atmospheric oxidants. The process of HONO formation remains unclear, and comparisons between field measurements and model results have highlighted the presence of unknown HONO sources. HONO production on plant surfaces was recently suggested to contribute to atmospheric HONO formation, but there is limited information on the quantification of HONO production and uptake by plants. To address this gap in the existing knowledge, the current study investigated HONO exchange on living Zea mays plants. Experiments were conducted in growth chambers under controlled experimental conditions (temperature, relative humidity, NO2 mixing ratio, light intensity, CO2 mixing ratio) at temperatures ranging between 283 and 299 K. To investigate the effect of drought on HONO plant-atmosphere exchanges, experiments were carried out on two sets of Zea mays plants exposed to two different water supply conditions during their growth: optimal watering (70% of the field capacity) and water stress (30% of the field capacity). Results indicated that the uptake of HONO by control Zea mays plants increased linearly with ambient temperature, and was correlated with CO2 assimilation for temperatures ranging from 283 to 299 K. At 299 K, HONO production on the leaves offset this uptake and Zea mays plants were a source of HONO, with a net production rate of 27 ± 7 ppt h-1. Deposition velocities were higher for HONO than CO2, suggesting a higher mesophyll resistance for CO2 than HONO. As water stress reduced the stomatal opening, it also decreased plant-atmosphere gas exchange. Thus, climate change, which may limit the availability of water, will have an impact on HONO exchange between plants and the atmosphere.

Quasi-two-day wave modulation of carbon dioxide in the mesosphere and lower thermosphere

In this paper, we report the quasi-two-day wave (QTDW) in daytime only SABER CO2 in January 2003. The QTDW in CO2 of ∼7 ppmv or 3–4% shows double peak structures at mid and low latitudes of both hemispheres. We compare the SABER measured QTDW disturbance in CO2 and temperature to those in the eCMAM (the extended Canadian Middle Atmosphere Model). Good agreement of QTDW CO2 spatial and temporal variations is seen, especially at southern mid-latitudes. eCMAM outputs are further analyzed to show that the QTDW in CO2 mixing ratio is mainly driven by both vertical transport and meridional advection. Because waves in vertical transport can be derived by temperature disturbance via a so-called adiabatic displacement approach, we can estimate the QTDW in CO2 mixing ratio from the SABER QTDW in temperature assuming meridional advection is weak at low and mid-latitudes.

Shipborne measurements of methane and carbon dioxide in the Middle East and Mediterranean areas and the contribution from oil and gas emissions

Abstract. The increase of atmospheric methane (CH4) and carbon dioxide (CO2), two of the main anthropogenic greenhouse gases, is largely driven by fossil sources. Sources and sinks remain insufficiently characterized in the Mediterranean and Middle East areas, where very few in situ measurements are available. We measured the atmospheric mixing ratios of CH4 and CO2 by ship in the region in July and August 2017. High mixing ratios were observed over the Suez Canal, Red Sea and Arabian Gulf, while generally lower mixing ratios were observed over the Gulf of Aden and Gulf of Oman. We probe the origin of the CO2 and CH4 excess mixing ratio by using correlations with light alkanes and through the use of a Lagrangian model coupled to two different emission inventories of anthropogenic sources. We find that the CO2 and especially the CH4 enhancements are mainly linked to nearby oil and gas (OG) activities over the Arabian Gulf and a mixture of other sources over the Red Sea. The isomeric ratio of pentane is shown to be a useful indicator of the OG component of atmospheric CH4 at the regional level. Upstream emissions linked to oil in the northern Arabian Gulf seem to be underestimated, while gas-related emissions in the southern Gulf are overestimated in our simulations. Our results highlight the need for improvement of inventories in the area to better characterize the changes in magnitude and the complex distribution of the OG sources in the Middle East.

