| 1. |
- Cai, Jing, et al.
(författare)
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Characterization of offline analysis of particulate matter with FIGAERO-CIMS
- 2023
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Ingår i: Atmospheric Measurement Techniques (AMT). - : Copernicus GmbH. - 1867-8610 .- 1867-8548 .- 1867-1381. ; 16:5, s. 1147-1165
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Tidskriftsartikel (refereegranskat)abstract
- Measurements of the molecular composition of organic aerosol (OA) constituents improve our understanding of sources, formation processes, and physicochemical properties of OA. One instrument providing such data at a time resolution of minutes to hours is the chemical ionization time-of-flight mass spectrometer with filter inlet for gases and aerosols (FIGAERO-CIMS). The technique collects particles on a filter, which are subsequently desorbed, and the evaporated molecules are ionized and analyzed in the mass spectrometer. However, long-term measurements using this technique and/or field deployments at several sites simultaneously require substantial human and financial resources. The analysis of filter samples collected outside the instrument (offline) may provide a more cost-efficient alternative and makes this technology available for the large number of particle filter samples collected routinely at many different sites globally. Filter-based offline use of the FIGAERO-CIMS limits this method, albeit to particle-phase analyses, which is likely at a reduced time resolution compared to online deployments. Here we present the application and assessment of offline FIGAERO-CIMS, using Teflon and quartz fiber filter samples that were collected in autumn 2018 in urban Beijing. We demonstrate the feasibility of the offline application with a “sandwich” sample preparation for the over 900 identified organic compounds with (1) high signal-to-noise ratios, (2) high repeatability, and (3) linear signal response to the filter loadings. Comparable overall signals were observed between the quartz fiber and Teflon filters for 12 and 24h samples but with larger signals for semi-volatile compounds for the quartz fiber filters, likely due to adsorption artifacts. We also compare desorption profile (thermogram) shapes for the two filter materials. Thermograms are used to derive volatility qualitatively based on the desorption temperature at which the maximum signal intensity of a compound is observed (Tmax). While we find that Tmax can be determined with high repeatability (±5.7∘C) from the duplicate tests for one filter type, we observe considerable differences in Tmax between the quartz and Teflon filters, warranting further investigation into the thermal desorption characteristics of different filter types. Overall, this study provides a basis for expanding OA molecular characterization by FIGAERO-CIMS to situations where and when deployment of the instrument itself is not possible.
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| 2. |
- Baron, P., et al.
(författare)
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The level 2 research product algorithms for the superconducting submillimeter-wave limb-emission sounder (SMILES)
- 2011
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Ingår i: Atmospheric Measurement Techniques Discussions. - : Copernicus GmbH. - 1867-8610. ; 4:3, s. 3593-3645
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Tidskriftsartikel (refereegranskat)abstract
- This paper describes the algorithms of the level-2 research (L2r) processingchain developed for the Superconducting Submillimeter-Wave Limb-EmissionSounder (SMILES). The chain has been developed in parallel to the operationalchain for conducting researches on calibration and retrieval algorithms. L2rchain products are available to the scientific community. The objective ofversion 2 is the retrieval of the vertical distribution of trace gases in thealtitude range of 18-90 km. An theoretical error analysis is conducted toestimate the retrieval feasibility of key parameters of the processing:line-of-sight elevation tangent altitudes (or angles), temperature and O3 profiles. The line-of-sight tangent altitudes are retrievedbetween 20 and 50 km from the strong ozone (O3) line at 625.371 GHz,with low correlation with the O3 volume-mixing ratio and temperatureretrieved profiles. Neglecting the non-linearity of the radiometric gain inthe calibration procedure is the main systematic error. It is large for theretrieved temperature (between 5-10 K). Therefore, atmospheric pressure cannot be derived from the retrieved temperature, and, then, in the altituderange where the line-of-sight tangent altitudes are retrieved, the retrievedtrace gases profiles are found to be better represented on pressure levelsthan on altitude levels. The error analysis for the retrieved HOCl profiledemonstrates that best results for inverting weak lines can be obtained byusing narrow spectral windows. Future versions of the L2r algorithms willimprove the temperature/pressure retrievals and also provide information inthe upper tropospheric/lower stratospheric region (e.g., water vapor, icecontent, O3) and on stratospheric and mesospheric line-of-sight winds.
