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  • 1
    In: Geophysical Research Letters, American Geophysical Union (AGU), Vol. 48, No. 7 ( 2021-04-16)
    Abstract: Process‐level understanding of new particle formation (NPF) in wintertime Beijing was obtained based on measurement state‐of‐the‐art instruments The analysis of sulfuric acid cluster composition and budget showed that sulfuric acid‐base clustering initiated NPF Condensable organic vapors were characterized and demonstrated to have a crucial influence on the growth of newly formed particles
    Type of Medium: Online Resource
    ISSN: 0094-8276 , 1944-8007
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2021
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    detail.hit.zdb_id: 7403-2
    SSG: 16,13
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  • 2
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 14, No. 2 ( 2021-02-17), p. 1239-1252
    Abstract: Abstract. Although optical components in Fourier transform infrared (FTIR) spectrometers are preferably wedged, in practice, infrared spectra typically suffer from the effects of optical resonances (“channeling”) affecting the retrieval of weakly absorbing gases. This study investigates the level of channeling of each FTIR spectrometer within the Network for the Detection of Atmospheric Composition Change (NDACC). Dedicated spectra were recorded by more than 20 NDACC FTIR spectrometers using a laboratory mid-infrared source and two detectors. In the indium antimonide (InSb) detector domain (1900–5000 cm−1), we found that the amplitude of the most pronounced channeling frequency amounts to 0.1 ‰ to 2.0 ‰ of the spectral background level, with a mean of (0.68±0.48) ‰ and a median of 0.60 ‰. In the mercury cadmium telluride (HgCdTe) detector domain (700–1300 cm−1), we find even stronger effects, with the largest amplitude ranging from 0.3 ‰ to 21 ‰ with a mean of (2.45±4.50) ‰ and a median of 1.2 ‰. For both detectors, the leading channeling frequencies are 0.9 and 0.11 or 0.23 cm−1 in most spectrometers. The observed spectral frequencies of 0.11 and 0.23 cm−1 correspond to the optical thickness of the beam splitter substrate. The 0.9 cm−1 channeling is caused by the air gap in between the beam splitter and compensator plate. Since the air gap is a significant source of channeling and the corresponding amplitude differs strongly between spectrometers, we propose new beam splitters with the wedge of the air gap increased to at least 0.8∘. We tested the insertion of spacers in a beam splitter's air gap to demonstrate that increasing the wedge of the air gap decreases the 0.9 cm−1 channeling amplitude significantly. A wedge of the air gap of 0.8∘ reduces the channeling amplitude by about 50 %, while a wedge of about 2∘ removes the 0.9 cm−1 channeling completely. This study shows the potential for reducing channeling in the FTIR spectrometers operated by the NDACC, thereby increasing the quality of recorded spectra across the network.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2505596-3
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  • 3
    In: Nature Communications, Springer Science and Business Media LLC, Vol. 12, No. 1 ( 2021-09-24)
    Abstract: Aerosol particles cool the climate by scattering solar radiation and by acting as cloud condensation nuclei. Higher temperatures resulting from increased greenhouse gas levels have been suggested to lead to increased biogenic secondary organic aerosol and cloud condensation nuclei concentrations creating a negative climate feedback mechanism. Here, we present direct observations on this feedback mechanism utilizing collocated long term aerosol chemical composition measurements and remote sensing observations on aerosol and cloud properties. Summer time organic aerosol loadings showed a clear increase with temperature, with simultaneous increase in cloud condensation nuclei concentration in a boreal forest environment. Remote sensing observations revealed a change in cloud properties with an increase in cloud reflectivity in concert with increasing organic aerosol loadings in the area. The results provide direct observational evidence on the significance of this negative climate feedback mechanism.