Australian Fires 2019–2020: Tropospheric and Stratospheric Pollution Throughout the Whole Fire Season

The historically large and severe wildfires in Australia from September 2019 to March 2020 are known to have injected a smoke plume into the stratosphere around New Year, due to pyro-cumulonimbus (pyro-Cb) activity, that was subsequently distributed throughout the Southern Hemisphere (SH). We show with satellite, ground based remote sensing, and in situ observations that the fires before New Year, had already a substantial impact on the SH atmosphere, starting as early as September 2019, with subsequent long-range transport of trace gas plumes in the upper-troposphere. Airborne in situ measurements above Southern Argentina in November 2019 show elevated CO mixing ratios at an altitude of 11 km and can be traced back using FLEXPART trajectories to the Australian fires in mid-November 2019. Ground based solar-FTS (Fourier Transform Spectroscopy) observations of biomass burning tracers CO, HCN and C2H6 at Lauder, South Island, New Zealand show enhanced tropospheric columns already starting in September 2019. In MLS observations averaged over 30°–60°S, enhanced CO mixing ratios compared to previous years become visible in late October 2019 only at and below the 147 hPa pressure level. Peak differences are found with satellite and ground-based observations for all altitude levels in the Southern Hemisphere in January. With still increased aerosol values following the Ulawun eruption in 2019, averaged satellite observations show no clear stratospheric and upper-tropospheric aerosol enhancements from the Australian fires, before the pyro-Cb events at the end of December 2019. However, with the clear enhancement of fire tracers, we suggest the period September to December 2019 (prior to the major pyro-Cb events) should be taken into account in terms of fire pollutant emissions when studying the impact of the Australian fires on the SH atmosphere.

Anthropogenic and natural controls on atmospheric <i>δ</i><sup>13</sup>C-CO<sub>2</sub> variations in the Yangtze River delta: insights from a carbon isotope modeling framework

Abstract. The atmospheric carbon dioxide (CO2) mixing ratio and its carbon isotope (δ13C-CO2) composition contain important CO2 sink and source information spanning from ecosystem to global scales. The observation and simulation for both CO2 and δ13C-CO2 can be used to constrain regional emissions and better understand the anthropogenic and natural mechanisms that control δ13C-CO2 variations. Such work remains rare for urban environments, especially megacities. Here, we used near-continuous CO2 and δ13C-CO2 measurements, from September 2013 to August 2015, and inverse modeling to constrain the CO2 budget and investigate the main factors that dominated δ13C-CO2 variations for the Yangtze River delta (YRD) region, one of the largest anthropogenic CO2 hotspots and densely populated regions in China. We used the WRF-STILT model framework with category-specified EDGAR v4.3.2 CO2 inventories to simulate hourly CO2 mixing ratios and δ13C-CO2, evaluated these simulations with observations, and constrained the total anthropogenic CO2 emission. We show that (1) top-down and bottom-up estimates of anthropogenic CO2 emissions agreed well (bias < 6 %) on an annual basis, (2) the WRF-STILT model can generally reproduce the observed diel and seasonal atmospheric δ13C-CO2 variations, and (3) anthropogenic CO2 emissions played a much larger role than ecosystems in controlling the δ13C-CO2 seasonality. When excluding ecosystem respiration and photosynthetic discrimination in the YRD area, δ13C-CO2 seasonality increased from 1.53 ‰ to 1.66 ‰. (4) Atmospheric transport processes in summer amplified the cement CO2 enhancement proportions in the YRD area, which dominated monthly δs (the mixture of δ13C-CO2 from all regional end-members) variations. These findings show that the combination of long-term atmospheric carbon isotope observations and inverse modeling can provide a powerful constraint on the carbon cycle of these complex megacities.

Potential Source Regions and Transportation Pathways of Reactive Gases at a Regional Background Site in Northwestern China

Reactive gases (O3, CO, NO2, and SO2) were collected hourly at the Akedala regional background station in northwestern China during September 2017 to August 2018. Wind rose, cluster analysis, potential source contribution function (PSCF), and concentration-weighted trajectory (CWT) methods were adopted for identifying the transport pathways and potential source regions of these atmosphere components at Akedala. The average O3, CO, NO2, and SO2 mixing ratios detected were 29.65 ± 11.44 ppb, 123.78 ± 73.35 ppb, 3.79 ± 0.98 ppb, and 4.59 ± 0.88 ppb during the observation period, and the statistical results of the monthly mean values revealed that there were differences during the highest pollution period, with O3 and CO mainly peaking in February, with mixing ratios of 38.03 ± 7.10 ppb and 208.50 ± 106.50 ppb, respectively. Meanwhile, NO2 peaked in March (4.51 ± 0.54 ppb) and SO2 in January (5.70 ± 1.92 ppb). The most obvious diurnal variation of CO and SO2 was observed in the winter, with maximum levels reaching between 13 : 00 and 14 : 00. The diurnal variations of O3 exhibited low values during the night and maximum values in the afternoon (16 : 00–18 : 00). Diurnal variation was not significant in the case of NO2. Cluster analysis showed that six main paths affected the Akedala atmosphere. In turn, the PSCF and CWT analysis results indicated that the Akedala reactive gas was affected by both local and foreign sources. The high PSCF value of the reactive gas potential source areas appeared in eastern Kazakhstan, northern Xinjiang, Western Mongolia, and Southern Russia. The WCWT (weighted concentration-weight trajectory) values of CO and SO2 in winter were the highest, totaling 180–240 ppb and 5–6.5 ppb, respectively. The WCWT value of O3 in the spring and summer was higher than that in the autumn and winter. The main source area of O3 was about 32–36 ppb in the spring and summer, and the main source area of NO2 in the summer had a low WCWT value of 3–3.5 ppb, whereas the NO2 WCWT value was concentrated at 4–4.5 ppb in the other seasons.

