Search

In this study, we carried out an independent validation of two methane retrieval algorithms using spectra from the Infrared Atmospheric Sounding Interferometer (IASI) that has been aboard the Meteorological Operational Satellite A (MetOp-A) since 2006. Both algorithms, one developed by the Laboratoire de Météorologie Dynamique (LMD), called the non-linear inference scheme (NLISv8.3), and the other by the Rutherford Appleton Laboratory (RAL), referred to as RALv2.0, provide long-term global CH4 concentrations using distinctively different retrieval approaches (neural network vs. optimal estimation, respectively). They also differ with respect to the vertical range covered, where LMD provides mid-tropospheric dry-air mole fractions (mt CH4), and RAL provides mixing ratio profiles from which we can derive total column-averaged dry-air mole fractions (X CH4) and potentially two partial column layers (q CH4). We compared both CH4 products using the Copernicus Atmospheric Monitoring Service (CAMS) model, in situ profiles (range extended using CAMS model data), and ground-based Fourier transform infrared (FTIR) remote-sensing measurements. The average difference (in mt CH4) with respect to in situ profiles for LMD ranges between -0.3 and 10.9 ppb, while for RAL the X CH4 difference ranges between -4.6 and -1.6 ppb. The standard deviation (SD) of the observed differences between in situ measurements and RAL retrievals is 14.1–21.9 ppb, which is consistently smaller than that between LMD retrievals and in situ measurements (15.2–30.6 ppb). By comparing with ground-based FTIR sites, the mean differences are within ±10 ppb for both RAL and LMD retrievals. However, the SD of the differences at the ground-based FTIR stations shows significantly lower values for RAL (11–15 ppb) than for LMD (about 25 ppb). The long-term trend and seasonal cycles of CH4 derived from the LMD and RAL products are further investigated and discussed. The seasonal variation in X CH4 derived from RAL is consistent with the seasonal variation observed by the ground-based FTIR measurements. However, the overall 2007–2015 X CH4 trend derived from RAL measurements is underestimated, if not adjusted, for an anomaly occurring on 16 May 2013 due to a L1 calibration change. For LMD, we see very good agreement at the (sub)tropics (<35 ° N– 35° S) but notice deviations in the seasonal cycle (both in the amplitude and phase) and an underestimation of the long-term trend with respect to the RAL and reference data at higher-latitude sites. [ABSTRACT FROM AUTHOR]

The increase in greenhouse gas concentrations, particularly CO2 , has significant implications for global climate patterns and various aspects of human life. Spaceborne remote sensing satellites play a crucial role in high-resolution monitoring of atmospheric CO2. However, the next generation of greenhouse gas monitoring satellites is expected to face challenges, particularly in terms of computational efficiency in atmospheric CO2 retrieval and analysis. To address these challenges, this study focuses on improving the speed of retrieving the column-averaged dry-air mole fraction of carbon dioxide (XCO2) using spectral data from the Orbiting Carbon Observatory-2 (OCO-2) satellite while still maintaining retrieval accuracy. A novel approach based on neural network (NN) models is proposed to tackle the nonlinear inversion problems associated with XCO2 retrievals. The study employs a data-driven supervised learning method and explores two distinct training strategies. Firstly, training is conducted using experimental data obtained from the inversion of the operational optimization model, which is released as the OCO-2 satellite products. Secondly, training is performed using a simulated dataset generated by an accurate forward calculation model. The inversion performance and prediction performance of the machine learning model for XCO2 are compared, analyzed, and discussed for the observed region over east Asia. The results demonstrate that the model trained on simulated data accurately predicts XCO2 in the target area. Furthermore, when compared to OCO-2 satellite product data, the developed XCO2 retrieval model not only achieves rapid predictions (<1 ms) with good accuracy (1.8 ppm or approximately 0.45 %) but also effectively captures sudden increases in XCO2 plumes near industrial emission sources. The accuracy of the machine learning model retrieval results is validated against reliable data from Total Carbon Column Observing Network (TCCON) sites, demonstrating its ability to effectively capture CO2 seasonal variations and annual growth trends. [ABSTRACT FROM AUTHOR]

Despite the importance of understanding the urban emission characteristics of greenhouse gases (GHGs) and air pollutants, few studies have conducted integrated assessments across diverse urban environments. Herein, we conducted a comprehensive evaluation of the emission characteristics of GHGs and air pollutants in seven cities in the Northern Hemisphere using ground‐based Fourier transform spectrometers. Our analysis primarily focused on emission ratios of excess column‐averaged dry‐air mole fractions of carbon monoxide (CO) to carbon dioxide (CO2) (∆XCO:∆XCO2) and those of methane (CH4) to CO2 (∆XCH4:∆XCO2). We found that the emission ratios varied significantly across cities. Xianghe (China) and Pasadena (USA), known for severe air pollution, showed the highest emission ratios. Notably, Seoul (South Korea) showed lower ∆XCO:∆XCO2 (3.32 ± 0.10 ppb/ppm) but relatively higher ∆XCH4:∆XCO2 (4.85 ± 0.04 ppb/ppm), which was comparable to the ∆XCH4:∆XCO2 value of Xianghe (5.15 ± 0.10 ppb/ppm), suggesting that targeted CH4 reduction strategies may be required for climate change mitigation in Seoul. Plain Language Summary: Many cities experience significant greenhouse gas and air pollutant emissions. We comprehensively analyzed the characteristics of these emissions using ground‐based solar‐viewing Fourier transform spectrometers (FTSs) in Northern Hemisphere cities including Seoul (South Korea), Thessaloniki (Greece), Tsukuba (Japan), Karlsruhe (Germany), Xianghe (China), Pasadena (USA), and Paris (France). First, we focused on variations in carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO). Based on these variations, their emission ratios were estimated in terms of excess column‐averaged dry‐air mole fractions of CO to CO2 (∆XCO:∆XCO2) and CH4 to CO2 (∆XCH4:∆XCO2) in urban sites. We found that the emission ratios differed across cities. For example, Xianghe and Pasadena, which generally exhibit high levels of air pollution, had the highest emission ratios. However, Seoul had lower emission ratios of ∆XCO:∆XCO2, but higher levels of ∆XCH4:∆XCO2. This study suggests that ground‐based Fourier transform spectrometer measurements can be used as a tool for comprehensively evaluating the emission characteristics of greenhouse gases and air pollutants in urban environments. Furthermore, extending our study to longer periods and more sites could further aid in formulating effective mitigation strategies for climate change. Key Points: We comprehensively assessed the emission characteristics of greenhouse gases and air pollutants in seven cities in the Northern HemisphereGround‐based Fourier transform spectrometers offers a comprehensive analysis of the urban emission characteristics of greenhouse gases and air pollutantsOur results can further support effective strategies for mitigating climate change [ABSTRACT FROM AUTHOR]