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| 3. |
- Kiefer, M., et al.
(författare)
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Impact of temperature field inhomogeneities on the retrieval of atmospheric species from MIPAS IR limb emission spectra
- 2010
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Ingår i: Atmospheric Measurement Techniques Discussions. - : Copernicus GmbH. - 1867-8610. ; 3:2, s. 1707-1742
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Tidskriftsartikel (refereegranskat)abstract
- We examine volume mixing ratios (vmr) retrieved from limb emission spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). In level 2 (L2) data products of three different retrieval processors, which perform one dimensional (1-D) retrievals, we find significant differences between species' profiles from ascending and descending orbit parts. The relative differences vary systematically with time of the year, latitude, and altitude. In the lower stratosphere their monthly means can reach maxima of 20% for CFC-11, CFC-12, HNO3, H2O, 10% for CH4 and N2O. Relative differences between monthly means of 1-D retrieval results and of the true atmospheric state can be expected to reach half of these percentage values, while relative differences in single vmr profiles might well exceed those numbers. Often there are no physical or chemical reasons for these differences, so they are an indicator for a problem in the data processing. The differences are generally largest at locations where the meridional temperature gradient of the atmosphere is strong. On the contrary, when performing the retrieval with a tomographic two dimensional (2-D) retrieval, L2 products generally do not show these differences. This implies that inhomogeneities in the temperature field, and possibly in the species' fields, which are accounted for in the 2-D algorithm and not in standard 1-D processors, may cause significant deviations in the results. Inclusion of an externally given adequate temperature gradient in the forward model of a 1-D processor helps to reduce the observed differences. However, only the full tomographic approach is suitable to resolve the horizontal inhomogeneities. Implications for the use of the 1-D data, e.g. for validation, are discussed. The dependence of the ascending/descending differences on the observation strategy suggests that this problem is to be expected to affect in general 1-D retrievals of infrared limb sounders, if the line of sight of the instrument has a significant component in the direction of the horizontal temperature variation.
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| 4. |
- Larsson, Richard, et al.
(författare)
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Modeling the Zeeman effect in high altitude SSMIS channels for numerical weather prediction profiles : Comparing a fast model and a line-by-line model
- 2015
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Ingår i: Atmospheric Measurement Techniques Discussions. - : Copernicus GmbH. - 1867-8610. ; 8:10, s. 10179-10211
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Tidskriftsartikel (refereegranskat)abstract
- We present a comparison of a reference and a fast radiative transfer model using numerical weather prediction profiles for the Zeeman-affected high altitude Special Sensor Microwave Imager/Sounder channels 19–22. We find that the models agree well for channels 21 and 22 compared to the channels' system noise temperatures (1.9 and 1.3 K, respectively) and the expected profile errors at the affected altitudes (estimated to be around 5 K). For channel 22 there is a 0.5 K average difference between the models, with a standard deviation of 0.24 K for the full set of atmospheric profiles. Same channel, there is 1.2 K in average between the fast model and the sensor measurement, with 1.4 K standard deviation. For channel 21 there is a 0.9 K average difference between the models, with a standard deviation of 0.56 K. Same channel, there is 1.3 K in average between the fast model and the sensor measurement, with 2.4 K standard deviation. We consider the relatively small model differences as a validation of the fast Zeeman effect scheme for these channels. Both channels 19 and 20 have smaller average differences between the models (at below 0.2 K) and smaller standard deviations (at below 0.4 K) when both models use a two-dimensional magnetic field profile. However, when the reference model is switched to using a full three-dimensional magnetic field profile, the standard deviation to the fast model is increased to almost 2 K due to viewing geometry dependencies causing up to ± 7 K differences near the equator. The average differences between the two models remain small despite changing magnetic field configurations. We are unable to compare channels 19 and 20 to sensor measurements due to limited altitude range of the numerical weather prediction profiles. We recommended that numerical weather prediction software using the fast model takes the available fast Zeeman scheme into account for data assimilation of the affected sensor channels to better constrain the upper atmospheric temperatures.
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| 5. |
- Lopez-Hilfiker, F. D., et al.