    Type of Medium: Online Resource
    ISSN: 2041-1723
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2021
    detail.hit.zdb_id: 2553671-0
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  • 4
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 9 ( 2020-09-10), p. 4791-4839
    Abstract: Abstract. The Total Carbon Column Observing Network (TCCON) is the baseline ground-based network of instruments that record solar absorption spectra from which accurate and precise column-averaged dry-air mole fractions of CO2 (XCO2), CH4 (XCH4), CO (XCO), and other gases are retrieved. The TCCON data have been widely used for carbon cycle science and validation of satellites measuring greenhouse gas concentrations globally. The number of stations in the network (currently about 25) is limited and has a very uneven geographical coverage: the stations in the Northern Hemisphere are distributed mostly in North America, Europe, and Japan, and only 20 % of the stations are located in the Southern Hemisphere, leaving gaps in the global coverage. A denser distribution of ground-based solar absorption measurements is needed to improve the representativeness of the measurement data for various atmospheric conditions (humid, dry, polluted, presence of aerosol), various surface conditions such as high albedo (〉0.4) and very low albedo, and a larger latitudinal distribution. More stations in the Southern Hemisphere are also needed, but a further expansion of the network is limited by its costs and logistical requirements. For this reason, several groups are investigating supplemental portable low-cost instruments. The European Space Agency (ESA) funded campaign Fiducial Reference Measurements for Ground-Based Infrared Greenhouse Gas Observations (FRM4GHG) at the Sodankylä TCCON site in northern Finland aims to characterise the assessment of several low-cost portable instruments for precise solar absorption measurements of XCO2, XCH4, and XCO. The test instruments under investigation are three Fourier transform spectrometers (FTSs): a Bruker EM27/SUN, a Bruker IRcube, and a Bruker Vertex70, as well as a laser heterodyne spectroradiometer (LHR) developed by the UK Rutherford Appleton Laboratory. All four remote sensing instruments performed measurements simultaneously next to the reference TCCON instrument, a Bruker IFS 125HR, for a full year in 2017. The TCCON FTS was operated in its normal high-resolution mode (TCCON data set) and in a special low-resolution mode (HR125LR data set), similar to the portable spectrometers. The remote sensing measurements are complemented by regular AirCore launches performed from the same site. They provide in situ vertical profiles of the target gas concentrations as auxiliary reference data for the column retrievals, which are traceable to the WMO SI standards. The reference measurements performed with the Bruker IFS 125HR were found to be affected by non-linearity of the indium gallium arsenide (InGaAs) detector. Therefore, a non-linearity correction of the 125HR data was performed for the whole campaign period and compared with the test instruments and AirCore. The non-linearity-corrected data (TCCONmod data set) show a better match with the test instruments and AirCore data compared to the non-corrected reference data. The time series, the bias relative to the reference instrument and its scatter, and the seasonal and the day-to-day variations of the target gases are shown and discussed. The comparisons with the HR125LR data set gave a useful analysis of the resolution-dependent effects on the target gas retrieval. The solar zenith angle dependence of the retrievals is shown and discussed. The intercomparison results show that the LHR data have a large scatter and biases with a strong diurnal variation relative to the TCCON and other FTS instruments. The LHR is a new instrument under development, and these biases are currently being investigated and addressed. The campaign helped to characterise and identify instrumental biases and possibly retrieval biases, which are currently under investigation. Further improvements of the instrument are ongoing. The EM27/SUN, the IRcube, the modified Vertex70, and the HR125LR provided stable and precise measurements of the target gases during the campaign with quantified small biases. The bias dependence on the humidity along the measurement line of sight has been investigated and no dependence was found. These three portable low-resolution FTS instruments are suitable to be used for campaign deployment or long-term measurements from any site and offer the ability to complement the TCCON and expand the global coverage of ground-based reference measurements of the target gases.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 5
