scholarly journals Development of a cavity-enhanced absorption spectrometer for airborne measurements of CH<sub>4</sub> and CO<sub>2</sub>

2013 ◽  
Vol 6 (5) ◽  
pp. 1095-1109 ◽  
Author(s):  
S. J. O'Shea ◽  
S. J.-B. Bauguitte ◽  
M. W. Gallagher ◽  
D. Lowry ◽  
C. J. Percival

Abstract. High-resolution CH4 and CO2 measurements were made on board the FAAM BAe-146 UK (Facility for Airborne Atmospheric Measurements, British Aerospace-146) atmospheric research aircraft during a number of field campaigns. The system was based on an infrared spectrometer using the cavity-enhanced absorption spectroscopy technique. Correction functions to convert the mole fractions retrieved from the spectroscopy to dry-air mole fractions were derived using laboratory experiments and over a 3 month period showed good stability. Long-term performance of the system was monitored using WMO (World Meteorological Office) traceable calibration gases. During the first year of operation (29 flights) analysis of the system's in-flight calibrations suggest that its measurements are accurate to 1.28 ppb (1σ repeatability at 1 Hz = 2.48 ppb) for CH4 and 0.17 ppm (1σ repeatability at 1 Hz = 0.66 ppm) for CO2. The system was found to be robust, no major motion or altitude dependency could be detected in the measurements. An inter-comparison between whole-air samples that were analysed post-flight for CH4 and CO2 by cavity ring-down spectroscopy showed a mean difference between the two techniques of −2.4 ppb (1σ = 2.3 ppb) for CH4 and −0.22 ppm (1σ = 0.45 ppm) for CO2. In September 2012, the system was used to sample biomass-burning plumes in Brazil as part of the SAMBBA project (South AMerican Biomass Burning Analysis). From these and simultaneous CO measurements, emission factors for savannah fires were calculated. These were found to be 2.2 ± 0.2 g (kg dry matter)−1 for CH4 and 1710 ± 171 g (kg dry matter)−1 for CO2, which are in excellent agreement with previous estimates in the literature.

2013 ◽  
Vol 6 (1) ◽  
pp. 1-41 ◽  
Author(s):  
S. J. O'Shea ◽  
S. J.-B. Bauguitte ◽  
M. W. Gallagher ◽  
D. Lowry ◽  
C. J. Percival

Abstract. High-resolution CH4 and CO2 measurements were made onboard the FAAM BAe 146 UK atmospheric research aircraft during a number of field campaigns. The system was based on an infrared spectrometer using the cavity enhanced absorption spectroscopy technique. Correction functions to convert the mole fractions retrieved from the spectroscopy to dry air mole fractions were derived using laboratory experiments and over a 3 month period showed good stability. Long-term performance of the system was monitored using WMO traceable calibration gases. During the first year of operation (29 flights) analysis of the system's in-flight calibrations suggest that its measurements are accurate to −0.07 ppbv (1 σ precision at 1 Hz = 2.48 ppbv) for CH4 and −0.06 ppmv (1 σ precision at 1 Hz = 0.66 ppmv) for CO2. The system was found to be very robust, no major motion or altitude dependency could be detected in the measurements. An inter-comparison between whole air samples that were analysed post-flight for CH4 and CO2 by cavity ring down spectroscopy showed a mean difference between the two techniques of −2.4 ppbv (1 σ = 2.3 ppbv) for CH4 and −0.22 ppmv (1 σ = 0.45 ppmv) for CO2. In September 2012, the system was used to sample biomass burning plumes in Brazil as part of the SAMBBA project (South American biomass burning analysis). From these and simultaneous CO measurements, emission factors for savannah fires were calculated. These were found to be 2.2 ± 0.2 g (kg dry matter)−1 for CH4 and 1710 ± 171 g (kg dry matter)−1 for CO2, which are in excellent agreement with previous estimates in the literature.


2011 ◽  
Vol 4 (3) ◽  
pp. 3499-3544 ◽  
Author(s):  
O. J. Kennedy ◽  
B. Ouyang ◽  
J. M. Langridge ◽  
M. J. S. Daniels ◽  
S. Bauguitte ◽  
...  

