Trace Gas Concentrations Research Articles

MAP-IO: an atmospheric and marine observatory program on board Marion Dufresne over the Southern Ocean

Abstract. This article is devoted to the presentation of the MAP-IO observation program. This program, launched in early 2021, has enabled the observation of nearly 700 d of measurements over the Indian and Southern Ocean with the equipment of 17 meteorological and oceanographic scientific instruments on board the ship Marion Dufresne. Several observational techniques have been developed to respond to the difficulties of observations on board the ship, in particular for passive remote sensing data, as well as for quasi-autonomous data acquisition and transfer. The first measurements made it possible to draw up unprecedented climatological data of the Southern Ocean regarding the size distribution and optical thickness of aerosols, the concentration of trace gases and greenhouse gases, UV, and integrated water vapor. High-resolution observations of phytoplankton in surface waters have also shown a great variability in latitude in terms of abundance and community structure (diversity). The operational success of this program and these unique scientific results together establish a proof of concept and underline the need to transform this program into a permanent observatory. The multi-year rotations over the Indian Ocean will enable us to assess the trends and seasonal variability of phytoplankton, greenhouse gases, ozone, and marine aerosols in a sensitive and poorly documented climatic region. Without being exhaustive, MAP-IO should make it possible to better understand and assess the biological carbon pump, to study the variability of gases and aerosols in a region that is remote in relation to the main anthropogenic sources, and to monitor the transport of stratospheric ozone by the Brewer–Dobson circulation. The meteorological MAP-IO data set is publicly available at https://www.aeris-data.fr/catalogue-map-io/ (last access: 26 August 2024) (atmospheric data) and at https://doi.org/10.17882/89505 (Thyssen et al., 2022a) (phytoplankton data).

Using the phase III slope of exhaled methane during a single breath DLCO test to assess ventilation heterogeneity

BackgroundThe Phase III slope from a single breath nitrogen washout test provides information about ventilation heterogeneity (VH) in the lungs. PurposeTo determine if the Phase III slope from the exhaled tracer gas concentration during a standard, single breath DLCO test using rapid gas analysis provides similar information about VH. Basic proceduresRetrospective analysis of clinical pulmonary function laboratory data including spirometry, lung volumes, and DLCO. The normalized Phase III slope from the exhaled CH4 concentration (SnCH4) was compared among different patterns of physiologic abnormality and with VA/TLC as an indicator of VH. Main findingsSnCH4 was the steepest in the group with “Obstruction and Low DLCO”, with significant differences between this group and the “Normal”, “Obstruction with Normal DLCO”, “Mixed Obstruction and Restriction” and “Isolated Low DLCO” groups. SnCH4 was steeper in current and former smokers compared to non-smokers. Among the entire study sample, SnCH4 correlated with VA/TLC (Spearman rho = −0.56, p < 0.01) and remained a significant determinant of VA/TLC by regression modeling. Principal conclusionsThe SnCH4 derived from a standard, single breath DLCO test using rapid gas analysis varied among distinct patterns of physiologic abnormalities and was associated with VA/TLC as a measure of VH.

Environmental conditions affecting air pollution dispersion over Richards Bay, South Africa

Air pollution dispersion over Richards Bay, South Africa is studied using satellite, reanalysis and in-situ measurements. Near-surface concentrations of trace gases and particulates reach high concentrations under dry stable ‘berg’ winds. Temporal records of CO, NO2, O3, PM2.5, SO2 (2000-2023) exhibit no trend and short-term dose exceedances of individual pollutants are rare and confined to winter mornings. Regional point-to-field correlation maps of a Richards Bay winter air pollution index found that anomalous warming of the west Indian Ocean accelerates the jet stream over Madagascar and pulls smoke- and dust-laden north-westerly winds across the South African plateau, implicating long-range transport. At daily and hourly time scales dewpoint temperature and boundary layer height best indicate changes in local air pollution dispersion that impact respiratory health. A case study of 15-17 June 2021 revealed a 10ºC thermal inversion caused by negative sensible heat fluxes of -40 W/m2 through the night, leading to SO2 concentrations above 100 ppb in the morning along the main access road (28.8ºS, 32ºE). Poor dispersion seldom happens in the summer when turbulent mixing and rainfall cleanse the air.