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 14, No. 3 ( 2021-03-11), p. 1993-2011
    Abstract: Abstract. In this paper, we compare column-averaged dry-air mole fractions of water vapor (XH2O) retrievals from the COllaborative Carbon Column Observing Network (COCCON) with retrievals from two co-located high-resolution Fourier transform infrared (FTIR) spectrometers as references at two boreal sites, Kiruna, Sweden, and Sodankylä, Finland, from 6 March 2017 to 20 September 2019. In the framework of the Network for the Detection of Atmospheric Composition Change (NDACC), an FTIR spectrometer is operated at Kiruna. The H2O product derived from these observations has been generated with the MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) processor. In Sodankylä, a Total Carbon Column Observing Network (TCCON) spectrometer is operated, and the official XH2O data as provided by TCCON are used for this study. The datasets are in good overall agreement, with COCCON data showing a wet bias of (49.20±58.61) ppm ((3.33±3.37) %, R2=0.9992) compared with MUSICA NDACC and (56.32±45.63) ppm ((3.44±1.77) %, R2=0.9997) compared with TCCON. Furthermore, the a priori H2O volume mixing ratio (VMR) profiles (MAP) used as a priori information in the TCCON retrievals (also adopted for COCCON retrievals) are evaluated with respect to radiosonde (Vaisala RS41) profiles at Sodankylä. The MAP and radiosonde profiles show similar shapes and a good linear correlation of integrated XH2O, indicating that MAP is a reasonable approximation of the true atmospheric state and an appropriate choice for the scaling retrieval methods as applied by COCCON and TCCON. COCCON shows a reduced dry bias (−14.96 %) in comparison with TCCON (−19.08 %) with respect to radiosonde XH2O. Finally, we investigate the quality of satellite data at high latitudes. For this purpose, the COCCON XH2O is compared with retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) generated with the MUSICA processor (MUSICA IASI) and with retrievals from the TROPOspheric Monitoring Instrument (TROPOMI). Both paired datasets generally show good agreement and similar correlations at the two sites. COCCON measures 4.64 % less XH2O at Kiruna and 3.36 % less at Sodankylä with respect to MUSICA IASI, whereas COCCON measures 9.71 % more XH2O at Kiruna and 7.75 % more at Sodankylä compared with TROPOMI. Our study supports the assumption that COCCON also delivers a well-characterized XH2O data product. This emphasizes that this approach might complement the TCCON network with respect to satellite validation efforts. This is the first published study where COCCON XH2O has been compared with MUSICA NDACC and TCCON retrievals and has been used for MUSICA IASI and TROPOMI validation.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2505596-3
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 9 ( 2020-09-09), p. 4751-4771
    Abstract: Abstract. We compare the atmospheric column-averaged dry-air mole fractions of carbon dioxide (XCO2) and methane (XCH4) measured with a pair of COllaborative Carbon Column Observing Network (COCCON) spectrometers at Kiruna and Sodankylä (boreal areas). We compare model data provided by the Copernicus Atmosphere Monitoring Service (CAMS) between 2017 and 2019 with XCH4 data from the recently launched Sentinel-5 Precursor (S5P) satellite between 2018 and 2019. In addition, measured and modeled gradients of XCO2 and XCH4 (ΔXCO2 and ΔXCH4) on regional scales are investigated. Both sites show a similar and very good correlation between COCCON retrievals and the modeled CAMS XCO2 data, while CAMS data are biased high with respect to COCCON by 3.72 ppm (±1.80 ppm) in Kiruna and 3.46 ppm (±1.73 ppm) in Sodankylä on average. For XCH4, CAMS values are higher than the COCCON observations by 0.33 ppb (±11.93 ppb) in Kiruna and 7.39 ppb (±10.92 ppb) in Sodankylä. In contrast, the S5P satellite generally measures lower atmospheric XCH4 than the COCCON spectrometers, with a mean difference of 9.69 ppb (±20.51 ppb) in Kiruna and 3.36 ppb (±17.05 ppb) in Sodankylä. We compare the gradients of XCO2 and XCH4 (ΔXCO2 and ΔXCH4) between Kiruna and Sodankylä derived from CAMS analysis and COCCON and S5P measurements to study the capability of detecting sources and sinks on regional scales. The correlations in ΔXCO2 and ΔXCH4 between the different datasets are generally smaller than the correlations in XCO2 and XCH4 between the datasets at either site. The ΔXCO2 values predicted by CAMS are generally higher