Abstract. A three channel broadband cavity enhanced absorption spectroscopy (BBCEAS) instrument has been developed for airborne measurements of atmospheric trace gases involved in night-time oxidation chemistry and air quality. The instrument was deployed on board the Facility for Airborne Atmospheric Measurements BAe 146-301 atmospheric research aircraft during the Role of Nighttime Chemistry in Controlling the Oxidising Capacity of the Atmosphere (RONOCO) measurement campaigns between December 2009 and January 2011. In its present configuration (i.e. specifications of the cavity optics and spectrometers) the instrument is designed to measure NO3, N2O5 (by detection of NO3 after thermal dissociation of N2O5), H2O and NO2 by characterising the wavelength dependent optical attenuation within ambient samples by molecular absorption around 662 nm (NO3 and H2O) and 445 nm (NO2). This paper reports novel advancements in BBCEAS instrumentation including a refined method for performing BBCEAS mirror reflectivity calibrations using measurements of the phase delay introduced by the optical cavities to amplitude modulated radiation. Furthermore, a new methodology is introduced for fitting the strong but unresolved transitions of water vapour, which is required for accurate retrieval of water absorption features from the 662 nm absorption band used to measure NO3 concentrations. The paper also details the first example of airborne measurements of NO3, N2O5 and NO2 over Europe from a flight over the North Sea and Thames Estuary on the night of the 20 July 2010, one of the most polluted days of the RONOCO summertime flying period. As part of this analysis, the performance of the BBCEAS instrument is assessed by comparing airborne NO2 measurements to those reported concurrently by a photolytic chemiluminescence based detector.


2011 ◽  
Vol 4 (9) ◽  
pp. 1759-1776 ◽  
Author(s):  
O. J. Kennedy ◽  
B. Ouyang ◽  
J. M. Langridge ◽  
M. J. S. Daniels ◽  
S. Bauguitte ◽  
...  

Abstract. A three channel broadband cavity enhanced absorption spectroscopy (BBCEAS) instrument has been developed for airborne measurements of atmospheric trace gases involved in night-time oxidation chemistry and air quality. The instrument was deployed on board the Facility for Airborne Atmospheric Measurements BAe 146-301 atmospheric research aircraft during the Role of Nighttime Chemistry in Controlling the Oxidising Capacity of the Atmosphere (RONOCO) measurement campaigns between December 2009 and January 2011. In its present configuration (i.e. specifications of the cavity optics and spectrometers) the instrument is designed to measure NO3, N2O5 (by detection of NO3 after thermal dissociation of N2O5), H2O and NO2 by characterising the wavelength dependent optical attenuation within ambient samples by molecular absorption around 662 nm (NO3 and H2O) and 445 nm (NO2). This paper reports novel advancements in BBCEAS instrumentation including a refined method for performing BBCEAS mirror reflectivity calibrations using measurements of the phase delay introduced by the optical cavities to amplitude modulated radiation. Furthermore, a new methodology is introduced for fitting the strong but unresolved transitions of water vapour, which is required for accurate retrieval of water absorption features from the 662 nm absorption band used to measure NO3 concentrations. The paper also details the first example of airborne measurements of NO3, N2O5 and NO2 over Europe from a flight over the North Sea and Thames Estuary on the night of the 20 July 2010, one of the most polluted days of the RONOCO summertime flying period. As part of this analysis, the performance of the BBCEAS instrument is assessed by comparing airborne NO2 measurements to those reported concurrently by a photolytic chemiluminescence based detector.


2010 ◽  
Vol 4 (4) ◽  
pp. 583-592 ◽  
Author(s):  
L. Kaleschke ◽  
N. Maaß ◽  
C. Haas ◽  
S. Hendricks ◽  
G. Heygster ◽  
...  

Abstract. In preparation for the European Space Agency's (ESA) Soil Moisture and Ocean Salinity (SMOS) mission, we investigated the potential of L-band (1.4 GHz) radiometry to measure sea-ice thickness. Sea-ice brightness temperature was measured at 1.4 GHz and ice thickness was measured along nearly coincident flight tracks during the SMOS Sea-Ice campaign in the Bay of Bothnia in March 2007. A research aircraft was equipped with the L-band Radiometer EMIRAD and coordinated with helicopter based electromagnetic induction (EM) ice thickness measurements. We developed a three layer (ocean-ice-atmosphere) dielectric slab model for the calculation of ice thickness from brightness temperature. The dielectric properties depend on the relative brine volume which is a function of the bulk ice salinity and temperature. The model calculations suggest a thickness sensitivity of up to 1.5 m for low-salinity (multi-year or brackish) sea-ice. For Arctic first year ice the modelled thickness sensitivity is less than half a meter. It reduces to a few centimeters for temperatures approaching the melting point. The campaign was conducted under unfavorable melting conditions and the spatial overlap between the L-band and EM-measurements was relatively small. Despite these disadvantageous conditions we demonstrate the possibility to measure the sea-ice thickness with the certain limitation up to 1.5 m. The ice thickness derived from SMOS measurements would be complementary to ESA's CryoSat-2 mission in terms of the error characteristics and the spatiotemporal coverage. The relative error for the SMOS ice thickness retrieval is expected to be not less than about 20%.