Measurement report: Cloud and environmental properties associated with aggregated shallow marine cumulus and cumulus congestus

Abstract. Mesoscale organization of marine convective clouds into linear or clustered states is prevalent across the tropical and subtropical oceans, and its investigation served as a guiding focus for a series of process study flights conducted as part of the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) during summer 2020, 2021, and 2022. These select ACTIVATE flights involved a novel strategy for coordinating two aircraft, with respective remote sensing and in situ sampling payloads, to probe regions of organized shallow convection for several hours. The main purpose of this measurement report is to summarize the aircraft sampling approach, describe the characteristics and evolution of the cases, and provide an overview of the datasets that can serve as a starting point for more detailed modeling and analysis studies. Six flights are described, involving a total of 80 dropsonde profiles that capture the environment surrounding clustered shallow convection. The flights include detailed observations of the vertical structure of cloud systems, comprising up to 20 in situ sampling levels. Four cases involved deepening convection rooted in the marine boundary layer that developed vertically to 2–5 km with varying precipitation amounts, while two cases captured more complex and developed cumulus congestus systems extending above 5 km. In addition to the thermodynamic and dynamic characterization afforded by dropsonde and in situ measurements, the datasets include cloud and aerosol microphysics, trace gas concentrations, aerosol and droplet composition, and cloud and aerosol remote sensing from high-spectral-resolution lidar and polarimetry.

MALTA: A Zonally Averaged Global Atmospheric Transport Model for Long‐Lived Trace Gases

AbstractWe present a two‐dimensional, zonally averaged global model of atmospheric transport named MALTA: Model of Averaged in Longitude Transport in the Atmosphere. It aims to be accessible to a broad community of users, with the primary function of quantifying emissions of greenhouse gases and ozone depleting substances. The model transport is derived from meteorological reanalysis data and flux‐gradient experiments using a three‐dimensional transport model. Atmospheric sinks are prescribed loss frequency fields. The zonally averaged model simulates important large‐scale transport features such as the influence on trace gas concentrations of the quasi‐biennial oscillation and variations in inter‐hemispheric transport rates. Stratosphere‐troposphere exchange is comparable to a three‐dimensional model and inter‐hemispheric transport is faster by up to 0.3 years than typical transport times of three‐dimensional models, depending on the metric used. Validation of the model shows that it can estimate emissions of CFC‐11 from an incorrect a priori emissions field well using three‐dimensional (3D) mole fraction fields generated using a different 3D model than which the flux gradient relationships were derived. The model is open source and is expected to be applicable to a wide range of studies requiring a fast, simple model of atmospheric transport and chemical processes for estimating associated emissions or mole fractions.

Insights into atmospheric trace gases, aerosols, and transport processes at a high-altitude station (2623 m a.s.l.) in Northeast Asia