Quantifying atmospheric CO2 over long periods from space is crucial in understanding the carbon cycle's response to climate change. However, a single satellite offers limited spatiotemporal coverage, making comprehensive monitoring challenging. Moreover, biases among various satellite retrievals hinder their direct integration. This study proposed a machine learning framework for fusing the column‐averaged dry‐air mole fraction of CO2 (XCO2) retrievals from Greenhouse Gases Observing Satellite (GOSAT) and OCO‐2 satellites. The best model (R2 = 0.85) presented improved consistency of GOSAT retrievals by reducing 71.5% of the average monthly bias while using OCO‐2 retrievals as a benchmark, indicating the fusion data set's potential to enhance observation coverage. Incorporating the adjusted GOSAT XCO2 retrievals into the OCO‐2 data set added an average of 84.7 thousand observations annually, enhancing the yearly temporal coverage by 53.6% (from 14 to 21.5 days per grid). This method can be adapted to other satellites, maximizing satellite resources for a more robust carbon flux inversion. Plain Language Summary: CO2 sources and sinks are primarily regulated by anthropogenic emissions, photosynthesis and respiration on land and in the ocean, as well as by physical dissolution and carbonate chemistry with ocean circulation. The consistent long‐term quantification of atmospheric CO2 concentrations using satellite observations plays a pivotal role in understanding the response of global and regional carbon cycles to climate change. However, satellites have a revisit period, and factors like cloud and aerosol scattering impact the quality and quantity of their observations. A single satellite currently falls short of the demand to monitor global carbon sources and sinks, necessitating the integration of observations from various satellites to conduct carbon flux inversions. Different satellites come with distinct sampling patterns, instrument parameters, and retrieval algorithms, which leads to biases in their retrieval products. Our study, focusing on OCO‐2 and GOSAT, employs machine learning models to improve consistency between retrievals derived from these two satellites, thus generating a harmonized data set. The bias‐corrected GOSAT XCO2 retrievals exhibit high spatiotemporal consistency with OCO‐2 XCO2 retrievals, immensely enhancing the observational constraints for carbon flux inversions. This method holds promise for application to recently launched and future satellites, aiming to offer carbon flux inversions with amplified spatiotemporal observational constraints. Key Points: This study employs machine learning (ML) models to enhance XCO2 consistency between OCO‐2 and Greenhouse Gases Observing Satellite (GOSAT), reducing monthly inconsistency by 71.5%Integrating the OCO‐2 data set with GOSAT retrievals increased yearly observations by 56.2%Fusing satellite data through ML models can pave the way for improved carbon flux inversions in the future [ABSTRACT FROM AUTHOR]

Propane (C3H8) is an important trace gas in the atmosphere, as it is a proxy for oil and gas production and has a significant impact on atmospheric chemical reactions related to the hydroxyl radical and tropospheric ozone formation. In this study, solar direct absorption spectra near 2967 cm−1 recorded by a ground-based Fourier Transform InfraRed spectrometer (FTIR) are applied to retrieve C3H8 total columns between June 2018 and July 2022 at Xianghe in North China. The systematic and random uncertainties of the C3H8 column retrieval are estimated to be 18.2 % and 18.1 %, respectively. The mean and standard deviation of the C3H8 columns derived from the FTIR spectra at Xianghe are 1.80±0.81(1 σ) × 1015 molecules / cm 2. Good correlations are found between C3H8 and other non-methane hydrocarbons, such as C2H6 (R=0.84) and C2H2 (R=0.79), as well as between C3H8 and CO (R=0.72). However, the correlation between C3H8 and CH4 is relatively weak (R=0.45). The FTIR C3H8 measurements are also compared against two atmospheric chemical transport model simulations (the Whole Atmosphere Community Climate Model (WACCM) and the Copernicus Atmosphere Monitoring Service (CAMS)). We find that the C3H8 columns from both models have different seasonal variations as compared to the FTIR measurements. Moreover, the mean C3H8 columns derived from the WACCM and CAMS models are about 68 % larger than the FTIR retrievals. The new FTIR measurements at Xianghe provide us an insight into the C3H8 column variations and underlying processes in North China. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) is the most important long-lived greenhouse gas and can be retrieved using solar absorption spectra recorded by a ground-based Fourier-transform infrared spectrometer (FTIR). In this study, we investigate the CO2 retrieval strategy using the Network for the Detection of Atmospheric Composition Change–Infrared Working Group (NDACC–IRWG) type spectra between August 2018 and April 2022 (~4 years) at Xianghe, China, aiming to find the optimal observed spectra, retrieval window, and spectroscopy. Two spectral regions, near 2600 and 4800 cm−1, are analyzed. The differences in column-averaged dry-air mole fraction of CO2 (XCO2) derived from spectroscopies (ATM18, ATM20, HITRAN2016, and HITRAN2020) can be up to 1.65 ± 0.95 ppm and 7.96 ± 2.02 ppm for NDACC-type 2600 cm−1 and 4800 cm−1 retrievals, respectively, which is mainly due to the CO2 differences in air-broadened Lorentzian HWHM coefficient (γair) and line intensity (S). HITRAN2020 provides the best fitting, and the retrieved CO2 columns and profiles from both 2600 and 4800 cm−1 are compared to the co-located Total Column Carbon Observing Network (TCCON) measurements and the greenhouse gas reanalysis dataset from the Copernicus Atmosphere Monitoring Service (CAMS). The amplitude of XCO2 seasonal variation derived from the NDACC-type (4800 cm−1) is closer to the TCCON measurements than that from the NDACC-type (2600 cm−1). Moreover, the NDACC-type (2600 cm−1) retrievals are strongly affected by the a priori profile. For tropospheric XCO2, the correlation coefficient between NDACC-type (4800 cm−1) and CAMS model is 0.73, which is higher than that between NDACC-type (2600 cm−1) and CAMS model (R = 0.56). [ABSTRACT FROM AUTHOR]

Atmospheric ammonia (NH3) is a chemically active trace gas that plays an important role in the atmospheric environment and climate change. Satellite remote sensing is a powerful technique to monitor NH3 concentration based on the absorption lines of NH3 in the thermal infrared region. In this study, we establish a retrieval algorithm to derive the NH3 column from the Hyperspectral Infrared Atmospheric Sounder (HIRAS) onboard the Chinese FengYun (FY)-3D satellite and present the first atmospheric NH3 column global map observed by the HIRAS instrument. The HIRAS observations can well capture NH3 hotspots around the world, e.g., India, West Africa, and East China, where large NH3 emissions exist. The HIRAS NH3 columns are also compared to the space-based Infrared Atmospheric Sounding Interferometer (IASI) measurements, and we find that the two instruments observe a consistent NH3 global distribution, with correlation coefficient (R) values of 0.28–0.73. Finally, some remaining issues about the HIRAS NH3 retrieval are discussed. [ABSTRACT FROM AUTHOR]

The joint construction of the Silk Road Economic Belt and the 21st Century Maritime Silk Road proposed by China has brought major development opportunities for the development of countries and regions along the routes. Traditional GDP statistics based on administrative units cannot describe the spatial differences of GDP within administrative units, which has certain limitations in exploring regional economic development analysis and supporting economic development decision making. Based on NPP-VIIRS luminous remote sensing data, land use data, and statistical yearbook data, this paper analyzes the spatial–temporal evolution pattern of economic level in China's coastal economic belt from 2012 to 2021 using the Moran index and standard deviation ellipse. An unbalanced distribution of economic development are found along China coastal area and the economic gravity center moved southwest since the Belt and Road Initiative. The results show thatthe Yangtze River Delta was extremely active , and the economic growth of the south was better than that of the north. The grided GDP map presents more details of regional economic development, and provides an opportunity for further mechanisms exploration of the development process. [ABSTRACT FROM AUTHOR]