Open‐Path Dual‐Comb Spectroscopy for Multispecies Trace Gas Detection in the 4.5–5 µm Spectral Region

AbstractOpen‐path dual‐comb spectroscopy provides multispecies atmospheric gas concentration measurements with high precision. Here, open‐path dual‐comb spectroscopy is extended to the mid‐infrared 5 µm atmospheric window, enabling atmospheric concentration retrievals of the primary greenhouse gases, N2O, CO2, and H2O, as well as the criteria air pollutants O3 and CO across 600 m and 2 km round‐trip paths. Measurements are demonstrated over a five‐day period at 2 min temporal resolution with 80% uptime. The achieved precision is sufficient to resolve the atmospheric concentration variations of the multiple gas species; retrieved dry mixing ratios of CO and N2O are in good agreement with a colocated point sensor. In addition, the retrieved ratio of excess CO versus CO2 agrees with similar urban studies but disagrees with the US National Emission Inventory by a factor of 3. The retrieved ratio of excess N2O versus CO2 exhibits a plume‐dependent value, indicating the variability of sources of the greenhouse gas N2O.

Contribution of source emissions in the air pollution modeling - a WRF/Chem case study

We investigate the capability of the WRF/Chem model in the simulation of some criteria air pollutants, during a major air pollution episode between 16 and 21 December 2017. In this study, by employing the EDGAR-HTAP_v2 global emissions data in the WRF/Chem model, we evaluate the simulations of the surface mixing ratios of NO2, SO2, and CO. The RADM2 chemical mechanism with MADE-SORGAM aerosol scheme has been used as the chemical option of the WRF/Chem model, to simulate the meteorology-chemistry interactions. The variations of the time series of the pollutants and the comparisons of the results in Tehran with the measurement data showed that although the WRF/Chem simulations in Tehran presented considerable over-estimations, but the model’s performance with regard to the time variations of the concentrations of the gaseous agents over the polluted episode is acceptable, and therefore, could be considered in the operational air quality systems. Since emission data are not available for many metropolitan areas over Iran, the HTAP_v2 global dataset could be used as the emissions data with reliable accuracy for the numerical air quality models.

Determination of the emission rates of CO<sub>2</sub> point sources with airborne lidar

Abstract. Anthropogenic point sources, such as coal-fired power plants, produce a major share of global CO2 emissions. International climate agreements demand their independent monitoring. Due to the large number of point sources and their global spatial distribution, the implementation of a satellite-based observation system is convenient. Airborne active remote sensing measurements demonstrate that the deployment of lidar is promising in this respect. The integrated path differential absorption lidar CHARM-F is installed on board an aircraft in order to detect weighted column-integrated dry-air mixing ratios of CO2 below the aircraft along its flight track. During the Carbon Dioxide and Methane Mission (CoMet) in spring 2018, airborne greenhouse gas measurements were performed, focusing on the major European sources of anthropogenic CO2 emissions, i.e., large coal-fired power plants. The flights were designed to transect isolated exhaust plumes. From the resulting enhancement in the CO2 mixing ratios, emission rates can be derived via the cross-sectional flux method. On average, our results roughly correspond to reported annual emission rates, with wind speed uncertainties being the major source of error. We observe significant variations between individual overflights, ranging up to a factor of 2. We hypothesize that these variations are mostly driven by turbulence. This is confirmed by a high-resolution large eddy simulation that enables us to give a qualitative assessment of the influence of plume inhomogeneity on the cross-sectional flux method. Our findings suggest avoiding periods of strong turbulence, e.g., midday and afternoon. More favorable measurement conditions prevail during nighttime and morning. Since lidars are intrinsically independent of sunlight, they have a significant advantage in this regard.