As part of the efforts to understand long-range air pollution transport in Northeast Asia, a comprehensive field measurement campaign was conducted at the top of Changbai Mountain (2623 m a.s.l.) from 25th July to 21st August in 2021. The ambient concentrations of trace gases and chemical characteristics of fine particulate matter (PM2.5) were comparable to those at background or free tropospheric locations in China, but exceeded levels at corresponding sites in Europe and the United States. Well-defined diurnal variations were evident in most air pollutants, including carbon monoxide (CO), sulfur dioxide (SO2), and nitrogen oxide (NOx), reflecting the influence of boundary layer development and local anthropogenic activities. Ozone (O3) exhibited a unique diurnal distribution, with lower concentrations during the daytime and higher levels at nighttime, indicating a pronounced impact of downward transport of O3-rich air from the upper troposphere during the nighttime. During the campaign, organic carbon (OC) constituted the predominant component of PM2.5, comprising 43% of the total, while sulfate (SO42−) was the most abundant secondary inorganic component in PM2.5, accounting for 26%. Combining the analysis of air mass backward trajectories, we found that Changbai Mountain is primarily influenced by air masses originating from North Korea and the Sea of Japan, constituting 62% of the total, and local vegetation biological emissions and anthropogenic emissions in North Korea notably affect the observation site. Conversely, the secondary aerosol components were most abundant in marine air mass originating from the marginal seas of China and the strait between the Korean peninsula and southern Japan. Utilizing the Lagrangian photochemical trajectory model (LPTM), a significant increase in particulate SO42− concentrations was observed when air mass passed through the marginal seas of China, primarily due to SO2 oxidation reaction. This study contributes to an improved understanding of the atmospheric chemistry in the high-altitude regions of Northeast Asia and underscores the substantial role of secondary inorganic aerosol formation during the transport of marine air masses.

Possible influence of Martian surface mineralogy on the detectability of atmospheric trace gases - mid-infrared simulation results

The paper focuses on the influence of the optical properties of Martian surface minerals on remotely detected gaseous components of the Martian atmosphere, when the spectrometer receives a combined signal from the Martian soil and atmosphere. Our considerations are primarily concerned with the detectability of methane, but the problem may also apply to other trace gases. Detections of methane in the Martian atmosphere have been reported from Mars Express (orbiting Mars), the Curiosity rover on the Martian surface, and from Earth. Its presence in the Martian atmosphere is being questioned today. The reason for these doubts is that both spectrometers onboard ExoMars Trace Gas Orbiter have not yet detected any methane in the Martian atmosphere using the very sensitive solar occultation method. The solar occultation method is unable to probe the lowest layers of the atmosphere at mid-latitudes, and so, its presence in this part of the atmosphere is assumed to be due to its possible source in the ground, as suggested by some works.This paper considers whether the spectral characteristics of the soil may hinder the remote detection of methane. One of the examples discussed in the article relates to the possible observation of methane over mineralogical surfaces that may be the source of this gas. The examples of other surface mineralogical compositions are also discussed. The series of numerical simulations carried out in the region of the strong methane absorption band and the examples where the optical properties of the surface change the shape and contrast of this absorption band are shown. The codes used provide estimates of the spectral reflectance/emittance and total radiance of the Martian surface and atmosphere in the mid-infrared spectral region. The surface covered by dust was described by the reflectance and emittance calculated from n,k using Mie and Hapke theories or known from laboratory measurements. The different concentrations of atmospheric trace gases were taken into account.

Statistical assessment of the concentration fluctuations in street canyons via time-resolved wind tunnel experiments

Time-resolved wind tunnel experiments are performed for three periodic street canyon configurations: one of uniform (H/W = 1) and two of variable building height (consisting of 0.5H and 1.5H tall towers in aligned and staggered arrangements) for perpendicular wind direction. The velocity field is mapped using Laser Doppler Anemometry (LDA), and the tracer gas concentration is sampled using Fast Flame Ionization Detection (FFID). The concentration field is characterized by the mean concentration and the characteristic percentiles of the concentration-time series, such as the median and the peak, represented by the 99th percentile, in a total of 1138 sampling points. The probability distribution of the concentration in each point is modeled using the gamma distribution, which is fitted based on the mean and the variance of the measured time series. The results show that the mean pedestrian exposure to air pollutants is significantly lower in the case of heterogeneous roof height, although the mean concentration at the leeward corner of the source canyon can locally exceed those of the uniform street canyons for both tower arrangements of variable building height. Moreover, it is shown that the concentration peaks for both tower configurations can significantly exceed those of the uniform canyons case, especially near the sources.