The temporal variability of both surface concentrations and column abundances of CO2, CH4 and CO at the Xianghe site in China are analyzed with the Weather Research and Forecast model coupled with Chemistry (WRF-Chem). Simulations of these in situ (PICARRO) and remote sensing (TCCON-affiliated) measurements are produced by the model's passive tracer option, called WRF-GHG, from September 2018 until September 2019. Our analysis found a good model performance with correlation coefficients between observations and simulations up to 0.85 for CO2 and 0.69 for CO. Key source sectors for every gas are revealed by tracking the anthropogenic fluxes in separate tracer fields. While there are slight variations in the relative impacts of these source sectors between surface and column observations, owing to differences in the sensitivity footprint of each observation type, the primary sectors influencing the various species are evident. For CO2 the industry, energy and biosphere sectors are found to be the primary contributors to the total simulated concentration, whereas CH4 concentrations are predominantly attributed to the energy, agriculture and residential & waste sectors. For CO, industry is the largest contributing sector at Xianghe, followed by residential and transportation sources. Differences among the various observation types were particularly visible in the contributions of the biosphere to CO2 and the energy sector to CH4, as their largest sources are located further away from Xianghe. Further, the influence of meteorological factors on the variability observed in the different time series was analyzed. We found that southwest winds typically bring polluted air masses from the North China Plain to the site, while northern winds are associated with cleaner conditions. Variability in surface measurements is primarily driven by the daily cycle of accumulation and atmospheric mixing linked with the planetary boundary layer height. Furthermore, the study demonstrates the ability to detect strong regional sources at Xianghe depending on wind direction. To address inconsistencies between the simulations and observations of CH4, we looked at TROPOspheric Monitoring Instrument (TROPOMI) satellite observations. We found that the model underestimation of CH4 in summer and overestimation in winter may result from a combination of a similar bias in the lateral boundary conditions and an incorrect monthly variation of the CH4 emissions in the agriculture and/or waste sectors of the CAMS-GLOB-ANT inventory over north China. Additionally, WRF-GHG simulations indicated a possible overestimation of coal mine emissions nearby Tangshan, which could not be confirmed nor contradicted by the TROPOMI observations. In summary, our findings highlight the value of WRF-GHG to interpret both surface and column observations at Xianghe, offering source sector attribution and insights in the link with local and large-scale winds based on the simultaneously computed meteorological fields. However, given the long lifetime of the considered species and the fact that WRF-GHG is a regional model, accurate initial and lateral boundary conditions remain crucial. The dependence on precise input emission data on the other hand, can be used to evaluate the existing bottom-up inventories. [ABSTRACT FROM AUTHOR]

Nitrous oxide (N2O) and methane (CH4) are two important greenhouse gases in the atmosphere. In 2019, mid-infrared (MIR) solar absorption spectra were recorded by a Bruker VERTEX 70 spectrometer and a Bruker IFS 125HR spectrometer at Sodankylä, Finland, at spectral resolutions of 0.2 and 0.005 cm-1 , respectively. The N2O and the CH4 retrievals from high-resolution MIR spectra have been well investigated within the Network for the Detection of Atmospheric Composition Change (NDACC) but not for MIR spectra gathered with instruments operating at low spectral resolution. In this study, N2O and CH4 retrieval strategies and retrieval uncertainties from the VERTEX 70 MIR low-resolution spectra are discussed and presented. The accuracy and precision of the VERTEX 70 N2O and CH4 retrievals are assessed by comparing them with the coincident 125HR retrievals and AirCore measurements. The relative differences between the N2O total columns retrieved from 125HR and VERTEX 70 spectra are - 0.3 ± 0.7 (1 σ) % with a correlation coefficient (R) of 0.93. Regarding the CH4 total column, we first used the same retrieval microwindows for 125HR and VERTEX 70 spectra, but there is an underestimation in the VERTEX 70 retrievals, especially in summer. The relative differences between the CH4 total columns retrieved from the 125HR and VERTEX 70 spectra are -1.3±1.1 (1 σ) % with a R value of 0.77. To improve the VERTEX 70 CH4 retrievals, we propose alternative retrieval microwindows. The relative differences between the CH4 total columns retrieved from the 125HR and VERTEX 70 spectra in these new windows become 0.0±0.8 (1 σ) %, along with an increase in the R value to 0.87. The coincident AirCore measurements confirm that the VERTEX 70 CH4 retrievals using the latter window choice are better, with relative mean differences between the VERTEX 70 CH4 retrievals and AirCore measurements of - 1.9 % for the standard NDACC microwindows and of 0.13 % for the alternative microwindows. This study provides insight into the N2O and CH4 retrievals from the low-resolution (0.2 cm-1) MIR spectra observed with a VERTEX 70 spectrometer, and it demonstrates the suitability of this kind of instrument for contributing to satellite validation, model verification, and other scientific campaigns with the advantage of its transportability and lower cost compared to standard NDACC-type Fourier-transform infrared (FTIR) instruments. [ABSTRACT FROM AUTHOR]

TanSat-2, the next-generation Chinese greenhouse gas monitoring satellite for measuring carbon dioxide (CO 2 ), has a new city-scale observing mode. We assess the theoretical capability of TanSat-2 to quantify integrated urban CO 2 emissions over the cities of Beijing, Jinan, Los Angeles, and Paris. A high-resolution emission inventory and a column-averaged CO 2 ( X CO 2 ) transport model are used to build an urban CO 2 inversion system. We design a series of numerical experiments describing this observing system to evaluate the impacts of sampling patterns and X CO 2 measurement errors on inferring urban CO 2 emissions. We find that the correction in systematic and random flux errors is correlated with the signal-to-noise ratio of satellite measurements. The reduction in systematic flux errors for the four cities are sizable, but are subject to unbiased satellite sampling and favorable meteorological conditions (i.e., less cloud cover and lower wind speed). The corresponding correction to the random flux error is 19–28%. Even though clear-sky satellite data from TanSat-2 have the potential to reduce flux errors for cities with high CO 2 emissions, quantifying urban emissions by satellite-based measurements is subject to additional limitations and uncertainties. [ABSTRACT FROM AUTHOR]

Methane (CH4) is an important greenhouse as well as a chemically active gas. Accurate monitoring and understanding of its spatiotemporal distribution are crucial for effective mitigation strategies. Nowadays, satellite measurements are widely used for CH4 studies. Here, we use the CH4 products from four commonly used satellites (GOSAT, TROPOMI, ARIS, and IASI) during the period from 2018 to 2020 to investigate the spatiotemporal variations of CH4 in China. In spite of the same target (CH4) for the four satellites, differences among them exist in terms of the instrument, spectrum, and retrieval algorithm. The GOSAT and TROPOMI CH4 retrievals use shortwave infrared spectra, with a better sensitivity near the surface, while the IASI and AIRS CH4 retrievals use thermal infrared spectra, showing a good sensitivity in the mid–upper troposphere but a weak sensitivity in the lower troposphere. The GOSAT and TROPOMI observe high CH4 concentrations in the east and south and low concentrations in the west and north, which is highly related to the CH4 emissions. The IASI and AIRS show a more uniform CH4 distribution over China, which reflects the variation of CH4 at a high altitude. However, a large discrepancy is observed between the IASI and AIRS despite using a similar retrieval band, e.g., significant differences in the seasonal variations of CH4 are observed between the IASI and AIRS across several regions in China. This study highlights the CH4 differences observed by the four satellites in China, and caution must be taken when using these satellite products. [ABSTRACT FROM AUTHOR]

We apply atmospheric methane column retrievals from two different satellite instruments (Greenhouse gases Observing SATellite – GOSAT; TROPOspheric Monitoring Instrument – TROPOMI) to a regional inversion framework to quantify East Asian methane emissions for 2019 at 0.5 ∘ × 0.625 ∘ horizontal resolution. The goal is to assess if GOSAT (relatively mature but sparse) and TROPOMI (new and dense) observations inform consistent methane emissions from East Asia with identically configured inversions. Comparison of the results from the two inversions shows similar correction patterns to the prior inventory in central northern China, central southern China, northeastern China, and Bangladesh, with less than 2.6 Tg a -1 differences in regional posterior emissions. The two inversions, however, disagree over some important regions, particularly in northern India and eastern China. The methane emissions inferred from GOSAT observations are 7.7 Tg a -1 higher than those from TROPOMI observations over northern India but 6.4 Tg a -1 lower over eastern China. The discrepancies between the two inversions are robust against varied inversion configurations (i.e., assimilation window and error specifications). We find that the lower methane emissions from eastern China inferred by the GOSAT inversion are more consistent with independent ground-based in situ and total column (TCCON) observations, indicating that the TROPOMI retrievals may have high XCH 4 biases in this region. We also evaluate inversion results against tropospheric aircraft observations over India during 2012–2014 by using a consistent GOSAT inversion of earlier years as an intercomparison platform. This indirect evaluation favors lower methane emissions from northern India inferred by the TROPOMI inversion. We find that in this case the discrepancy in emission inference is contributed by differences in data coverage (almost no observations by GOSAT vs. good spatial coverage by TROPOMI) over the Indo-Gangetic Plain. The two inversions also differ substantially in their posterior estimates for northwestern China and neighboring Kazakhstan, which is mainly due to seasonally varying biases between GOSAT and TROPOMI XCH 4 data that correlate with changes in surface albedo. [ABSTRACT FROM AUTHOR]