than those observed with COCCON with a slope of 0.51. The ΔXCH4 values predicted by CAMS are mostly higher than those observed with COCCON with a slope of 0.65, covering a larger dataset than the comparison between S5P and COCCON. When comparing CAMS ΔXCH4 with COCCON ΔXCH4 only in S5P overpass days (slope = 0.53), the correlation is close to that between S5P and COCCON (slope = 0.51). CAMS, COCCON, and S5P predict gradients in reasonable agreement. However, the small number of observations coinciding with S5P limits our ability to verify the performance of this spaceborne sensor. We detect no significant impact of ground albedo and viewing zenith angle on the S5P results. Both sites show similar situations with the average ratios of XCH4 (S5P/COCCON) of 0.9949±0.0118 in Kiruna and 0.9953±0.0089 in Sodankylä. Overall, the results indicate that the COCCON instruments have the capability of measuring greenhouse gas (GHG) gradients on regional scales, and observations performed with the portable spectrometers can contribute to inferring sources and sinks and to validating spaceborne greenhouse gas sensors. To our knowledge, this is the first published study using COCCON spectrometers for the validation of XCH4 measurements collected by S5P.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 22 ( 2021-11-16), p. 16661-16687
    Abstract: Abstract. Satellite-based observations of atmospheric carbon dioxide (CO2) provide measurements in remote regions, such as the biologically sensitive but undersampled northern high latitudes, and are progressing toward true global data coverage. Recent improvements in satellite retrievals of total column-averaged dry air mole fractions of CO2 (XCO2) from the NASA Orbiting Carbon Observatory 2 (OCO-2) have allowed for unprecedented data coverage of northern high-latitude regions, while maintaining acceptable accuracy and consistency relative to ground-based observations, and finally providing sufficient data in spring and autumn for analysis of satellite-observed XCO2 seasonal cycles across a majority of terrestrial northern high-latitude regions. Here, we present an analysis of XCO2 seasonal cycles calculated from OCO-2 data for temperate, boreal, and tundra regions, subdivided into 5∘ latitude by 20∘ longitude zones. We quantify the seasonal cycle amplitudes (SCAs) and the annual half drawdown day (HDD). OCO-2 SCAs are in good agreement with ground-based observations at five high-latitude sites, and OCO-2 SCAs show very close agreement with SCAs calculated for model estimates of XCO2 from the Copernicus Atmosphere Monitoring Services (CAMS) global inversion-optimized greenhouse gas flux model v19r1 and the CarbonTracker2019 model (CT2019B). Model estimates of XCO2 from the GEOS-Chem CO2 simulation version 12.7.2 with underlying biospheric fluxes from CarbonTracker2019 (GC-CT2019) yield SCAs of larger magnitude and spread over a larger range than those from CAMS, CT2019B, or OCO-2; however, GC-CT2019 SCAs still exhibit a very similar spatial distribution across northern high-latitude regions to that from CAMS, CT2019B, and OCO-2. Zones in the Asian boreal forest were found to have exceptionally large SCA and early HDD, and both OCO-2 data and model estimates yield a distinct longitudinal gradient of increasing SCA from west to east across the Eurasian continent. In northern high-latitude regions, spanning latitudes from 47 to 72∘ N, longitudinal gradients in both SCA and HDD are at least as pronounced as latitudinal gradients, suggesting a role for global atmospheric transport patterns in defining spatial distributions of XCO2 seasonality across these regions. GEOS-Chem surface contact tracers show that the largest XCO2 SCAs occur in areas with the greatest contact with land surfaces, integrated over 15–30 d. The correlation of XCO2 SCA with these land surface contact tracers is stronger than the correlation of XCO2 SCA with the SCA of CO2 fluxes or the total annual CO2 flux within each 5∘ latitude by 20∘ longitude zone. This indicates that accumulation of terrestrial CO2 flux during atmospheric transport is a major driver of regional variations in XCO2 SCA.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 8
    In: GIScience & Remote Sensing, Informa UK Limited, Vol. 57, No. 7 ( 2020-10-02), p. 943-964
    Type of Medium: Online Resource
    ISSN: 1548-1603 , 1943-7226
    Language: English
    Publisher: Informa UK Limited
    Publication Date: 2020
    detail.hit.zdb_id: 2209042-3
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  • 9
    In: Environmental Science & Technology Letters, American Chemical Society (ACS), Vol. 9, No. 5 ( 2022-05-10), p. 375-382