New evidence for CH4 enhancement in the upper troposphere associated with the Asian summer monsoon

The Asian summer monsoon (ASM) region is a key region transporting air to the upper troposphere (UT), significantly influencing the distribution and concentration of trace gases, including methane (CH4), an important greenhouse gas. We investigate the seasonal enhancement of CH4 in the UT over the ASM region, utilizing retrievals from the Atmospheric Infrared Sounder (AIRS), model simulations and in-situ measurements. Both the AIRS data and model simulation reveal a substantial enhancement in CH4 concentrations within the active monsoon region of up to 3%, referring to the zonal means, and of up to 6% relative to the pre-monsoon season. Notably, the spatial distribution of the CH4 plume demonstrates a southwestward shift in the AIRS retrievals, in contrast to the model simulations, which predict a broader enhancement, including a significant increase to the east. A cross-comparison with in-situ measurements, including AirCore measurements over the Tibetan Plateau and airline sampling across the ASM anticyclone (ASMA), favors the enhancement represented by model simulation. Remarkable CH4 enhancement over the west Pacific is also evidenced by in-situ data and simulation as a dynamical extension of the ASMA. Our findings underscore the necessity for cautious interpretation of satellite-derived CH4 distributions, and highlight the critical role of in-situ data in anchoring the assimilation of CH4.

Identification of exhaust stack sampling location of a research reactor considering ANSI/HPS N13.1-2011 mixing criteria using computational fluid dynamics

ABSTRACT Research Reactors have exhaust stacks that emit filtered radioactive gaseous waste into the atmosphere. In this research work, to check whether the radioactive gaseous waste met the requirements of ANSI/HPS N13.1–2011 mixing criteria, computational fluid dynamics (CFD) analysis was performed. According to ANSI criteria, Coefficient of Variance (COV) of velocity uniformity, flow angle, tracer gas, and aerosol particles concentration should be less than 20%. Therefore, the COV of the four parameters at different sampling positions along the stack height, with eight tracer gas and eight particles injection cases, were analyzed. The COV of velocity at 6 m height is 17.5% and flow cyclone is 9.8 degree. The results indicated that the 6 m height of the stack is enough for cyclone angle and COV of velocity to fulfill the ANSI mixing criteria. The COV of tracer gas concentration in one to eight injection cases is 10%, 4.8%, 7.5%, 17%, 2.5%, 6%, 13%, and 5% at 14 m stack height so the tracer gas also satisfied the standard mixing criteria in a concise length of 14 m because of the minimal difference in densities of tracer gas and air. However, due to their much higher density, aerosol particles took much longer to mix into the air. At 60 m stack height, the COV of aerosol particle concentration in one to eight injection cases is 14.8%, 18%, 8%, 12%, 11%, 15%, 15.5%, and 2%, respectively. As a result, when the stack height is set to 60 m, the COV of velocity, cyclone flow angle, tracer gas concentration, and aerosol particle concentration are found to meet the ANSI mixing criteria. Therefore, the minimum recommended height of the stack is proposed to be 60 m for the case under consideration.

CFD modelling of velocity fields around a fume cupboard: Evaluating static and dynamic meshes with experimental measurements

This paper presents a comparison of experimental and numerical modelling results of the velocity field around a fume cupboard with a static and a dynamic mesh. During fume cupboard testing, components are required to move which mimic typical operating conditions, the amount of tracer gas released is then measured. This tracer gas is harmful to the environment and so an alternative is required. Advanced Computational Fluid Dynamics (CFD) techniques, such as dynamic meshing, have been utilised to replicate aspects of the current tests. The fume cupboard was tested in normal operating conditions and under the influence of a board inducing a wake close to the fume cupboard entrance. The velocity fields have been compared and show a reasonable level of accuracy with a percentage difference between experimental and simulated results of around 5% using both a static and a dynamic domain. This is an improvement on the 15–20% accuracy for detecting concentration of tracer gas using previous experimental methods. The aim of this work is to satisfy the scientific community and fume cupboard operators that CFD is sufficiently accurate to assess fume cupboard performance under real world scenarios.