The National Institute for Environmental Studies has provided the column-averaged dry-air mole fraction of carbon dioxide and methane (XCO 2 and XCH 4) products (L2 products) obtained from the Greenhouse gases Observing SATellite (GOSAT) for more than a decade. Recently, we updated the retrieval algorithm used to produce the new L2 product, V03.00. The main changes from the previous version (V02) of the retrieval algorithm are the treatment of cirrus clouds, the degradation model of the Thermal And Near-infrared Spectrometer for carbon Observation–Fourier Transform Spectrometer (TANSO–FTS), solar irradiance spectra, and gas absorption coefficient tables. The retrieval results from the updated algorithm showed improvements in fitting accuracies in the O 2 A, weak CO 2 , and CH 4 bands of TANSO–FTS, although the residuals increase in the strong CO 2 band over the ocean. The direct comparison of the new product obtained from the updated (V03) algorithm with the previous version V02.90/91 and the validations using the Total Carbon Column Observing Network revealed that the V03 algorithm increases the amount of data without diminishing the data qualities of XCO 2 and XCH 4 over land. However, the negative bias of XCO 2 is larger than that of the previous version over the ocean, and bias correction is still necessary. Additionally, the V03 algorithm resolves the underestimation of the XCO 2 growth rate compared with the in situ measurements over the ocean recently found using V02.90/91 and V02.95/96. [ABSTRACT FROM AUTHOR]

Measurements of carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) are of great importance in the Qinghai-Tibetan region, as it is the highest and largest plateau in the world affecting global weather and climate systems. In this study, for the first time, we present CO2, CH4, and CO column measurements carried out by a Bruker EM27/SUN Fourier-transform infrared spectrometer (FTIR) at Golmud (36.42°E, 94.91°N, 2808 m) in August 2021. The mean and standard deviation of the column-average dry-air mixing ratio of CO2, CH4, and CO (XCO2, XCH4, and XCO) are 409.3 ± 0.4 ppm, 1905.5 ± 19.4 ppb, and 103.1 ± 7.7 ppb, respectively. The differences between the FTIR co-located TROPOMI/S5P satellite measurements at Golmud are 0.68 ± 0.64% (13.1 ± 12.2 ppb) for XCH4 and 9.81 ± 3.48% (−10.7 ± 3.8 ppb) for XCO, which are within their retrieval uncertainties. High correlations for both XCH4 and XCO are observed between the FTIR and S5P satellite measurements. Using the FLEXPART model and satellite measurements, we find that enhanced CH4 and CO columns in Golmud are affected by anthropogenic emissions transported from North India. This study provides an insight into the variations of the CO2, CH4, and CO columns in the Qinghai-Tibetan Plateau. [ABSTRACT FROM AUTHOR]

Carbon monoxide (CO), acetylene (C 2 H 2), ethane (C 2 H 6), formaldehyde (H 2 CO), and hydrogen cyanide (HCN) are important trace gases in the atmosphere. They are highly related to biomass burning, fossil fuel combustion, and biogenic emissions globally, affecting air quality and climate change. However, the variations and correlations among these species are not well known in northern China due to limited measurements. In June 2018, we installed a new ground-based Fourier transform infrared (FTIR) spectrometer (Bruker IFS 125HR) recording mid-infrared high spectral resolution solar-absorption spectra at Xianghe (39.75 ∘ N, 116.96 ∘ E), China. In this study, we use the latest SFIT4 code, together with advanced a priori profiling and spectroscopy, to retrieve these five species from the FTIR spectra measured between June 2018 and November 2021. The retrieval strategies, retrieval information and retrieval uncertainties are presented and discussed. For the first time, the time series, variations, and correlations of these five species are analyzed at a typical polluted site in northern China. The seasonal variations in C 2 H 2 and C 2 H 6 total columns show a maximum in winter–spring and a minimum in autumn, whereas the seasonal variations in H 2 CO and HCN show a maximum in summer and a minimum in winter. Unlike the other four species, the FTIR measurements show that there is almost no seasonal variation in the CO column. The correlation coefficients (R) between the synoptic variations in CO and the other four species (C 2 H 2 , C 2 H 6 , H 2 CO, and HCN) are between 0.68 and 0.80, indicating that they are affected by common sources. Using the FLEXPART model backward simulations and satellite fire measurements, we find that the variations in CO, C 2 H 2 , C 2 H 6 , and H 2 CO columns are mainly dominated by the local anthropogenic emissions, while HCN column observed at Xianghe is a good tracer to identify fire emissions. [ABSTRACT FROM AUTHOR]

Synthetic halogenated organic chlorofluorocarbons (CFCs) play an important role in stratospheric ozone depletion and contribute significantly to the greenhouse effect. In this work, the mid-infrared solar spectra measured by ground-based high-resolution Fourier transform infrared spectroscopy (FTIR) were used to retrieve atmospheric CFC-11 (CCl 3 F) and CFC-12 (CCl 2 F 2) at Hefei, China. The CFC-11 columns observed from January 2017 to December 2020 and CFC-12 columns from September 2015 to December 2020 show a similar annual decreasing trend and seasonal cycle, with an annual rate of -0.47±0.06 % yr -1 and -0.68±0.03 % yr -1 , respectively. So the decline rate of CFC-11 is significantly lower than that of CFC-12. CFC-11 total columns were higher in summer, and CFC-12 total columns were higher in summer and autumn. Both CFC-11 and CFC-12 total columns reached the lowest in spring. Further, FTIR data of NDACC (Network for the Detection of Atmospheric Composition Change) candidate station Hefei were compared with the ACE-FTS (Atmospheric Chemistry Experiment Fourier transform spectrometer) satellite data, WACCM (Whole Atmosphere Community Climate Model) data, and the data from other NDACC-IRWG (InfraRed Working Group) stations (St. Petersburg, Jungfraujoch, and Réunion). The mean relative difference between the vertical profiles observed by FTIR and ACE-FTS is -5.6±3.3 % and 4.8±0.9 % for CFC-11 and CFC-12 for an altitude of 5.5 to 17.5 km, respectively. The results demonstrate that our FTIR data agree relatively well with the ACE-FTS satellite data. The annual decreasing rate of CFC-11 measured from ACE-FTS and calculated by WACCM is -1.15±0.22 % yr -1 and -1.68±0.18 % yr -1 , respectively. The interannual decreasing rates of atmospheric CFC-11 obtained from ACE-FTS and WACCM data are higher than that from FTIR observations. Also, the annual decreasing rate of CFC-12 from ACE-FTS and WACCM is -0.85±0.15 % yr -1 and -0.81±0.05 % yr -1 , respectively, close to the corresponding values from the FTIR measurements. The total columns of CFC-11 and CFC-12 at the Hefei and St. Petersburg stations are significantly higher than those at the Jungfraujoch and Réunion (Maïdo) stations, and the two values reached the maximum in local summer or autumn and the minimum in local spring or winter at the four stations. The seasonal variability at the three stations in the Northern Hemisphere is higher than that at the station in the Southern Hemisphere. [ABSTRACT FROM AUTHOR]

