scholarly journals Airborne measurements of oxygen concentration from the surface to the lower stratosphere and pole to pole

Author(s):  
Britton B. Stephens ◽  
Eric J. Morgan ◽  
Jonathan D. Bent ◽  
Ralph F. Keeling ◽  
Andrew S. Watt ◽  
...  

Abstract. We have developed in situ and flask sampling systems for airborne measurements of variations in the O2/N2 ratio at the part per million level. We have deployed these instruments on a series of aircraft campaigns to measure the distribution of atmospheric O2 from 0–14 km and 87° N to 85° S throughout the seasonal cycle. The NCAR airborne oxygen instrument (AO2) uses a vacuum ultraviolet (VUV) absorption detector for O2 and also includes an infrared CO2 sensor. The VUV detector has a precision in 5 seconds of ±1.25 per meg (1σ) δ(O2/N2), but thermal fractionation and motion effects increase this to ±2.5–4.0 per meg when sampling ambient air in flight. The NCAR/Scripps airborne flask sampler (Medusa) collects 32 cryogenically dried air samples per flight under actively controlled flow and pressure conditions. For in situ or flask O2 measurements, fractionation and surface effects can be important at the required high levels of relative precision. We describe our sampling and measurement techniques, and efforts to reduce potential biases. We also present a selection of observational results highlighting the individual and combined instrument performance. These include vertical profiles, O2 : CO2 correlations, and latitudinal cross sections reflecting the distinct influences of terrestrial photosynthesis, air-sea gas exchange, burning of various fuels, and stratospheric dynamics. When present, we have corrected the flask δ(O2/N2) measurements for fractionation during sampling or analysis, with the use of the concurrent δ(Ar/N2) measurements. We have also corrected the in situ δ(O2/N2) measurements for inlet fractionation and humidity effects by comparison to the corrected flask values. A comparison of Ar/N2-corrected Medusa flask δ(O2/N2) measurements to regional Scripps O2 Network station observations shows no systematic biases over 10 recent campaigns (+0.2 ± 8.2 per meg, mean and standard deviation, n = 86). For AO2, after resolving sample drying and inlet fractionation biases previously on the order of 10–100 per meg, independent AO2 δ(O2/N2) measurements over 6 more recent campaigns differ from coincident Medusa flask measurements by −0.3 ± 7.2 per meg (mean and standard deviation, n = 1361), with campaign-specific means ranging from −5 to +5 per meg.

2021 ◽  
Vol 14 (3) ◽  
pp. 2543-2574
Author(s):  
Britton B. Stephens ◽  
Eric J. Morgan ◽  
Jonathan D. Bent ◽  
Ralph F. Keeling ◽  
Andrew S. Watt ◽  
...  

Abstract. We have developed in situ and flask sampling systems for airborne measurements of variations in the O2/N2 ratio at the part per million level. We have deployed these instruments on a series of aircraft campaigns to measure the distribution of atmospheric O2 from 0–14 km and 87∘ N to 86∘ S throughout the seasonal cycle. The National Center for Atmospheric Research (NCAR) airborne oxygen instrument (AO2) uses a vacuum ultraviolet (VUV) absorption detector for O2 and also includes an infrared CO2 sensor. The VUV detector has a precision in 5 s of ±1.25 per meg (1σ) δ(O2/N2), but thermal fractionation and motion effects increase this to ±2.5–4.0 per meg when sampling ambient air in flight. The NCAR/Scripps airborne flask sampler (Medusa) collects 32 cryogenically dried air samples per flight under actively controlled flow and pressure conditions. For in situ or flask O2 measurements, fractionation and surface effects can be important at the required high levels of relative precision. We describe our sampling and measurement techniques and efforts to reduce potential biases. We also present a selection of observational results highlighting the individual and combined instrument performance. These include vertical profiles, O2:CO2 correlations, and latitudinal cross sections reflecting the distinct influences of terrestrial photosynthesis, air–sea gas exchange, burning of various fuels, and stratospheric dynamics. When present, we have corrected the flask δ(O2/N2) measurements for fractionation during sampling or analysis with the use of the concurrent δ(Ar/N2) measurements. We have also corrected the in situ δ(O2/N2) measurements for inlet fractionation and humidity effects by comparison to the corrected flask values. A comparison of Ar/N2-corrected Medusa flask δ(O2/N2) measurements to regional Scripps O2 Program station observations shows no systematic biases over 10 recent campaigns (+0.2±8.2 per meg, mean and standard deviation, n=86). For AO2, after resolving sample drying and inlet fractionation biases previously on the order of 10–100 per meg, independent AO2 δ(O2/N2) measurements over six more recent campaigns differ from coincident Medusa flask measurements by -0.3±7.2 per meg (mean and standard deviation, n=1361) with campaign-specific means ranging from −5 to +5 per meg.