(författare)
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A novel method for on-line analysis of gas and particle composition: description and evaluation of a Filter Inlet for Gases and AEROsols (FIGAERO)
- 2013
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Ingår i: Atmospheric Measurement Techniques Discussions. - : Copernicus Publications. - 1867-8610. ; 6:5, s. 9347-9395
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Tidskriftsartikel (refereegranskat)abstract
- We describe a novel inlet that allows measurement of both gas and particle molecular composition when coupled to mass spectrometric, chromatographic, or optical sensors: the Filter Inlet for Gas and AEROsol (FIGAERO). The design goals for the FIGAERO are to allow unperturbed observation of ambient air while simultaneously analyzing gases and collecting particulate matter on a Teflon filter via an entirely separate sampling port. The filter is analyzed periodically by the same sensor on hourly or faster timescales using temperature-programmed thermal desorption. We assess the performance of the FIGAERO by coupling it to a high-resolution time-of-flight chemical-ionization mass spectrometer (HRToF-CIMS) in laboratory chamber studies of α-pinene oxidation and field measurements at a boreal forest location. Low instrument backgrounds give detection limits of ppt or lower for compounds in the gas-phase and in the pg m−3 range for particle phase compounds. The FIGAERO-HRToF-CIMS provides molecular information about both gases and particle composition on the 1 Hz and hourly timescales, respectively for hundreds of compounds. The FIGAERO thermal desorptions are highly reproducible (better than 10%), allowing a calibrated assessment of the effective volatility of desorbing compounds and the role of thermal decomposition during the desorption process. We show that the often multi-modal desorption thermograms arising from secondary organic aerosol (SOA) provide additional insights into molecular composition and/or particle morphology, and exhibit changes with changes in SOA formation or aging pathways.
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| 6. |
- Reinap, Ausra, 1973-, et al.
(författare)
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Dry deposition of NaCl aerosols: theory and method for a modified leaf-washing technique
- 2010
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Ingår i: Atmospheric Measurement Techniques Discussions. - : Copernicus Publications on behalf of the European Geosciences Union. - 1867-8610. ; 3:4, s. 3851-3876
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Tidskriftsartikel (refereegranskat)abstract
- Within the framework of aerosol deposition to vegetation we present a specially designed leaf wash-off method used in a wind-tunnel based study, where leaves of Quercus robur L. were exposed to NaCl aerosols. We summarise the principles and illustrate the method for two types of substances, the chloride ion and the sodium ion, and for two levels of aerosol exposure prior to leaf washing. On the average, in the low-exposure experiments (S1), the 1st (2nd) wash-off step provided 90% (96%) of the amount of Cl− on the leaves. In the high-exposure experiments (S2) the corresponding values were 96% and 99%. For sodium, the general dynamics resembles that of chloride, but the amounts washed off were, in both series, on the average below what would be expected if the equivalent ratio in the tunnel aerosol were to be preserved. Na+ showed adsorption and/or absorption at the leaf surfaces. The difference between the mean values of the amounts of chloride and of sodium washed off in S1 was not statistically significant, the mean Na+ to Cl− difference as a fraction of Cl− being minus 18%±27%; corresponding values for S2 were minus 16%±9%, however (p<0.05). In the latter case, 101±57 μequiv Na+ per m2 of leaf area were missing for the equivalent relationship 1:1 with Cl− to be met. Although uncertainties are thus large, this indicates the magnitude of the Na+-retention. The method is suitable not only for chloride, an inexpensive and easy-to-handle tracer, but also for sodium under exposure at high aerosol concentrations. Our findings will help design further studies of aerosol/forest interactions.
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| 7. |
- Yuan, Yunxia
(författare)
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Atmosphere density measurements using GPS data from rigid falling spheres
- 2017
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Ingår i: Atmospheric Measurement Techniques Discussions. - 1867-8610.
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric density profiles in the stratosphere and mesosphere are determined by means of low cost Global Positioning System (GPS) receivers on in situ rigid falling spheres released from a sounding rocket. Values below an altitude of 80 km are obtained. Aerodynamic drag relates atmospheric densities to other variables such as velocities of spheres, drag coefficients,and reference area. The densities are reconstructed by iterative solution. The calculated density is reasonably accurate,with deviation within 10% with respect to the European Centre for Medium-range Weather Forecasts ( ECMWF) reference value. The atmospheric temperature and wind profiles are obtained as well, and compared to independent data.
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