Since its launch on 13 October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor (S5P) mission has been measuring the solar radiation backscattered by Earth's atmosphere and surface. In this study, we evaluate the TROPOMI operational methane (CH4) and carbon monoxide (CO) products' performance results covering about 3 years using the only two global Total Carbon Column Observing Network (TCCON) sites in China, i.e., the Hefei site and the Xianghe site. These two sites have recently joined the TCCON, and this study uses the both sites simultaneously to validate the TROPOMI products over China for the first time. We found that the systematic bias with rescaling between the TROPOMI CO products and the Hefei site is on average 1.78 ± 6.35 ppb or 1.18 ± 5.35%. The systematic bias with rescaling between the TROPOMI CO products and the Xianghe site is on average 5.33 ± 14.24 ppb or 3.85 ± 10.30%. Both the stations show a correlation above 0.9. The TROPOMI CO data are systematically higher than the two TCCON sites measurements in China. We found that the systematic bias with rescaling between the TROPOMI CH4 products and the Hefei site is on average −4.13 ± 11.65 ppb or −0.22 ± 0.62%. The systematic bias between the TROPOMI CH4 products and Xianghe site is on average −7.25 ± 10.72 ppb or −0.39 ± 0.57%. Both the stations show a correlation above 0.9. The TROPOMI CH4 data are systematically lower than the two TCCON sites measurements in China. We found that the bias between the TROPOMI and the two sites' data as a function of the coincident radius around the two sites is mostly affected by localized emissions for both CO and CH4. We also observe a CO decreasing trend and a CH4 increasing trend in the year-to-year relative changes from 2019 to 2021. Validating against reference from Hefei and Xianghe TCCON site demonstrates the high quality of TROPOMI CO and CH4 data over China. [ABSTRACT FROM AUTHOR]

Carbon monoxide (CO), acetylene (C2H2), ethane (C2H6), formaldehyde (H2CO), and hydrogen cyanide (HCN) are important trace gases in the atmosphere. They are highly related to biomass burning, fossil fuel combustion, and biogenic emissions globally, affecting air quality and climate change. However, the variations and correlations among these species are not well known in North China, due to limited measurements. In June 2018, we installed a new ground-based Fourier-transform infrared (FTIR) spectrometer (Bruker IFS 125HR) recording mid-infrared high spectral resolution solar-absorption spectra at Xianghe (39.75° N, 116.96° E), China. In this study, we use the latest SFIT4 code, together with advanced a priori profile and spectroscopy, to retrieve these five species from the FTIR spectra measured between June 2018 and November 2021. The retrieval strategies, retrieval information, and retrieval uncertainties are presented and discussed. For the first time, the time series, variations, and correlations of these five species are analyzed at a typical polluted site in North China. The seasonal variations of C2H2 and C2H6 total columns show a maximum in winter-spring and a minimum in autumn, whereas the seasonal variations of H2CO and HCN show a maximum in summer and a minimum in winter. Unlike the other four species, the FTIR measurements show that there is almost no seasonal variation in the CO column. The correlation coefficients (R) between the synoptic variations of CO and the other four species (C2H2, C2H6, H2CO, and HCN) are between 0.68 and 0.80, indicating that they are affected by common sources. Using the FLEXPART model backward simulations and satellite fire measurements, we find that the variations of CO, C2H2, C2H6, and H2CO columns are mainly dominated by the local anthropogenic emissions, while HCN column observed at Xianghe is a good tracer to identify fire emissions. [ABSTRACT FROM AUTHOR]

Monitoring the atmospheric CO 2 columns inside and around a city is of great importance to understand the temporal–spatial variation of XCO 2 near strong anthropogenic emissions. In this study, we use two FTIR CO 2 column measurements in Beijing (Bruker EM27/SUN) and Xianghe (Bruker IFS 125HR) between 2019 and 2021 to investigate the differences of XCO 2 between Beijing (urban) and Xianghe (suburb) in North China and to validate the OCO-2 and OCO-3 satellite XCO 2 retrievals. The mean and standard deviation (std) of the Δ XCO 2 between Beijing and Xianghe (Beijing–Xianghe) observed by two FTIR instruments are 0.206 ± 1.736 ppm, which has a seasonal variation and varies with meteorological conditions (wind speed and wind direction). The mean and std of the XCO 2 differences between co-located satellite and FTIR measurements are −0.216 ± 1.578 ppm in Beijing and −0.343 ± 1.438 ppm in Xianghe for OCO-2 and 0.637 ± 1.594 ppm in Beijing and 1.206 ± 1.420 ppm in Xianghe for OCO-3. It is found that the OCO-3 snapshot area mode (SAM) measurements can capture the spatial gradient of XCO 2 between urban and suburbs well. However, the FTIR measurements indicate that the OCO-3 SAM measurements are about 0.9–1.4 ppm overestimated in Beijing and Xianghe. [ABSTRACT FROM AUTHOR]

Nitric oxide (NO) is a key active trace gas in the atmosphere, which contributes to form harmful ozone in the troposphere and to the destruction of ozone in the stratosphere. In this study, we present the NO retrieval from ground-based Fourier-transform infrared (FTIR) solar absorption spectrometry measurements at a polluted site (Xianghe, China) and a background site (Maïdo, Reunion Island). The degree of freedom (DOF) of the NO retrieval is 2.3±0.4 (1σ) at Xianghe and 1.3±0.1 at Maïdo. By looking at the FTIR NO retrievals at Xianghe and Maïdo, we find that the stratospheric NO partial column is large in summer as compared to winter at both sites, and the seasonal variation in the FTIR stratospheric NO partial columns is consistent with that observed by the co-located Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite measurements. A large diurnal variation in the stratospheric NO partial column is observed by the FTIR measurements at Maïdo, with an increase from the early morning to about 14:00 local time and a decrease thereafter. Due to the low NO concentration near the surface, the FTIR NO retrieval is only sensitive to the stratosphere at Maïdo. The high NO mole fraction near the surface at Xianghe allows us to derive tropospheric and stratospheric NO partial columns separately, although the tropospheric column is very difficult to retrieve in summer (June–August) because of the high water vapor abundance. A good correlation is found between the NO observed by the FTIR measurements and other air pollutants (NO2 and CO) in the troposphere at Xianghe. It is the first study of a successful analysis of NO in the troposphere from a ground-based FTIR site. The tropospheric and stratospheric NO retrieval might be possible at other potential FTIR sites inside or near large cities with enhanced levels of NO near the surface. [ABSTRACT FROM AUTHOR]

Atmospheric CO2 mole fractions are observed at Beijing (BJ), Xianghe (XH), and Xinglong (XL) in North China using Picarro G2301 cavity ring-down spectroscopy instruments. The measurement system is described comprehensively for the first time. The geographical distances among these three sites are within 200 km , but they have very different surrounding environments: BJ is inside the megacity; XH is in the suburban area; XL is in the countryside on a mountain. The mean and standard deviation of CO2 mole fractions at BJ, XH, and XL between October 2018 and September 2019 are 448.4±12.8 , 436.0±9.2 , and 420.6±8.2 ppm , respectively. The seasonal variations of CO2 at these three sites are similar, with a maximum in winter and a minimum in summer, which is dominated by the terrestrial ecosystem. However, the seasonal variations of CO2 at BJ and XH are more affected by human activities as compared to XL. Using CO2 at XL as the background, CO2 enhancements are observed simultaneously at BJ and XH. The diurnal variations of CO2 are driven by the boundary layer height, photosynthesis, and human activities at BJ, XH, and XL. We also compare the CO2 measurements at BJ, XH, and XL with five urban sites in the USA, and it is found that the CO2 mean concentration at BJ is the largest. Moreover, we address the impact of the wind on the CO2 mole fractions at BJ and XL. This study provides an insight into the spatial and temporal variations of CO2 mole fractions in North China. [ABSTRACT FROM AUTHOR]