Air-broadening in near-infrared carbon dioxide line shapes: Quantifying contributions from O2, N2, and Ar

We measured air broadening in the (30012) ← (00001) carbon dioxide (CO2) band up to Jʺ = 50 using frequency-agile rapid scanning cavity ring-down spectroscopy. By using synthetic air samples with varying levels of nitrogen, oxygen, and argon, multi-spectrum fitting allowed for the collisional broadening terms of each major air component to be simultaneously determined in addition to advanced line shape parameters at atmospherically relevant CO2 mixing ratios. These values were compared to broadener-specific line shape parameters from the literature. Fits to measured spectra were also constrained with results from requantized classical molecular dynamic simulations. We show that this approach enables differentiation between narrowing mechanisms in advanced line shape parameters retrieved from experimental spectra of limited signal-to-noise ratio.

Venus upper atmosphere revealed by a GCM: II. Model validation with temperature and density measurements

An improved high resolution (96 longitude by 96 latitude points) ground-to-thermosphere version of the Institut Pierre-Simon Laplace (IPSL) Venus General Circulation Model (VGCM), including non-orographic gravity waves (GW) parameterization and fine-tuned non-LTE parameters, is presented here. We focus on the validation of the model built from a collection of data mostly from Venus Express (2006–2014) experiments and coordinated ground-based telescope campaigns, in the upper mesosphere/lower thermosphere of Venus (80–150 km). These simulations result in an overall better agreement with temperature observations above 90 km, compared with previous versions of the VGCM. Density of CO2 and light species, such as CO and O, are also comparable with observations in terms of trend and order of magnitude. Systematic biases in the temperature structure are found between 80 and 100 km approximately (e.g. GCM is 20 to 40 K warmer than measurements) and above 130 km at the terminator (e.g. GCM is up to 50 K colder than observed). Possible candidates for those discrepancies are the uncertainties on the collisional rate coefficients used in the non-LTE parameterization (above 130 km), and assumptions on the CO2 mixing ratio made for stellar/solar occultation retrievals. Diurnal and latitudinal distribution of dynamical tracers (i.e. CO and O) are also analyzed, in a region poorly constrained by wind measurements and characterized by high variability over daily to weekly timescale. Overall, our simulations indicate that a weak westward retrograde wind is present in the mesosphere, up to about 120 km, producing the CO bulge displacement toward 2 h–3 h in the morning, instead of piling up at the anti-solar point, as for an idealized sub-solar to anti-solar circulation. This retrograde imbalance is suggested to be produced by perturbations of a ~ 5 days Kelvin wave impacting the mesosphere up to 110 km (described in a companion paper Navarro et al., 2021), combined with GW westward acceleration in the lower thermosphere, mostly above 110 km. On the whole, these model developments point to the importance of the inclusion of the lower atmosphere, higher resolution and finely tuned parameterizations in GCM of the Venusian upper atmosphere, in order to shed light on existing observations.

Validation of WRF-Chem Model and CAMS Performance in Estimating Near-Surface Atmospheric CO2 Mixing Ratio in the Area of Saint Petersburg (Russia)