    Type of Medium: Online Resource
    ISSN: 2328-8930 , 2328-8930
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2022
    detail.hit.zdb_id: 2745499-X
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  • 10
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 9 ( 2020-09-28), p. 5033-5063
    Abstract: Abstract. Seasonal CO2 exchange in the boreal forest plays an important role in the global carbon budget and in driving interannual variability in seasonal cycles of atmospheric CO2. Satellite-based observations from polar orbiting satellites like the Orbiting Carbon Observatory-2 (OCO-2) offer an opportunity to characterize boreal forest seasonal cycles across longitudes with a spatially and temporally rich data set, but data quality controls and biases still require vetting at high latitudes. With the objective of improving data availability at northern, terrestrial high latitudes, this study evaluates quality control methods and biases of OCO-2 retrievals of atmospheric column-averaged dry air mole fractions of CO2 (XCO2) in boreal forest regions. In addition to the standard quality control (QC) filters recommended for the Atmospheric Carbon Observations from Space (ACOS) B8 (B8 QC) and ACOS B9 (B9 QC) OCO-2 retrievals, a third set of quality control filters were specifically tailored to boreal forest observations (boreal QC) with the goal of increasing data availability at high latitudes without sacrificing data quality. Ground-based reference measurements of XCO2 include observations from two sites in the Total Carbon Column Observing Network (TCCON) at East Trout Lake, Saskatchewan, Canada, and Sodankylä, Finland. OCO-2 retrievals were also compared to ground-based observations from two Bruker EM27/SUN Fourier transform infrared spectrometers (FTSs) at Fairbanks, Alaska, USA. The EM27/SUN spectrometers that were deployed in Fairbanks were carefully monitored for instrument performance and were bias corrected to TCCON using observations at the Caltech TCCON site. The B9 QC were found to pass approximately twice as many OCO-2 retrievals over land north of 50∘ N than the B8 QC, and the boreal QC were found to pass approximately twice as many retrievals in May, August, and September as the B9 QC. While boreal QC results in a substantial increase in passable retrievals, this is accompanied by increases in the standard deviations in biases at boreal forest sites from ∼1.4 parts per million (ppm) with B9 QC to ∼1.6 ppm with boreal QC. Total average biases for coincident OCO-2 retrievals at the three sites considered did not consistently increase or decrease with different QC methods, and instead, responses to changes in QC varied according to site and satellite viewing geometries. Regardless of the quality control method used, seasonal variability in biases was observed, and this variability was more pronounced at Sodankylä and East Trout Lake than at Fairbanks. Long-term coincident observations from TCCON, EM27/SUN, and satellites from multiple locations would be necessary to determine whether the reduced seasonal variability in bias at Fairbanks is due to geography or instrumentation. Monthly average biases generally varied between −1 and +1 ppm at the three sites considered, with more negative biases in spring (March, April, and May – MAM) and autumn (September and October – SO) but more positive biases in the summer months (June, July, and August – JJA). Monthly standard deviations in biases ranged from approximately 1.0 to 2.0 ppm and did not exhibit strong seasonal dependence, apart from exceptionally high standard deviation observed with all three QC methods at Sodankylä in June. There was no evidence found to suggest that seasonal variability in bias is a direct result of air mass dependence in ground-based retrievals or of proximity bias from coincidence criteria, but there were a number of retrieval parameters used as quality control filters that exhibit seasonality and could contribute to seasonal dependence in OCO-2 bias. Furthermore, it was found that OCO-2 retrievals of XCO2 without the standard OCO-2 bias correction exhibit almost no perceptible seasonal dependence in average monthly bias at these boreal forest sites, suggesting that seasonal variability in bias is introduced by the bias correction. Overall, we found that modified quality controls can allow for significant increases in passable OCO-2 retrievals with only marginal compromises in data quality, but seasonal dependence in biases still warrants further exploration.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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