In this study, we present O3 retrievals from ground-based Fourier transform infrared (FTIR) solar absorption measurements between June 2018 and December 2019 at Xianghe, China (39.75 ∘ N, 116.96 ∘ E). The FTIR spectrometer at Xianghe is operated with indium gallium arsenide (InGaAs) and indium antimonide (InSb) detectors, recording the spectra between 1800 and 11 000 cm -1. As the harmonized FTIR O3 retrieval strategy within the Network for the Detection of Atmospheric Composition Change (NDACC) uses the 1000 cm -1 spectral range, we apply the O3 retrieval in the 3040 cm -1 spectral range at Xianghe. The retrieved O3 profile is mainly sensitive to the vertical range between 10 and 40 km, and the degrees of freedom for signal is 2.4±0.3 (1σ), indicating that there are two individual pieces of information in partial columns between the surface and 20 km and between 20 and 40 km. According to the optimal estimation method, the systematic and random uncertainties of the FTIR O3 total columns are about 13.6 % and 1.4 %, respectively. The random uncertainty is consistent with the observed daily standard deviation of the FTIR retrievals. To validate the FTIR O3 total and partial columns, we apply the same O3 retrieval strategy at Maïdo, Réunion (a.k.a. Reunion Island; 21.08 ∘ N, 55.38 ∘ E). The FTIR O3 (3040 cm -1) measurements at Xianghe and Maïdo are then compared with the nearby ozonesondes at Beijing (39.81 ∘ N, 116.47 ∘ E) and at Gillot (20.89 ∘ S, 55.53 ∘ E), respectively, as well as with co-located TROPOspheric Monitoring Instrument (TROPOMI) satellite measurements at both sites. In addition at Maïdo, we compare the FTIR O3 (3040 cm -1) retrievals with the standard NDACC FTIR O3 measurements using the 1000 cm -1 spectral range. It was found that the total columns retrieved from the FTIR O3 3040 cm -1 measurements are underestimated by 5.5 %–9.0 %, which is mainly due to the systematic uncertainty in the partial column between 20 and 40 km (about -10.4 %). The systematic uncertainty in the partial column between surface and 20 km is relatively small (within 2.4 %). By comparison with other measurements, it was found that the FTIR O3 (3040 cm -1) retrievals capture the seasonal and synoptic variations of the O3 total and two partial columns very well. Therefore, the ongoing FTIR measurements at Xianghe can provide useful information on the O3 variations and (in the future) long-term trends. [ABSTRACT FROM AUTHOR]

The column-averaged dry-air mole fractions of CO2 (XCO2), CH4 (XCH4) and CO (XCO) have been measured with a Bruker IFS 125HR Fourier-transform infrared (FTIR) spectrometer at Xianghe (39.75 ∘ N, 116.96 ∘ E, north China) since June 2018. This paper presents the site, the characteristics of the FTIR system and the measurements. The instrumental setup follows the guidelines of the Total Carbon Column Observing Network (TCCON): the near-infrared spectra are recorded by an InGaAs detector together with a CaF2 beam splitter, and the HCl cell measurements are recorded regularly to derive the instrument line shape (ILS) showing that the instrument is correctly aligned. The TCCON standard retrieval code (GGG2014) is applied to retrieve XCO2 , XCH4 and XCO. The resulting time series between June 2018 and July 2019 are presented, and the observed seasonal cycles and day-to-day variations in XCO2 , XCH4 and XCO at Xianghe are discussed. In addition, the paper shows comparisons between the data products retrieved from the FTIR measurements at Xianghe and co-located Orbiting Carbon Observatory-2 (OCO-2) and Tropospheric Monitoring Instrument (TROPOMI) satellite observations. The comparison results appear consistent with validation results obtained at TCCON sites for XCO2 and XCH4 , while for XCO they highlight the occurrence of frequent high-pollution events. As Xianghe lies in a polluted area in north China where there are currently no TCCON sites, this site can fill the TCCON gap in this region and expand the global coverage of the TCCON measurements. The Xianghe FTIR XCO2 , XCH4 and XCO data can be obtained at 10.18758/71021049. [ABSTRACT FROM AUTHOR]

The Total Carbon Column Observing Network (TCCON) column-averaged dry air mole fraction of CH4 (XCH4) measurements have been widely used to validate satellite observations and to estimate model simulations. The GGG2014 code is the standard TCCON retrieval software used in performing a profile scaling retrieval. In order to obtain several vertical pieces of information in addition to the total column, in this study, the SFIT4 retrieval code is applied to retrieve the CH4 mole fraction vertical profile from the Fourier transform spectrometer (FTS) spectrum at six sites (Ny-Ålesund, Sodankylä, Bialystok, Bremen, Orléans and St Denis) during the time period of 2016–2017. The retrieval strategy of the CH4 profile retrieval from ground-based FTS near-infrared (NIR) spectra using the SFIT4 code (SFIT4NIR) is investigated. The degree of freedom for signal (DOFS) of the SFIT4NIR retrieval is about 2.4, with two distinct pieces of information in the troposphere and in the stratosphere. The averaging kernel and error budget of the SFIT4NIR retrieval are presented. The data accuracy and precision of the SFIT4NIR retrievals, including the total column and two partial columns (in the troposphere and stratosphere), are estimated by TCCON standard retrievals, ground-based in situ measurements, Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) satellite observations, TCCON proxy data and AirCore and aircraft measurements. By comparison against TCCON standard retrievals, it is found that the retrieval uncertainty of SFIT4NIR XCH4 is similar to that of TCCON standard retrievals with systematic uncertainty within 0.35 % and random uncertainty of about 0.5 %. The tropospheric and stratospheric XCH4 from SFIT4NIR retrievals are assessed by comparison with AirCore and aircraft measurements, and there is a 1.0 ± 0.3 % overestimation in the SFIT4NIR tropospheric XCH4 and a 4.0 ± 2.0 % underestimation in the SFIT4NIR stratospheric XCH4 , which are within the systematic uncertainties of SFIT4NIR-retrieved partial columns in the troposphere and stratosphere respectively. [ABSTRACT FROM AUTHOR]

Column-averaged dry-air mole fraction of CO (X CO) measurements are obtained from two ground-based Fourier transform infrared (FTIR) spectrometer networks: the Total Carbon Column Observing Network (TCCON) and the Network for the Detection of Atmospheric Composition Change (NDACC). In this study, the differences between the TCCON and NDACC X CO measurements are investigated and discussed based on six NDACC–TCCON sites using data over the period 2007–2017. A direct comparison shows that the NDACC X CO measurements are about 5.5 % larger than the TCCON data at Ny-Ålesund, Bremen, and Izaña (Northern Hemisphere), and the absolute bias between the NDACC and TCCON data is within 2 % at Saint-Denis, Wollongong and Lauder (Southern Hemisphere). The hemispheric dependence of the bias is mainly attributed to their smoothing errors. The systematic smoothing error of the TCCON X CO data varies in the range between 0.2 % (Bremen) and 7.9 % (Lauder), and the random smoothing error varies in the range between 2.0 % and 3.6 %. The systematic smoothing error of NDACC data is between 0.1 % and 0.8 %, and the random smoothing error of NDACC data is about 0.3 %. For TCCON data, the smoothing error is significant because it is higher than the reported uncertainty, particularly at Southern Hemisphere sites. To reduce the influence from the a priori profiles and different vertical sensitivities, the scaled NDACC a priori profiles are used as the common a priori profiles for comparing TCCON and NDACC retrievals. As a result, the biases between TCCON and NDACC X CO measurements become more consistent (5.6 %–8.5 %) with a mean value of 6.8 % at these sites. To determine the sources of the remaining bias, regular AirCore measurements at Orléans and Sodankylä are compared to co-located TCCON measurements. It is found that TCCON X CO measurements are 6.1 ± 1.6 % and 8.0 ± 3.2 % smaller than the AirCore measurements at Orléans and Sodankylä, respectively, indicating that the scaling factor of TCCON X CO data should be around 1.0000 instead of 1.0672. Further investigations should be carried out in the TCCON community to determine the correct scaling factor to be applied to the TCCON X CO data. This paper also demonstrates that the smoothing error must be taken into account when comparing FTIR X CO data, and especially TCCON X CO data, with model or satellite data. [ABSTRACT FROM AUTHOR]