Nowadays, different approaches for CO2 anthropogenic emission estimation are applied to control agreements on greenhouse gas reduction. Some methods are based on the inverse modelling of emissions using various measurements and the results of numerical chemistry transport models (CTMs). Since the accuracy and precision of CTMs largely determine errors in the approaches for emission estimation, it is crucial to validate the performance of such models through observations. In the current study, the near-surface CO2 mixing ratio simulated by the CTM Weather Research and Forecasting—Chemistry (WRF-Chem) at a high spatial resolution (3 km) using three different sets of CO2 fluxes (anthropogenic + biogenic fluxes, time-varying and constant anthropogenic emissions) and from Copernicus Atmosphere Monitoring Service (CAMS) datasets have been validated using in situ observations near the Saint Petersburg megacity (Russia) in March and April 2019. It was found that CAMS reanalysis data with a low spatial resolution (1.9° × 3.8°) can match the observations better than CAMS analysis data with a high resolution (0.15° × 0.15°). The CAMS analysis significantly overestimates the observed near-surface CO2 mixing ratio in Peterhof in March and April 2019 (by more than 10 ppm). The best match for the CAMS reanalysis and observations was observed in March, when the wind was predominantly opposite to the Saint Petersburg urbanized area. In contrast, the CAMS analysis fits the observed trend of the mixing ratio variation in April better than the reanalysis with the wind directions from the Saint Petersburg urban zone. Generally, the WRF-Chem predicts the observed temporal variations in the near-surface CO2 reasonably well (mean bias ≈ (−0.3) − (−0.9) ppm, RMSD ≈ 8.7 ppm, correlation coefficient ≈ 0.61 ± 0.04). The WRF-Chem data where anthropogenic and biogenic fluxes were used match the observations a bit better than the WRF-Chem data without biogenic fluxes. The diurnal time variation in the anthropogenic emissions influenced the WRF-Chem data insignificantly. However, in general, the data of all three WRF-Chem model runs give almost the same CO2 temporal variation in Peterhof in March and April 2019. This could be related to the late start of the growing season, which influences biogenic CO2 fluxes, inaccuracies in the estimation of the biogenic fluxes, and the simplified time variation pattern of the CO2 anthropogenic emissions.

GIS-Based Approach to Spatio-Temporal Interpolation of Atmospheric CO2 Concentrations in Limited Monitoring Dataset

Understanding the magnitude and distribution of the mixes of the near-ground carbon dioxide (CO2) components spatially (related to the surface characteristics) and temporally (over seasonal timescales) is critical to evaluating present and future climate impacts. Thus, the application of in situ measurement approaches, combined with the spatial interpolation methods, will help to explore variations in source contribution to the total CO2 mixing ratios in the urban atmosphere. This study presents the spatial characteristic and temporal trend of atmospheric CO2 levels observed within the city of Wroclaw, Poland for the July 2017–August 2018 period. The seasonal variability of atmospheric CO2 around the city was directly measured at the selected sites using flask sampling with a Picarro G2201-I Cavity Ring-Down Spectroscopy (CRDS) technique. The current work aimed at determining the accuracy of the interpolation techniques and adjusting the interpolation parameters for estimating the magnitude of CO2 time series/seasonal variability in terms of limited observations during the vegetation and non-vegetation periods. The objective was to evaluate how different interpolation methods will affect the assessment of air pollutant levels in the urban environment and identify the optimal sampling strategy. The study discusses the schemes for optimization of the interpolation results that may be adopted in areas where no observations are available, which is based on the kriging error predictions for an appropriate spatial density of measurement locations. Finally, the interpolation results were extended regarding the average prediction bias by exploring additional experimental configurations and introducing the limitation of the future sampling strategy on the seasonal representation of the CO2 levels in the urban area.

Characteristics of atmospheric CO2 fluxes and the estimation of their potential sources around Boseong Standard Weather Observatory (BSWO)

We report the characteristics of the mixing ratios and fluxes of atmospheric carbon dioxide, observed in the period from July 2015 to December 2019. Measurements were noted for three different levels (60 m, 140 m, and 300 m above ground level (a.g.l.)) on a very tall (~300 m) tower in the Boseong Standard Weather Observatory (BSWO), located at the center of barley–rice double-crop fields in Boseong-gun, Jeolla-do, South Korea. The averaged CO2 mixing ratios show 420.7 ± 18.8 (60 m), 410.9 ± 16.7 (140 m) and 403.4 ± 16.7 ppm (300 m). The mixing ratios measured at the 140-m and 300-m heights display a typical seasonal pattern that is lower in the summer due to vegetation uptake and higher in the winter due to plant decaying combined with fossil-fuel emissions, but those at 60 m presented higher values in the spring and autumn, mainly owing to agricultural activities. During the study period, the averaged CO2 fluxes are −0.28 ± 8.81 (60 m), 0.34 ± 8.08 (140 m), and 0.79 ± 9.08 μmol m-2 s-1 (300 m). The monthly averaged fluxes show two dominant negative peaks, one in April and another in August, mainly caused by CO2 uptake during the barley and rice growing periods, respectively. The fluxes represent a strong correlation between daytime solar radiation and photosynthesis and between nighttime air temperatures and respiration. Directional analysis of the fluxes revealed dominant anthropogenic CO2 sources from not only the main industrial areas in the NE directions using geographic information system (GIS), but also from the aquaculture industry in the SE. We compare our measured CO2 fluxes (top-down) with a few bottom-up emissions datasets, which reveal an underestimation of the range from 31% to 69% within the footprint areas. The application of direct measurements of CO2 fluxes, combined with estimation of potential vicinity sources, can be a useful tool to detect local unknown or missing sources and supplement the gap between top-down and bottom-up approaches.