Evaluation of the first year of Pandora NO2 measurements over Beijing and application to satellite validation

Abstract. Nitrogen dioxide (NO2) is a highly photochemically reactive gas, has a lifetime of only a few hours, and at high concentrations is harmful to human beings. Therefore, it is important to monitor NO2 with high-precision, time-resolved instruments. To this end, a Pandora spectrometer has been installed on the roof of the laboratory building of the Aerospace Information Research Institute of the Chinese Academy of Sciences in the Olympic Park, Beijing, China. The concentrations of trace gases (including NO2, HCHO, O3) measured with Pandora are made available through the open-access Pandora database (https://data.pandonia-global-network.org/Beijing-RADI/Pandora171s1/, last access: 11 July 2023). In this paper, an overview is presented of the Pandora total and tropospheric NO2 vertical column densities (VCDs) and surface concentrations collected during the first year of operation, i.e., from August 2021 to July 2022. The data show that NO2 concentrations were high in the winter and low in the summer, with a diurnal cycle where the concentrations reached a minimum during the daytime. The concentrations were significantly lower during the 2022 Winter Olympics in Beijing, showing the effectiveness of the emission control measures during that period. The Pandora observations show that during northerly winds, clean air is transported to Beijing with low NO2 concentrations, whereas during southerly winds, pollution from surrounding areas is transported to Beijing and NO2 concentrations are high. The contribution of tropospheric NO2 to the total NO2 VCD varies significantly on daily to seasonal timescales; i.e., monthly averages vary between 50 % and 60 % in the winter and between 60 % and 70 % in the spring and autumn. A comparison of Pandora-measured surface concentrations with collocated in situ measurements using a Thermo Scientific 42i-TL analyzer shows that the Pandora data are low and that the relationship between Pandora-derived surface concentrations and in situ measurements is different for low and high NO2 concentrations. Explanations for these differences are offered in terms of measurement techniques and physical (transport) phenomena. The use of Pandora total and tropospheric NO2 VCDs for validation of collocated TROPOspheric Monitoring Instrument (TROPOMI) data, resampled to 100 m × 100 m, shows that although on average the TROPOMI VCDs are slightly lower, they are well within the expected error for TROPOMI of 0.5 Pmolec.cm-2 + (0.2 to 0.5) ⋅ VCDtrop (1 Pmolec.cm-2 = 1 × 1015 molec cm−2). The location of the Pandora instrument within a sub-orbital TROPOMI pixel of 3.5 km × 5.5 km may result in an error in the TROPOMI-derived tropospheric NO2 VCD between 0.223 and 0.282 Pmolec.cm-2, i.e., between 1.7 % and 2 %. In addition, the data also show that the Pandora observations at the Beijing-RADI site are representative of an area with a radius of 10 km.

Exploring Spatial and Temporal Dynamics of Red Sea Air Quality through Multivariate Analysis, Trajectories, and Satellite Observations

The Red Sea, a significant ecoregion and vital marine transportation route, has experienced a consistent rise in air pollution in recent years. Hence, it is imperative to assess the spatial and temporal distribution of air quality parameters across the Red Sea and identify temporal trends. This study concentrates on utilizing multiple satellite observations to gather diverse meteorological data and vertical tropospheric columns of aerosols and trace gases, encompassing carbon monoxide (CO), nitrogen dioxide (NO2), sulfur dioxide (SO2), and ozone (O3). Furthermore, the study employs the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model to analyze the backward trajectory of air mass movement, aiding in the identification of significant sources of air pollutants. A principal component analysis (PCA) with varimax rotation is applied to explore the relationship and co-variance between the aerosol index (AI), trace gas concentrations, and meteorological data. The investigation reveals seasonal and regional patterns in the tropospheric columns of trace gases and AI over the Red Sea. The correlation analysis indicates medium-to-low positive correlations (0.2 &lt; r &lt; 0.6) between air pollutants (NO2, SO2, and O3) and meteorological parameters, while negative correlations (−0.3 &lt; r &lt; −0.7) are observed between O3, aerosol index, and wind speed. The results from the HYSPLIT model unveil long-range trajectory patterns. Despite inherent limitations in satellite observations compared to in situ measurements, this study provides an encompassing view of air pollution across the Red Sea, offering valuable insights for future researchers and policymakers.