Nitrous oxide (N2O) is an important greenhouse gas and it can also generate nitric oxide, which depletes ozone in the stratosphere. It is a common target species of ground-based Fourier transform infrared (FTIR) near-infrared (TCCON) and mid-infrared (NDACC) measurements. Both TCCON and NDACC networks provide a long-term global distribution of atmospheric N2O mole fraction. In this study, the dry-air column-averaged mole fractions of N2O (XN2O) from the TCCON and NDACC measurements are compared against each other at seven sites around the world (Ny-Ålesund, Sodankylä, Bremen, Izaña, Réunion, Wollongong, Lauder) in the time period of 2007–2017. The mean differences in XN2O between TCCON and NDACC (NDACC–TCCON) at these sites are between -3.32 and 1.37 ppb (-1.1 %–0.5 %) with standard deviations between 1.69 and 5.01 ppb (0.5 %–1.6 %), which are within the uncertainties of the two datasets. The NDACC N2O retrieval has good sensitivity throughout the troposphere and stratosphere, while the TCCON retrieval underestimates a deviation from the a priori in the troposphere and overestimates it in the stratosphere. As a result, the TCCON XN2O measurement is strongly affected by its a priori profile. Trends and seasonal cycles of XN2O are derived from the TCCON and NDACC measurements and the nearby surface flask sample measurements and compared with the results from GEOS-Chem model a priori and a posteriori simulations. The trends and seasonal cycles from FTIR measurement at Ny-Ålesund and Sodankylä are strongly affected by the polar winter and the polar vortex. The a posteriori N2O fluxes in the model are optimized based on surface N2O measurements with a 4D-Var inversion method. The XN2O trends from the GEOS-Chem a posteriori simulation (0.97±0.02 (1σ) ppb yr -1) are close to those from the NDACC (0.93±0.04 ppb yr -1) and the surface flask sample measurements (0.93±0.02 ppb yr -1). The XN2O trend from the TCCON measurements is slightly lower (0.81±0.04 ppb yr -1) due to the underestimation of the trend in TCCON a priori simulation. The XN2O trends from the GEOS-Chem a priori simulation are about 1.25 ppb yr -1 , and our study confirms that the N2O fluxes from the a priori inventories are overestimated. The seasonal cycles of XN2O from the FTIR measurements and the model simulations are close to each other in the Northern Hemisphere with a maximum in August–October and a minimum in February–April. However, in the Southern Hemisphere, the modeled XN2O values show a minimum in February–April while the FTIR XN2O retrievals show different patterns. By comparing the partial column-averaged N2O from the model and NDACC for three vertical ranges (surface–8, 8–17, 17–50 km), we find that the discrepancy in the XN2O seasonal cycle between the model simulations and the FTIR measurements in the Southern Hemisphere is mainly due to their stratospheric differences. [ABSTRACT FROM AUTHOR]

The seasonal evolution of O3 and its photochemical production regime in a polluted region of eastern China between 2014 and 2017 has been investigated using observations. We used tropospheric ozone (O3), carbon monoxide (CO), and formaldehyde (HCHO, a marker of VOCs (volatile organic compounds)) partial columns derived from high-resolution Fourier transform spectrometry (FTS); tropospheric nitrogen dioxide (NO2, a marker of NOx (nitrogen oxides)) partial column deduced from the Ozone Monitoring Instrument (OMI); surface meteorological data; and a back trajectory cluster analysis technique. A broad O3 maximum during both spring and summer (MAM/JJA) is observed; the day-to-day variations in MAM/JJA are generally larger than those in autumn and winter (SON/DJF). Tropospheric O3 columns in June are 1.55 x 1018 molecules cm-2 (56DU (Dobson units)), and in December they are 1.05 x 1018 molecules cm-2 (39 DU). Tropospheric O3 columns in June were *** 50% higher than those in December. Compared with the SON/DJF season, the observed tropospheric O3 levels in MAM/JJA are more influenced by the transport of air masses from densely populated and industrialized areas, and the high O3 level and variability in MAM/JJA is determined by the photochemical O3 production. The tropospheric-column HCHO/NO2 ratio is used as a proxy to investigate the photochemical O3 production rate (PO3). The results show that the PO3 is mainly nitrogen oxide (NOx) limited in MAM/JJA, while it is mainly VOC or mixed VOC--NOx limited in SON/DJF. Statistics show that NOx-limited, mixed VOC--NOx-limited, and VOC-limited PO3 accounts for 60.1 %, 28.7 %, and 11% of days, respectively. Considering most of PO3 is NOx limited or mixed VOC--NOx limited, reductions in NOx would reduce O3 pollution in eastern China. [ABSTRACT FROM AUTHOR]

Atmospheric carbon monoxide (CO) and methane (CH4) mole fractions are measured by ground-based in situ cavity ring-down spectroscopy (CRDS) analyzers and Fourier transform infrared (FTIR) spectrometers at two sites (St Denis and Maïdo) on Reunion Island (21° S, 55° E) in the Indian Ocean. Currently, the FTIR Bruker IFS 125HR at St Denis records the direct solar spectra in the near-infrared range, contributing to the Total Carbon Column Observing Network (TCCON). The FTIR Bruker IFS 125HR at Maïdo records the direct solar spectra in the mid-infrared (MIR) range, contributing to the Network for the Detection of Atmospheric Composition Change (NDACC). In order to understand the atmospheric CO and CH4 variability on Reunion Island, the time series and seasonal cycles of CO and CH4 from in situ and FTIR (NDACC and TCCON) measurements are analyzed. Meanwhile, the difference between the in situ and FTIR measurements are discussed. The CO seasonal cycles observed from the in situ measurements at Maïdo and FTIR retrievals at both St Denis and Maïdo are in good agreement with a peak in September-November, primarily driven by the emissions from biomass burning in Africa and South America. The dry-air column averaged mole fraction of CO (XCO) derived from the FTIR MIR spectra (NDACC) is about 15.7 ppb larger than the CO mole fraction near the surface at Maïdo, because the air in the lower troposphere mainly comes from the Indian Ocean while the air in the middle and upper troposphere mainly comes from Africa and South America. The trend for CO on Reunion Island is unclear during the 2011-2017 period, and more data need to be collected to get a robust result. A very good agreement is observed in the tropospheric and stratospheric CH4 seasonal cycles between FTIR (NDACC and TCCON) measurements, and in situ and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite measurements, respectively. In the troposphere, the CH4 mole fraction is high in August-September and low in December-January, which is due to the OH seasonal variation. In the stratosphere, the CH4 mole fraction has its maximum in March-April and its minimum in August-October, which is dominated by vertical transport. In addition, the different CH4 mole fractions between the in situ, NDACC and TCCON CH4 measurements in the troposphere are discussed, and all measurements are in good agreement with the GEOS-Chem model simulation. The trend of XCH4 is 7.6±0.4 ppb yr-1 from the TCCON measurements over the 2011 to 2017 time period, which is consistent with the CH4 trend of 7.4±0.5 ppb yr-1 from the in situ measurements for the same time period at St Denis. [ABSTRACT FROM AUTHOR]

