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著者人数: 60名, 形態: カラー図版あり, Number of authors: 60, Physical characteristics: Original contains color illustrations, Accepted: 2021-08-18, 資料番号: PA2210074000

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, affecting air quality and climate change. Mid-infrared high spectral resolution solar-absorption spectra are continuously recorded by a Fourier-transform infrared (FTIR) spectrometer (Bruker IFS 125HR) at Xianghe (39.75° N, 116.96° E), China. In this study, we use the SFIT4 code to retrieve these five species from the FTIR spectra measured between June 2018 and November 2021. The retrieval strategies, retrieval information, and uncertainties are presented and discussed. For the first time, the time series, variations, and correlations of these five species are analyzed 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, there is almost no seasonal variation of the CO total column. Using the monthly means as the background, the synoptic variations of these species are investigated as well. The FTIR measurements at Xianghe reveal high correlations among these species, indicating that they are affected by common sources. The correlation coefficients (R) between CO and the other four species (C2H2, C2H6, H2CO, and HCN) are between 0.68 and 0.80. The FLEXible PARTicle dispersion model (FLEXPART) v10.4 backward simulations are used to understand the airmass sources observed at Xianghe, and it is found that the high column abundances are coming mainly from local anthropogenic emissions. Using satellite measurements, we show that the boreal forest fire emissions in Russia can lead to enhanced HCN total columns at Xianghe.

Réunion Island is situated in the Indian Ocean and holds one of the very few atmospheric observatories in the tropical Southern Hemisphere. Moreover, it hosts experiments providing both ground-based surface and column observations of CO2, CH4, and CO atmospheric concentrations. This work presents a comprehensive study of these observations made in the capital Saint-Denis and at the high-altitude Maïdo Observatory. We used simulations of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), in its passive tracer option (WRF-GHG), to gain more insight to the factors that determine the observed concentrations. Additionally, this study provides an evaluation of the WRF-GHG performance in a region of the globe where it has not yet been applied. A comparison of the basic meteorological fields near the surface and along atmospheric profiles showed that WRF-GHG has decent skill in reproducing these meteorological measurements, especially temperature. Furthermore, a distinct diurnal CO2 cycle with values up to 450 ppm was found near the surface in Saint-Denis, driven by local anthropogenic emissions, boundary layer dynamics, and accumulation due to low wind speed at night. Due to an overestimation of local wind speed, WRF-GHG underestimates this nocturnal buildup. At Maïdo, a similar diurnal cycle is found but with much smaller amplitude. There, surface CO2 is essentially driven by the surrounding vegetation. The hourly column-averaged mole fractions of CO2 (XCO2) of WRF-GHG and the corresponding TCCON observations were highly correlated with a Pearson correlation coefficient of 0.90. These observations represent different air masses to those near the surface; they are influenced by processes from Madagascar, Africa, and further away. The model shows contributions from fires during the Southern Hemisphere biomass burning season but also biogenic enhancements associated with the dry season. Due to a seasonal bias in the boundary conditions, WRF-GHG fails to accurately reproduce the CH4 observations at Réunion Island. Furthermore, local anthropogenic fluxes are the largest source influencing the surface CH4 observations. However, these are likely overestimated. Furthermore, WRF-GHG is capable of simulating CO levels on Réunion Island with a high precision. As to the observed CO column (XCO), we confirmed that biomass burning plumes from Africa and elsewhere are important for explaining the observed variability. The in situ observations at the Maïdo Observatory can characterize both anthropogenic signals from the coastal regions and biomass burning enhancements from afar. Finally, we found that a high model resolution of 2 km is needed to accurately represent the surface observations. At Maïdo an even higher resolution might be needed because of the complex topography and local wind patterns. To simulate the column Fourier transform infrared (FTIR) observations on the other hand, a model resolution of 50 km might already be sufficient.

Magnesium (Mg) is essential for many biological processes in plant cells, and its deficiency causes yield reduction in crop systems. Low Mg status reportedly affects photosynthesis, sucrose partitioning and biomass allocation. However, earlier physiological responses to Mg deficiency are scarcely described. Here, we report that Mg deficiency in Arabidopsis thaliana first modified the mineral profile in mature leaves within 1 or 2 days, then affected sucrose partitioning after 4 days, and net photosynthesis and biomass production after 6 days. The short-term Mg deficiency reduced the contents of phosphorus (P), potassium, manganese, zinc and molybdenum in mature but not in expanding (young) leaves. While P content decreased in mature leaves, P transport from roots to mature leaves was not affected, indicating that Mg deficiency triggered retranslocation of the mineral nutrients from mature leaves. A global transcriptome analysis revealed that Mg deficiency triggered the expression of genes involved in defence response in young leaves.

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.

Dual-scan ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric nitrogen dioxide (NO2) and aerosols have been carried out in Uccle (50.8° N, 4.35° E; Brussels region, Belgium) for two years, from March 2018 to February 2020. The MAX-DOAS instrument has been operating in both UV and Visible wavelength ranges in a dual-scan configuration consisting of two sub-modes: (1) an elevation scan in a fixed viewing azimuthal direction and (2) an azimuthal scan in a fixed low elevation angle (2°). By analyzing the O4 and NO2 dSCDs at six different wavelength intervals along every azimuthal direction and by applying a new Optimal-Estimation-based inversion approach, the horizontal distribution of the NO2 near-surface concentrations and vertical column densities (VCDs) and the aerosols near-surface extinction coefficient are retrieved along ten azimuthal directions. The retrieved horizontal NO2 concentration profiles allow the identification of the main NO2 hotspots in the Brussels area. Correlative comparisons of the retrieved horizontal NO2 distribution have been conducted with airborne, mobile, and satellite datasets, and overall a good agreement is found. The comparison with TROPOMI observations reveals that the characterization of the horizontal distribution of tropospheric NO2 VCDs by ground-based measurements, the appropriate sampling of TROPOMI pixels, and an adequate a priori NO2 profile shape in TROPOMI retrievals lead to a better consistency between satellite and ground-based datasets.