Compensation of composition variation-induced sensitivity changes in gas phase photoacoustics

Infrared photoacoustic (PA) spectroscopy is a widely used technique to monitor trace gas concentration changes during industrial processes where the bulk composition may vary considerably. However, the PA signal is prone to changes in bulk composition, leading to relative uncertainties in measurements of up to 10%, due to the complex dependence of the sensitivity of a PA system (S) on the thermal and acoustic properties of the gas sample. A novel calibration and concentration calculation method is proposed to keep the relative accuracy of the PA measurements in the few percentages range even in case of large-scale composition variations. The main novelty of the proposed method is that it tackles the complex dependence of the PA system's sensitivity in a way that while it varies the resonance frequency of the calibration gas, it keeps the heat capacity ratio of calibration gases at a constant value. We prove that it determines the analyte’s concentration with relative accuracy of about 1 %, even when the composition of the gas varies drastically. It rigorously compensates for the frequency and heat capacity ratio dependence of S and for the dependence of the half-width of the resonance curve of the PA cell on the thermal and acoustic properties of the gas. Although the reported demonstration measurements are executed in a relatively simple gas mixture, the proposed method has widespread applicability in high-precision monitoring.

Aerosol properties derived from ground-based Fourier transform spectra within the COllaborative Carbon Column Observing Network

Abstract. Fourier transform infrared (FTIR) spectroscopy is particularly relevant for climate studies due to its ability to provide information on both fine absorption structures (i.e. trace gases) and broadband continuum signatures (i.e. aerosols or water continuum) across the entire infrared (IR) domain. In this context, this study assesses the capability of the portable and compact EM27/SUN spectrometer, used within the research infrastructure COCCON (COllaborative Carbon Column Observing Network), to retrieve spectral aerosol properties from low-resolution FTIR solar absorption spectra (0.5 cm−1). The study focuses on the retrieval of aerosol optical depth (AOD) and its spectral dependence in the 873–2314 nm spectral range from COCCON measurements at the subtropical high-mountain Izaña Observatory (IZO, Tenerife, Spain), which were coincidentally carried out with standard sun photometry within the Aerosol Robotic Network (AERONET) in the 3-year period from December 2019 to September 2022. The co-located AERONET–COCCON database was used to cross-validate these two independent techniques in the common spectral range (870–1640 nm), demonstrating an excellent agreement at the near-coincident spectral bands (mean AOD differences limited to 0.005, standard deviations up to 0.021 and Pearson regression coefficients up to 0.97). This indicates that the low-resolution COCCON instruments are suitable for detecting the aerosol broadband signal contained in the IR spectra in addition to the retrieval of precise trace gas concentrations, provided a robust calibration procedure (Langley-based or absolute calibration procedures) is used to compensate for the optical degradation of the external system (∼ 0.72 % per month). The study also assesses the capability of the EM27/SUN to simultaneously infer aerosols and trace gases and relate their common emission sources in two case study events: a volcanic plume from the La Palma eruption in 2021 and a nearby forest fire in Tenerife in 2022. Overall, our results demonstrate the potential of the portable low-resolution COCCON instruments to enhance the multi-parameter capability of the FTIR technique for atmospheric monitoring.