2005 ◽  
Vol 5 (3) ◽  
pp. 2897-2945 ◽  
Author(s):  
C. Hak ◽  
I. Pundt ◽  
C. Kern ◽  
U. Platt ◽  
J. Dommen ◽  
...  

Abstract. Results from an intercomparison of several currently used in-situ techniques for the measurement of atmospheric formaldehyde (CH2O) are presented. The measurements were carried out at Bresso, an urban site in the periphery of Milan (Italy) as part of the FORMAT-I field campaign. Eight instruments were employed by six independent research groups using four different techniques: Differential Optical Absorption Spectroscopy (DOAS), Fourier Transform Infra Red (FTIR) interferometry, the fluorimetric Hantzsch reaction technique (five instruments) and a chromatographic technique employing C18-DNPH-cartridges (2,4-dinitrophenylhydrazine). White type multi-reflection systems were employed for the optical techniques in order to avoid spatial CH2O gradients and ensure the sampling of nearly the same air mass by all instruments. Between 23 and 31 July 2002, up to 13 ppbv of CH2O were observed. The concentrations lay well above the detection limits of all instruments. The formaldehyde concentrations determined with DOAS, FTIR and the Hantzsch instruments were found to agree within ±11%, with the exception of one Hantzsch instrument, which gave systematically higher values. The two hour integrated samples by DNPH yielded up to 25% lower concentrations than the data of the continuously measuring instruments averaged over the same time period. The consistency between the DOAS and the Hantzsch method was better than during previous intercomparisons in ambient air with slopes of the regression line not significantly differing from one. The differences between the individual Hantzsch instruments could be attributed in part to the calibration standards used. Possible systematic errors of the methods are discussed.


2014 ◽  
Vol 7 (9) ◽  
pp. 3127-3138 ◽  
Author(s):  
R. L. Herman ◽  
J. E. Cherry ◽  
J. Young ◽  
J. M. Welker ◽  
D. Noone ◽  
...  

Abstract. The EOS (Earth Observing System) Aura Tropospheric Emission Spectrometer (TES) retrieves the atmospheric HDO / H2O ratio in the mid-to-lower troposphere as well as the planetary boundary layer. TES observations of water vapor and the HDO isotopologue have been compared with nearly coincident in situ airborne measurements for direct validation of the TES products. The field measurements were made with a commercially available Picarro L1115-i isotopic water analyzer on aircraft over the Alaskan interior boreal forest during the three summers of 2011 to 2013. TES special observations were utilized in these comparisons. The TES averaging kernels and a priori constraints have been applied to the in situ data, using version 5 (V005) of the TES data. TES calculated errors are compared with the standard deviation (1σ) of scan-to-scan variability to check consistency with the TES observation error. Spatial and temporal variations are assessed from the in situ aircraft measurements. It is found that the standard deviation of scan-to-scan variability of TES δD is ±34.1‰ in the boundary layer and ± 26.5‰ in the free troposphere. This scan-to-scan variability is consistent with the TES estimated error (observation error) of 10–18‰ after accounting for the atmospheric variations along the TES track of ±16‰ in the boundary layer, increasing to ±30‰ in the free troposphere observed by the aircraft in situ measurements. We estimate that TES V005 δD is biased high by an amount that decreases with pressure: approximately +123‰ at 1000 hPa, +98‰ in the boundary layer and +37‰ in the free troposphere. The uncertainty in this bias estimate is ±20‰. A correction for this bias has been applied to the TES HDO Lite Product data set. After bias correction, we show that TES has accurate sensitivity to water vapor isotopologues in the boundary layer.