2017 ◽  
Vol 10 (5) ◽  
pp. 1803-1812 ◽  
Author(s):  
Irène Ventrillard ◽  
Irène Xueref-Remy ◽  
Martina Schmidt ◽  
Camille Yver Kwok ◽  
Xavier Faïn ◽  
...  

Abstract. We present the first comparison of carbon monoxide (CO) measurements performed with a portable laser spectrometer that exploits the optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS) technique, against a high-performance automated gas chromatograph (GC) with a mercuric oxide reduction gas detector (RGD). First, measurements of atmospheric CO mole fraction were continuously collected in a Paris (France) suburb over 1 week. Both instruments showed an excellent agreement within typically 2 ppb (part per billion in volume), fulfilling the World Meteorological Organization (WMO) recommendation for CO inter-laboratory comparison. The compact size and robustness of the OF-CEAS instrument allowed its operation aboard a small aircraft employed for routine tropospheric air analysis over the French Orléans forest area. Direct OF-CEAS real-time CO measurements in tropospheric air were then compared with later analysis of flask samples by the gas chromatograph. Again, a very good agreement was observed. This work establishes that the OF-CEAS laser spectrometer can run unattended at a very high level of sensitivity ( <  1 ppb) and stability without any periodic calibration.


2019 ◽  
Author(s):  
Jingwei Liu ◽  
Xin Li ◽  
Yiming Yang ◽  
Haichao Wang ◽  
Yusheng Wu ◽  
...  

Abstract. A system based on incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS) has been developed for simultaneous measurement of nitrogen dioxide (NO2), glyoxal (GLY) and methylglyoxal (MGLY). On this system, the absorption of light around 460 nm is spectrally resolved. The concentration of absorbers is determined from a multi-component fit. At an integration time of 100 s, the measurement sensitivity (2σ) for NO2, GLY, and MGLY can reach 18 ppt, 30 ppt, and 100 ppt, respectively. The measurement uncertainty which mainly originates from path length calibration, sampling loss, and uncertainty of absorption cross sections is estimated to be 8 % for NO2, 8 % for GLY, and 16 % for MGLY. When applying the instrument during field observations, we found significant influence of NO2 on spectra fitting for retrieving GLY and MGLY concentration, which is caused by the fact that NO2 has higher absorption cross section and higher ambient concentration. In order to minimize such an effect, a NO2 photolytic convertor (NPC) which removes sampled NO2 at an efficiency of 76 % was integrated on the IBBCEAS system. Since sampled GLY and MGLY are mostly conserved (≥ 95 %) after passing through the NPC, the quality of the spectra fitting and the measurement accuracy of ambient GLY and MGLY were largely improved.


2019 ◽  
Vol 12 (8) ◽  
pp. 4439-4453 ◽  
Author(s):  
Jingwei Liu ◽  
Xin Li ◽  
Yiming Yang ◽  
Haichao Wang ◽  
Yusheng Wu ◽  
...  

Abstract. A system based on incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) has been developed for simultaneous measurement of nitrogen dioxide (NO2), glyoxal (GLY), and methylglyoxal (MGLY). In this system, the measured light absorption at around 460 nm is spectrally resolved. The concentration of absorbers is determined from a multicomponent fit. At an integration time of 100 s, the measurement sensitivity (2σ) for NO2, GLY, and MGLY is 18, 30, and 100 ppt, respectively. The measurement uncertainty, which mainly originates from path length calibration, sampling loss, and uncertainty of absorption cross sections is estimated to be 8 % for NO2, 8 % for GLY, and 16 % for MGLY. When deploying the instrument during field observations, we found significant influence of NO2 on the spectra fitting for retrieving GLY and MGLY concentrations, which is caused by the fact that NO2 has a higher absorption cross section and higher ambient concentration. In order to minimize such an effect, a NO2 photolytic convertor (NPC), which removes sampled NO2 at an efficiency of 76 %, was integrated on the IBBCEAS system. Since sampled GLY and MGLY are mostly (≥95 %) conserved after passing through the NPC, the quality of the spectra fitting and the measurement accuracy of ambient GLY and MGLY under NO2-rich environments could be improved.


2013 ◽  
Vol 13 (24) ◽  
pp. 12451-12467 ◽  
Author(s):  
S. J. O'Shea ◽  
G. Allen ◽  
M. W. Gallagher ◽  
S. J.-B. Bauguitte ◽  
S. M. Illingworth ◽  
...  