Single field-of-view sounder atmospheric product retrieval algorithm: establishing radiometric consistency for hyper-spectral sounder retrievals

Abstract. The single field-of-view (SFOV) sounder atmospheric product (SiFSAP) retrieval algorithm has been developed to address the need to retrieve high-spatial-resolution atmospheric data products from hyper-spectral sounders and ensure the radiometric consistency between the retrieved properties and measured spectral radiances. It is based on an integrated optimal-estimation inversion scheme that processes data from the satellite-based synergistic microwave (MW) and infrared (IR) spectral measurements from advanced sounders. The retrieval system utilizes the principal component radiative transfer model (PCRTM), which performs radiative transfer calculations monochromatically and includes accurate cloud-scattering simulations. SiFSAP includes temperature, water vapor, surface skin temperature and emissivity, cloud height and microphysical properties, and concentrations of essential trace gases for each SFOV at a native instrument spatial resolution. Error estimations are provided based on a rigorous analysis for uncertainty propagation from the top-of-atmosphere (TOA) spectral radiances to the retrieved geophysical properties. As a comparison, the spatial resolution for the traditional hyper-spectral sounder retrieval products is much coarser than the native resolution of the instruments due to the common use of the “cloud-clearing” technique to compensate for the lack of cloud-scattering simulation in the forward model. The degraded spatial resolution in traditional cloud-clearing sounder retrieval products limits their applications for capturing meteorological or climate signals at finer spatial scales. Moreover, a rigorous uncertainty propagation estimation needed for long-term climate trend studies cannot be given due to the lack of direct radiative transfer relationships between the observed TOA radiances and the retrieved geophysical properties. With the advantages of the higher spatial resolution; the simultaneous retrieval of atmospheric, cloud, and surface properties using all available spectral information; and the establishment of “radiance closure” in the sounder spectral measurements, the SiFSAP provides additional information needed for various weather and climate studies and applications using sounding observations. This paper gives an overview of the SiFSAP retrieval algorithm and assessment of SiFSAP atmospheric temperature, water vapor, clouds, and surface products derived from the Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) data.

Impact of COVID-19 pandemic lockdown on atmospheric concentrations of particulate matter, trace gases and volatile organic compounds at a suburban site of Agra

Impact of COVID-19 pandemic lockdown on atmospheric concentrations of particulate matter, trace gases and volatile organic compounds at a suburban site of Agra

Spectral aerosol optical depth from SI-traceable spectral solar irradiance measurements

Abstract. Spectroradiometric measurements of direct solar irradiance traceable to the SI were performed by three spectroradiometer systems during a 3-week campaign in September 2022 at the Izaña Atmospheric Observatory (IZO) located on the island of Tenerife, Canary Islands, Spain. The spectroradiometers provided direct spectral irradiance measurements in the spectral ranges 300 to 550 nm (QASUME), 550 to 1700 nm (QASUME-IR), 300 to 2150 nm (BiTec Sensor, BTS), and 316 to 1030 nm (Precision Solar Spectroradiometer, PSR), with relative standard uncertainties of 0.7 %, 0.9 %, and 1 % for QASUME/QASUME-IR, the PSR, and the BTS respectively. The calibration of QASUME and QASUME-IR was validated prior to this campaign at Physikalisch-Technische Bundesanstalt (PTB) by measuring the spectral irradiance from two spectral irradiance sources, the high-temperature blackbody BB3200pg as a national primary standard and the tuneable laser facility TULIP. The top-of-atmosphere (ToA) solar irradiance spectra from the spectroradiometers were retrieved from direct solar irradiance measurements using zero-air-mass extrapolation during cloud-free conditions, which were then compared to the TSIS-1 Hybrid Solar Reference Spectrum (HSRS). These ToA solar spectra agreed to within 1 % for spectral ranges longer than 400 nm (for QASUME also at shorter wavelengths) in the spectral regions free of significant trace gas absorption and were well within the combined uncertainties over the full investigated spectral range. Using the results from the comparison with QASUME, the relative standard uncertainty of the TSIS-1 HSRS ToA solar spectrum in the spectral range 308 to 400 nm could be reduced from its nominal 1.3 % to 0.8 %, representing the relative standard uncertainty of the QASUME ToA solar spectrum in this spectral range. The spectral aerosol optical depth (AOD) retrieved from the solar irradiance measurements of these spectroradiometers using the TSIS-1 HSRS as the reference ToA solar spectrum agreed to within 0.01 in optical depth in nearly all common spectral channels of two narrowband filter radiometers belonging to the Global Atmosphere Watch Precision Filter Radiometer (GAW-PFR) network and Aerosol Robotic Network (AERONET). This study shows that it is now possible to retrieve spectral AOD over the extended spectral range from 300 to 1700 nm using solar irradiance measurements traceable to the SI using laboratory-calibrated spectroradiometers with similar quality to that from traditional Langley-based calibrated instruments. The main improvement to previous investigations is the recent availability of the high-spectral-resolution TSIS-1 HSRS with very low uncertainties, which provides the top-of-atmosphere reference for the spectral atmospheric transmission measurements obtained from ground-based solar irradiance measurements.