2011 ◽  
Vol 11 (12) ◽  
pp. 5655-5672 ◽  
Author(s):  
I. Xueref-Remy ◽  
C. Messager ◽  
D. Filippi ◽  
M. Pastel ◽  
P. Nedelec ◽  
...  

Abstract. Atmospheric airborne measurements of CO2 are very well suited for estimating the time-varying distribution of carbon sources and sinks at the regional scale due to the large geographical area covered over a short time. We present here an analysis of two cross-European airborne campaigns carried out on 23–26 May 2001 (CAATER-1) and 2–3 October 2002 (CAATER-2) over Western Europe. The area covered during CAATER-1 and CAATER-2 was 4° W to 14° E long; 44° N to 52° N lat and 1° E to 17° E long; 46° N to 52° N lat respectively. High precision in situ CO2, CO and Radon 222 measurements were recorded. Flask samples were collected during both campaigns to cross-validate the in situ data. During CAATER-1 and CAATER-2, the mean CO2 concentration was 370.1 ± 4.0 (1-σ standard deviation) ppm and 371.7 ± 5.0 (1-σ) ppm respectively. A HYSPLIT back-trajectories analysis shows that during CAATER 1, northwesterly winds prevailed. In the planetary boundary layer (PBL) air masses became contaminated over Benelux and Western Germany by emissions from these highly urbanized areas, reaching about 380 ppm. Air masses passing over rural areas were depleted in CO2 because of the photosynthesis activity of the vegetation, with observations as low as 355 ppm. During CAATER-2, the back-trajectory analysis showed that air masses were distributed among the 4 sectors. Air masses were enriched in CO2 and CO over anthropogenic emission spots in Germany but also in Poland, as these countries have part of the most CO2-emitting coal-based plants in Europe. Simultaneous measurements of in situ CO2 and CO combined with back-trajectories helped us to distinguish between fossil fuel emissions and other CO2 sources. The ΔCO/ΔCO2 ratios (R2 = 0.33 to 0.88, slopes = 2.42 to 10.37), calculated for anthropogenic-influenced air masses over different countries/regions matched national inventories quite well, showing that airborne measurements can help to identify the origin of fossil fuel emissions in the PBL even when distanced by several days/hundreds of kms from their sources. We have compared airborne CO2 observations to nearby ground station measurements and thereby, confirmed that measurements taken in the lower few meters of the PBL (low-level ground stations) are representative of the local scale, while those located in the free troposphere (FT) (moutain stations) are representative of atmospheric CO2 regionally on a scale of a few hundred kilometers. Stations located several 100 km away from each other differ from a few ppm in their measurements indicating the existence of a gradient within the free troposphere. Observations at stations located on top of small mountains may match the airborne data if the sampled air comes from the FT rather than coming up from the valley. Finally, the analysis of the CO2 vertical variability conducted on the 14 profiles recorded in each campaign shows a variability at least 5 to 8 times higher in the PBL (the 1-σ standard deviation associated to the CO2 mean of all profiles within the PBL is 4.0 ppm and 5.7 ppm for CAATER-1 and CAATER-2, respectively) than in the FT (within the FT, 1-σ is 0.5 ppm and 1.1 ppm for CAATER-1 and CAATER-2, respectively). The CO2 jump between the PBL and the FT equals 3.7 ppm for the first campaign and −0.3 ppm for the second campaign. A very striking zonal CO2 gradient of about 11 ppm was observed in the mid-PBL during CAATER-2, with higher concentrations in the west than in the east. This gradient may originate from differences in atmospheric mixing, ground emission rates or Autumn's earlier start in the west. More airborne campaigns are currently under analysis in the framework of the CARBOEUROPE-IP project to better assess the likelihood of these different hypotheses. In a companion paper (Xueref-Remy et al., 2011, Part 2), a comparison of vertical profiles from observations and several modeling frameworks was conducted for both campaigns.