Abstract. In situ airborne measurements were made over eastern Canada in summer 2011 as part of the BORTAS experiment (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites). In this paper we present observations of greenhouse gases (CO2 and CH4) and other biomass burning tracers (CO, HCN and CH3CN), both climatologically and through case studies, as recorded on board the FAAM BAe-146 research aircraft. Vertical profiles of CO2 were generally characterised by depleted boundary layer concentrations relative to the free troposphere, consistent with terrestrial biospheric uptake. In contrast, CH4 concentrations were found to rise with decreasing altitude due to strong local and regional surface sources. BORTAS observations were found to be broadly comparable with both previous measurements in the region during the regional burning season and with reanalysed composition fields from the EU Monitoring Atmospheric Composition and Change (MACC) project. We use coincident tracer–tracer correlations and a Lagrangian trajectory model to characterise and differentiate air mass history of intercepted plumes. In particular, CO, HCN and CH3CN were used to identify air masses that have been recently influenced by biomass burning. Examining individual cases we were able to quantify emissions from biomass burning. Using both near-field (< 1 day) and far-field (> 1 day) sampling, boreal forest fire plumes were identified throughout the troposphere. Fresh plumes from fires in northwestern Ontario yield emission factors for CH4 and CO2 of 8.5 ± 0.9 g (kg dry matter)−1 and 1512 ± 185 g (kg dry matter)−1, respectively. We have also investigated the efficacy of calculating emission factors from far-field sampling, in which there might be expected to be limited mixing with background and other characteristic air masses, and we provide guidance on best practice and limitations in such analysis. We have found that for measurements within plumes that originated from fires in northwestern Ontario 2–4 days upwind, emission factors can be calculated that range between 1618 ± 216 and 1702 ± 173 g (kg dry matter)−1 for CO2 and 1.8 ± 0.2 and 6.1 ± 1 g (kg dry matter)−1 for CH4.


2021 ◽  
Author(s):  
Corinna Kloss ◽  
Vicheith Tan ◽  
J. Brian Leen ◽  
Garrett L. Madsen ◽  
Aaron Gardner ◽  
...  

Abstract. We describe the Airborne Mid-Infrared Cavity enhanced Absorption spectrometer (AMICA) designed to measure trace gases in situ on research aircraft using Off-Axis Integrated Cavity Output Spectroscopy (OA-ICOS). AMICA contains two largely independent and exchangeable OA-ICOS arrangements, allowing for the simultaneous measurement of multiple substances in different infrared wavelength windows tailored to scientific questions related to a particular flight mission. Three OA-ICOS setups have been implemented to measure OCS, CO2, CO and H2O at 2050 cm−1, O3, NH3 and CO2 at 1035 cm−1, and HCN, C2H2 and N2O at 3331 cm−1. The 2050 cm−1 setup has been fully characterized in the lab and successfully used for atmospheric measurements during two campaigns with the research aircraft M55-Geophysica and one with the German HALO aircraft. Nominal measurement precision is 30 ppt for OCS, 1 ppm for CO2, 3 ppb for CO and 100 ppm for H2O. The 1035 and 3331 cm−1 arrangements have only partially been characterized and are still in development. The ~100 kg instrument with a typical in-flight power consumption of about 500 VA is dimensioned to fit into one 19 inch rack typically used for deployment inside the aircraft cabin. Its rugged design and a pressurized and temperature stabilized compartment containing the sensitive optical and electronic hardware also allow for deployment in payload bays outside the pressurized cabin even at high altitudes of 20 km. A sample flow system with two parallel proportional solenoid valves of different size orifices allows for precise regulation of cavity pressure over the wide range of inlet port pressures encountered between the ground and maximum flight altitudes. Sample flow on the order of 1 SLM maintained by an exhaust-side pump limits the useful time resolution to about 2.5 s (corresponding to the average cavity flush time).


2020 ◽  
Vol 12 (10) ◽  
pp. 1557 ◽  
Author(s):  
Aristeidis K. Georgoulias ◽  
Eleni Marinou ◽  
Alexandra Tsekeri ◽  
Emmanouil Proestakis ◽  
Dimitris Akritidis ◽  
...  

We present here the first cloud condensation nuclei (CCN) concentration profiles derived from measurements with the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO), for different aerosol types at a supersaturation of 0.15%. CCN concentrations, along with the corresponding uncertainties, were inferred for a nighttime CALIPSO overpass on 9 September 2011, with coincident observations with the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft, within the framework of the Evaluation of CALIPSO’s Aerosol Classification scheme over Eastern Mediterranean (ACEMED) research campaign over Thessaloniki, Greece. The CALIPSO aerosol typing is evaluated, based on data from the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis. Backward trajectories and satellite-based fire counts are used to examine the origin of air masses on that day. Our CCN retrievals are evaluated against particle number concentration retrievals at different height levels, based on the ACEMED airborne measurements and compared against CCN-related retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard Terra and Aqua product over Thessaloniki showing that it is feasible to obtain CCN concentrations from CALIPSO, with an uncertainty of a factor of two to three.


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