Spatiotemporal distribution of air pollutants during a heat wave-induced forest fire event in Uttarakhand.

Prevailing dry conditions and rainfall deficit during the spring season in North India led to heat wave conditions which resulted in widespread and intense forest fire events in the Himalayan state of Uttarakhand during April 16-30, 2022. A total of 7589 active fires were detected by VIIRS during the second half of April 2022 compared to 1558 during the first half. The TROPOMI observed total column values of CO and NO2 increased by 4.4% and 11.7%, respectively during April 16-30, 2022 with respect to April 1-15, 2022. A noticeable increase in surface level concentration of trace gases was also observed at Dehradun. In situ measurements of CO, NOx, and O3 during April 16-30, 2022 show an increase of 133, 35, and 6%compared to previous year observations during the same period. Weather Research and Forecasting model with chemistry (WRF-Chem) is utilized to quantitatively estimate the contribution of this event on the distribution of air pollutants over this state. The model results were evaluated against ERA5 reanalysis, upper air soundings, and TROPOMI-retrieved total column density (TCD) of CO, NO2, and O3. Two simulations with (Fire) and without (NoFire) biomassburning emissions input were performed to quantify the contribution of forest fires to the concentration of trace gases and particulates. The CO, NO2, and O3 emitted/produced from forest fire over Uttarakhand during April 2022 contributed approximately 39.95, 35.73, and 9.97% to the surface concentration of respective gas. In the case of aerosols, it was around 71.20, 71.44, and 33.62% for PM2.5, PM10, and BCrespectively. The vertical profile analysis of pollutants revealed that extreme forest fire events can perturb the distribution of air pollutants from the surface up to 450 hPa.

Examining the Summertime Ozone Formation Regime in Southeast Michigan Using MOOSE Ground‐Based HCHO/NO2 Measurements and F0AM Box Model

AbstractAmbient ozone (O3) concentrations in Southeast Michigan (SEMI) can exceed the U.S. National Ambient Air Quality Standard. Despite past efforts to measure O3 precursors and elucidate reaction mechanisms, changing emission patterns and atmospheric composition in SEMI warrant new measurements and updated mechanisms to understand the causes of observed O3 exceedances. In this study, we examine the chemical drivers of O3 exceedances in SEMI, based on the Phase I MOOSE (Michigan‐Ontario Ozone Source Experiment) field study performed during May to June 2021. A zero‐dimensional (0‐D) box model is constrained with measurement data of meteorology and trace gas concentrations. Box model sensitivity simulations suggest that the formaldehyde to nitrogen dioxide ratio (HCHO/NO2) for the transition between the volatile organic compounds (VOCs)‐ and nitrogen oxides (NOx)‐limited O3 production regimes is 3.0 ± 0.3 in SEMI. The midday (12:00–16:00) averaged HCHO/NO2 ratio during the MOOSE Phase I study is 1.62 ± 1.03, suggesting that O3 production in SEMI is limited by VOC emissions. This finding implies that imposing stricter regulations on VOC emissions should be prioritized for the SEMI O3 nonattainment area. This study, through its use of ground‐based HCHO/NO2 ratios and box modeling to assess O3‐VOC‐NOx sensitivities, has significant implications for air quality policy and the design of effective O3 pollution control strategies, especially in O3 nonattainment areas.