2016 ◽  
Author(s):  
W. Reed Espinosa ◽  
Lorraine Remer ◽  
Oleg Dubovik ◽  
Luke Ziemba ◽  
Andreas Beyersdorf ◽  
...  

Abstract. A method for the retrieval of optical and microphysical properties from in situ light scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3° to 177°. The resulting retrieval produces particle size distributions (PSD) that agree, to within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salts particles, whose refractive index is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represent the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.


2013 ◽  
Vol 6 (12) ◽  
pp. 3369-3392 ◽  
Author(s):  
C. Pöhlker ◽  
J. A. Huffman ◽  
J.-D. Förster ◽  
U. Pöschl

Abstract. Primary biological aerosol particles (PBAP) are important factors in atmospheric cycling, climate, and public health. Pollen is a major fraction of PBAP and is receiving increasing attention due to its high allergenic potential and the associated impacts on personal life quality and economy. Recently, autofluorescence-based techniques have proven to be valuable tools for real time, in situ quantification and classification of PBAP. First studies suggest that the autofluorescence of pollen may be sufficiently selective to be utilized for an automated and real-time monitoring of pollen in ambient air. However, the degree of selectivity autofluorescence can provide is still in question and actively debated. This study addresses the origin, properties, and selectivity of autofluorescence from natural pollen by fluorescence microscopy and spectroscopy measurements along with a systematic synthesis of related literature. We show that dry pollen reveals characteristic and reproducible autofluorescence signatures which are shaped by cell wall associated fluorophores, such as phenolic compounds and carotenoid pigments. In addition, fluorescence signals from proteins and chlorophyll a were observed in some species. The abundance and intensity of the individual fluorescence signals show certain taxonomic trends and allow systematic differentiation from bacteria and fungal spores due to the lack of proteins on the grain surface. Principal component analysis was used to explore the discrimination potential of pollen autofluorescence, in combination with size and shape, revealing a differentiation of pollen on family level. Our results help explore the levels of selectivity that autofluorescence-based techniques can provide to PBAP analysis and will support the development and application of autofluorescence-based detectors for monitoring of allergenic pollen in the atmosphere.


2017 ◽  
Vol 10 (3) ◽  
pp. 811-824 ◽  
Author(s):  
W. Reed Espinosa ◽  
Lorraine A. Remer ◽  
Oleg Dubovik ◽  
Luke Ziemba ◽  
Andreas Beyersdorf ◽  
...  

Abstract. A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177°. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.


2014 ◽  
Vol 777 ◽  
pp. 231-236
Author(s):  
R.K. Dutta ◽  
R.M. Huizenga ◽  
M. Amirthalingam ◽  
H. Gao ◽  
A. King ◽  
...  

In-situ phase transformation behaviour of a high strength (830 MPa yield stress) quenched and tempered S690QL1 (Fe-0.16C-0.2Si-0.87Mn-0.33Cr-0.21Mo (wt. %)) structural steel, during continuous cooling under different mechanical loading conditions to promote the bainitic transformation, was studied. Time-temperature-load resolved 2D synchrotron diffraction patterns were recorded and used to calculate the transformation strains. The temperature dependent elastic constants of ferrite in the steel were also determined using \textit{in-situ} tensile tests at different temperatures in a synchrotron X-ray diffractometer. The transformation strains were calculated under different loading conditions.The elastic constants were calculated from the lattice parameters at 25 °C, 200 °C, 300 °C, 400 °C, 500 °C and 600 °C. The elastic constants varied from 202 GPa at 25 °C to 143 GPa at 600 °C. The variation in lattice plane strains during phase transformation under small external loads were calculated. Bulk measurement techniques such as dilatation experiments give the averaged transformation strains. However, in-situ synchrotron measurements performed in this work describe the transformation strains of the individual transforming phases and the strains arising due to possible variant selection.