Multi-instrument analysis of far-ultraviolet aurora in the southern hemisphere of comet 67P/Churyumov-Gerasimenko

Aims.We aim to determine whether dissociative excitation of cometary neutrals by electron impact is the major source of far-ultraviolet (FUV) emissions at comet 67P/Churyumov-Gerasimenko in the southern hemisphere at large heliocentric distances, both during quiet conditions and impacts of corotating interaction regions observed in the summer of 2016.Methods.We combined multiple datasets from the Rosetta mission through a multi-instrument analysis to complete the first forward modelling of FUV emissions in the southern hemisphere of comet 67P and compared modelled brightnesses to observations with the Alice FUV imaging spectrograph. We modelled the brightness of OI1356, OI1304, Lyman-β, CI1657, and CII1335 emissions, which are associated with the dissociation products of the four major neutral species in the coma: CO2, H2O, CO, and O2. The suprathermal electron population was probed by the Ion and Electron Sensor of the Rosetta Plasma Consortium and the neutral column density was constrained by several instruments: the Rosetta Orbiter Spectrometer for Ion and Neutral Analysis (ROSINA), the Microwave Instrument for the Rosetta Orbiter and the Visual InfraRed Thermal Imaging Spectrometer.Results.The modelled and observed brightnesses of the FUV emission lines agree closely when viewing nadir and dissociative excitation by electron impact is shown to be the dominant source of emissions away from perihelion. The CII1335 emissions are shown to be consistent with the volume mixing ratio of CO derived from ROSINA. When viewing the limb during the impacts of corotating interaction regions, the model reproduces brightnesses of OI1356 and CI1657 well, but resonance scattering in the extended coma may contribute significantly to the observed Lyman-βand OI1304 emissions. The correlation between variations in the suprathermal electron flux and the observed FUV line brightnesses when viewing the comet’s limb suggests electrons are accelerated on large scales and that they originate in the solar wind. This means that the FUV emissions are auroral in nature.

Characteristics of sub-10 nm particle emissions from in-use commercial aircraft observed at Narita International Airport

Abstract. The characterization of ultrafine particle emissions from jet aircraft equipped with turbofan engines, which are commonly used in civil aviation, is an important issue in the assessment of the impacts of aviation on climate and human health. We conducted field observations of aerosols and carbon dioxide (CO2) near a runway at Narita International Airport, Japan, in February 2018. We used an ultrafine condensation particle counter (UCPC) and a condensation particle counter (CPC) with unheated and 350 ∘C heated operation modes to investigate the contributions of sub-10 nm size ranges to the total and the non-volatile particle number concentrations. The performance of the 350 ∘C heated mode was tested in the laboratory to verify the consistency with existing methods for non-volatile particle measurements. We also used a scanning mobility particle sizer with unheated and 350 ∘C heated modes and an engine exhaust particle sizer for the measurements of particle number size distributions. Spiked increases in the particle number concentrations and CO2 mixing ratios were observed to be associated with the directions of wind from the runway, which can be attributed to diluted aircraft exhaust plumes. We estimated the particle number emission indices (EIs) for discrete take-off plumes using the UCPC, CPC, and CO2 data. The median values of the total and the non-volatile particle number EIs for diameters larger than 2.5 nm as derived from the UCPC data were found to be 1.1×1017 and 5.7×1015 kg per fuel, respectively. More than half the particle number EIs were in the size range smaller than 10 nm for both the total and the non-volatile particles in most of the cases analyzed in this study. The significance of sub-10 nm size ranges for the total particles in the diluted plumes was qualitatively consistent with previous studies, but that for the non-volatile particles was unexpected. Possible factors affecting the similarities and differences compared with the previous findings are discussed.