SF6 total columns were successfully retrieved from FTIR (Fourier transform infrared) measurements (Saint Denis and Maïdo) on Reunion Island (21° S, 55° E) between 2004 and 2016 using the SFIT4 algorithm: the retrieval strategy and the error budget were presented. The FTIR SF6 retrieval has independent information in only one individual layer, covering the whole of the troposphere and the lower stratosphere. The trend in SF6 was analysed based on the FTIR-retrieved dry-air column-averaged mole fractions (XSF6) on Reunion Island, the in situ measurements at America Samoa (SMO) and the collocated satellite measurements (Michelson Interferometer for Passive Atmospheric Sounding, MIPAS, and Atmospheric Chemistry Experiment Fourier Transform Spectrometer, ACE-FTS) in the southern tropics. The SF6 annual growth rate from FTIR retrievals is 0.265 ± 0.013 pptv year-1 for 2004-2016, which is slightly weaker than that from the SMO in situ measurements (0.285 ± 0.002 pptv year-1) for the same time period. The SF6 trend in the troposphere from MIPAS and ACE-FTS observations is also close to the ones from the FTIR retrievals and the SMO in situ measurements. [ABSTRACT FROM AUTHOR]

Profiles of CFC-11 (CCl3F), CFC-12 (CCl2F2) and HCFC-22 (CHF2Cl) have been obtained from Fourier transform infrared (FTIR) solar absorption measurements above the Saint-Denis (St Denis) and MaÃ'do sites at Reunion Island (21° & S, 55° & E) with low vertical resolution. FTIR profile retrievals are performed by the SFIT4 program and the detail retrieval strategies along with the systematic/random uncertainties of CFC-11, CFC-12, and HCFC-22 are discussed in this study. The FTIR data of all three species are sensitive to the whole troposphere and the lowermost stratosphere, with the peak sensitivity between 5 and 10 & km. The trends derived from the combined St Denis and MaÃ'do FTIR time-series are -0.86 & ± & 0.12 & % and 2.75 & ± & 0.12 & % for CFC-11 and HCFC-22, respectively, for the period 2004 to 2016, and -0.76 & ± & 0.05 & % for CFC-12 for 2009 to 2016. These measurements are consistent with the trends observed by the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Division's (GMD) Halocarbons & other Atmospheric Trace Species Group (HATS) measurements at Samoa (14.2° & S, 170.5° & W) for CFC-11 (-0.87 & ± & 0.04 & %), but slightly weaker for HCFC-22 (3.46 & ± & 0.05 & %) and stronger for CFC-12 (-0.60 & ± & 0.02 & %). The ground-based FTIR data have also been compared with the collocated Michelson Interferometer for Passive Atmospheric Sounding (MIPAS/ENVISAT) data, and found to be in good agreement: the observed mean relative biases and standard deviations of the differences between the smoothed MIPAS and FTIR partial columns (6-30 & km) are (-4.3 & % and 4.4 & %), (-2.9 & % and 4.6 & %) and (-0.7 & % and 6.0 & %) for CFC-11, CFC-12, and HCFC-22, respectively, which are within the combined error budgets from both measurements. [ABSTRACT FROM AUTHOR]

The nationwide lockdown due to the COVID-19 pandemic in 2020 reduced industrial and human activities in China. In this study, we investigate atmospheric carbon monoxide (CO) concentration changes during the lockdown from observations at the surface and from two satellites (TROPOspheric Monitoring Instrument (TROPOMI) and Infrared Atmospheric Sounding Interferometer (IASI)). It is found that the average CO surface concentration in 2020 was close to that in 2019 before the lockdown, and became 18.7% lower as compared to 2019 during the lockdown. The spatial variation of the change in the CO surface concentration is high, with an 8–27% reduction observed for Beijing, Shanghai, Chengdu, Zhengzhou, and Guangzhou, and almost no change in Wuhan. The TROPOMI and IASI satellite observations show that the CO columns decreased by 2–13% during the lockdown in most regions in China. However in South China, there was an 8.8% increase in the CO columns observed by TROPOMI and a 36.7% increase observed by IASI, which is contrary to the 23% decrease in the surface CO concentration. The enhancement of the CO column in South China is strongly affected by the fire emissions transported from Southeast Asia. This study provides an insight into the impact of COVID-19 on CO concentrations both at the surface and in the columns in China, and it can be extended to evaluate other areas using the same approach. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) is the most important greenhouse gas and several satellites have been launched to monitor the atmospheric CO2 at regional and global scales. Evaluation of the measurements obtained from these satellites against accurate and precise instruments is crucial. In this work, aircraft measurements of CO2 were carried out over Qinhuangdao, China (39.9354°N, 119.6005°E), on 14, 16, and 19 March 2019 to validate the Greenhous gases Observing SATellite (GOSAT) and the Orbiting Carbon Observatory 2 (OCO-2) CO2 retrievals. The airborne in situ instruments were mounted on a research aircraft and the measurements were carried out between the altitudes of ~0.5 and 8.0 km to obtain the vertical profiles of CO2. The profiles captured a decrease in CO2 concentration from the surface to maximum altitude. Moreover, the vertical profiles from GEOS-Chem and the National Oceanic and Atmospheric Administration (NOAA) CarbonTracker were also compared with in situ and satellite datasets. The satellite and the model datasets captured the vertical structure of CO2 when compared with in situ measurements, which showed good agreement among the datasets. The dry-air column-averaged CO2 mole fractions (XCO2) retrieved from OCO-2 and GOSAT showed biases of 1.33 ppm (0.32%) and −1.70 ppm (−0.41%), respectively, relative to the XCO2 derived from in situ measurements. [ABSTRACT FROM AUTHOR]

Phthalate esters (PAEs) are widely used as plasticizers and have become one of the emerging contaminants with an increasing public concern. The residues of PAEs frequently co-exist with heavy metals such as cadmium (Cd) in waters; however, their joint ecotoxicity remains largely unknown. We herein investigated the single and joint toxicity of commonly used PAEs and Cd using freshwater luminescent bacteria Vibrio qinghaiensis sp.-Q67 . The median effective concentration (EC 50 ) of benzyl butyl phthalate (BBP), dibutyl phthalate (DBP), diethyl phthalate (DEP), dimethyl phthalate (DMP), diisooctyl phthalate (DIOP) and di- n -octyl phthalate (DOP) were determined to be in the range from 134.4 mg/L to as high as 1000 mg/L, indicating very weak toxicity to Vibrio qinghaiensis sp.-Q67 . The toxicity of single PAEs showed a significant linear relationship with Log K ow , indicating the dependence of the elevated toxicity on the increasing hydrophilicity. The toxicity of binary mixture of PAEs was further evaluated in silico using the independent action (IA) model and concentration addition (CA) model. DMP-DEP, DEP-DBP or DMP-DBP exhibited antagonistic effects with the toxic unit value higher than 1.2. The CA and IA models poorly predicted the joint toxicity of DMP-DEP, DEP-DBP or DMP-DBP. The joint toxicity of the binary mixtures of DMP, DEP or DBP with Cd was simple additive as predicted by the CA and IA models. Our results indicated the potentially higher risk of PAEs in the presence of Cd, emphasizing the importance of determining the impact of their joint effects on aquatic organisms. The integrated in vitro and in silico methods employed in this study will be beneficial to study the joint toxicity and better assess the aquatic ecological risk of PAEs. [ABSTRACT FROM AUTHOR]