2014 ◽  
Vol 7 (4) ◽  
pp. 3801-3833 ◽  
Author(s):  
R. L. Herman ◽  
J. E. Cherry ◽  
J. Young ◽  
J. M. Welker ◽  
D. Noone ◽  
...  

Abstract. The EOS Aura Tropospheric Emission Spectrometer (TES) retrieves the atmospheric HDO/H2O ratio in the mid-to-lower troposphere as well as the planetary boundary layer. TES observations of water vapor and the HDO isotopologue have been compared with nearly coincident in situ airborne measurements for direct validation of the TES products. The field measurements were made with a commercially available Picarro L1115-i isotopic water analyzer on aircraft over the Alaskan interior boreal forest during the three summers of 2011 to 2013. TES special observations were utilized in these comparisons. The TES averaging kernels and a priori constraints have been applied to the in situ data, using Version Five (V005) of the TES data. TES calculated errors are compared with the standard deviation (1-σ) of scan-to-scan variability to check consistency with the TES observation error. Spatial and temporal variations are assessed from the in situ aircraft measurements. It is found that the standard deviation of scan-to-scan variability of TES δD is ±34.1‰ in the boundary layer, and ±26.5‰ in the free troposphere. This scan-to-scan variability is consistent with the TES estimated error (observation error) of 10–18‰ after accounting for the atmospheric variations along the TES track of ±16‰ in the boundary layer, increasing to ±30‰ in the free troposphere observed by the aircraft in situ measurements. We estimate that TES V005 δD is biased high by an amount that decreases with pressure: approximately +12.3% at 1000 hPa, +9.8% in the boundary layer, and +3.7% in the free troposphere. The uncertainty in this bias estimate is ±2%. After bias correction, we show that TES has accurate sensitivity to water vapor isotopologues in the boundary layer.


2005 ◽  
Vol 5 (11) ◽  
pp. 2881-2900 ◽  
Author(s):  
C. Hak ◽  
I. Pundt ◽  
S. Trick ◽  
C. Kern ◽  
U. Platt ◽  
...  

Abstract. Results from an intercomparison of several currently used in-situ techniques for the measurement of atmospheric formaldehyde (CH2O) are presented. The measurements were carried out at Bresso, an urban site in the periphery of Milan (Italy) as part of the FORMAT-I field campaign. Eight instruments were employed by six independent research groups using four different techniques: Differential Optical Absorption Spectroscopy (DOAS), Fourier Transform Infra Red (FTIR) interferometry, the fluorimetric Hantzsch reaction technique (five instruments) and a chromatographic technique employing C18-DNPH-cartridges (2,4-dinitrophenylhydrazine). White type multi-reflection systems were employed for the optical techniques in order to avoid spatial CH2O gradients and ensure the sampling of nearly the same air mass by all instruments. Between 23 and 31 July 2002, up to 13 ppbv of CH2O were observed. The concentrations lay well above the detection limits of all instruments. The formaldehyde concentrations determined with DOAS, FTIR and the Hantzsch instruments were found to agree within ±11%, with the exception of one Hantzsch instrument, which gave systematically higher values. The two hour integrated samples by DNPH yielded up to 25% lower concentrations than the data of the continuously measuring instruments averaged over the same time period. The consistency between the DOAS and the Hantzsch method was better than during previous intercomparisons in ambient air with slopes of the regression line not significantly differing from one. The differences between the individual Hantzsch instruments could be attributed in part to the calibration standards used. Possible systematic errors of the methods are discussed.


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