scholarly journals A new Differential Optical Absorption Spectroscopy instrument to study atmospheric chemistry from a high-altitude unmanned aircraft

2017 ◽  
Vol 10 (3) ◽  
pp. 1017-1042 ◽  
Author(s):  
Jochen Stutz ◽  
Bodo Werner ◽  
Max Spolaor ◽  
Lisa Scalone ◽  
James Festa ◽  
...  

Abstract. Observations of atmospheric trace gases in the tropical upper troposphere (UT), tropical tropopause layer (TTL), and lower stratosphere (LS) require dedicated measurement platforms and instrumentation. Here we present a new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument developed for NASA's Global Hawk (GH) unmanned aerial system and deployed during the Airborne Tropical TRopopause EXperiment (ATTREX). The mini-DOAS system is designed for automatic operation under unpressurized and unheated conditions at 14–18 km altitude, collecting scattered sunlight in three wavelength windows: UV (301–387 nm), visible (410–525 nm), and near infrared (900–1700 nm). A telescope scanning unit allows selection of a viewing angle around the limb, as well as real-time correction of the aircraft pitch. Due to the high altitude, solar reference spectra are measured using diffusors and direct sunlight. The DOAS approach allows retrieval of slant column densities (SCDs) of O3, O4, NO2, and BrO with relative errors similar to other aircraft DOAS systems. Radiative transfer considerations show that the retrieval of trace gas mixing ratios from the observed SCD based on O4 observations, the most common approach for DOAS measurements, is inadequate for high-altitude observations. This is due to the frequent presence of low-altitude clouds, which shift the sensitivity of the O4 SCD into the lower atmosphere and make it highly dependent on cloud coverage. A newly developed technique that constrains the radiative transfer by comparing in situ and DOAS O3 observations overcomes this issue. Extensive sensitivity calculations show that the novel O3-scaling technique allows the retrieval of BrO and NO2 mixing ratios at high accuracies of 0.5 and 15 ppt, respectively. The BrO and NO2 mixing ratios and vertical profiles observed during ATTREX thus provide new insights into ozone and halogen chemistry in the UT, TTL, and LS.

2016 ◽  
Author(s):  
Jochen Stutz ◽  
Bodo Werner ◽  
Max Spolaor ◽  
Lisa Scalone ◽  
James Festa ◽  
...  

Abstract. Observations of atmospheric trace gases in the tropical upper troposphere (UT), tropical tropopause layer (TTL) and lower stratosphere (LS) require dedicated measurement platforms and instrumentation. Here we present a new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument developed for NASA’s Global Hawk unmanned aerial system (GH) during the Airborne Tropical TRopopause EXperiment (ATTREX). The mini-DOAS system is designed for automatic operation under unpressurized and unheated conditions at 14–18 km altitude, collecting scattered sunlight in three wavelength windows: UV (301–387 nm), visible (410–525 nm) and near infrared (900–1700 nm). A telescope scanning unit allows selection of a viewing angle around the limb, as well as real-time correction of the aircraft pitch. Due to the high altitude, solar reference spectra are measured using diffusors and direct sunlight. The DOAS approach allows retrieval of slant column densities (SCD) of O3, O4, NO2, and BrO with relative errors similar to other aircraft DOAS systems. Radiative transfer considerations show that the retrieval of trace gas mixing ratios from the observed SCD based on O4 observations, the most common approach for DOAS measurements, is inadequate for high-altitude observations, due to frequent presence of low altitude clouds. A newly developed technique that constrains the radiative transfer (RT) by comparing in-situ and DOAS O3 observations overcomes this issue. Extensive sensitivity calculations show that the novel O3-scaling technique allows the retrieval of BrO and NO2 mixing ratios at high accuracies of 0.3–0.6 ppt and 15 ppt, respectively. The BrO and NO2 mixing ratios and vertical profiles observed during ATTREX thus provide new insights into ozone and halogen chemistry in the UT, TTL, and LS.


2007 ◽  
Vol 7 (5) ◽  
pp. 1293-1303 ◽  
Author(s):  
R. Sinreich ◽  
R. Volkamer ◽  
F. Filsinger ◽  
U. Frieß ◽  
C. Kern ◽  
...  

Abstract. The direct detection of glyoxal (CHOCHO), the smallest α-dicarbonyl, in the open atmosphere by active differential optical absorption spectroscopy (DOAS) has recently been demonstrated (Volkamer et al., 2005a) and triggered the very recent successful detection of CHOCHO from space (Kurosu et al., 2005; Wittrock et al., 2006; Beirle et al., 2006). Here we report the first comprehensive analysis of CHOCHO by passive multi axis differential optical absorption spectroscopy (MAX-DOAS). CHOCHO and NO2 slant column measurements were conducted at the Massachusetts Institute of Technology (MIT), Cambridge, USA, and on board the research vessel Ron Brown in the Gulf of Maine as part of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) 2004 campaign. For a day with nearly clear sky conditions, radiative transfer modeling was employed to derive diurnal CHOCHO mixing ratios in the planetary boundary layer (PBL) for both sites. CHOCHO mixing ratios at MIT varied from 40 to 140 ppt, with peak values observed around noon. Mixing ratios over the Gulf of Maine were found to be up to 2.5 times larger than at MIT. The CHOCHO-to-NO2 ratio at MIT was <0.03, and enhancements of this ratio by up to two orders of magnitude were found over the Gulf of Maine. This paper focuses on the methodological aspects involved with MAX-DOAS measurements of CHOCHO.


2009 ◽  
Vol 9 (5) ◽  
pp. 21371-21398 ◽  
Author(s):  
K. Seitz ◽  
J. Buxmann ◽  
D. Pöhler ◽  
T. Sommer ◽  
J. Tschritter ◽  
...  

Abstract. We present investigations of the reactive iodine species (RIS) IO, OIO and I2 in a coastal region from a field campaign simultaneously employing active long path differential optical absorption spectroscopy (LP-DOAS) as well as passive multi-axis differential optical absorption spectroscopy (MAX-DOAS). The campaign took place at the Martin Ryan Institute (MRI) in Carna, County Galway at the Irish West Coast about 6 km south-east of the atmospheric research station Mace Head in summer 2007. In order to study the horizontal distribution of the trace gases of interest, we established two almost parallel active LP-DOAS light paths, the shorter of 1034 m length just crossing the intertidal area, whereas the longer one of 3946 m length also crossed open water during periods of low tide. In addition we operated two passive Mini-MAX-DOAS instruments with the same viewing direction. While neither OIO nor I2 could be unambiguously identified with any of the instruments, IO could be detected with active as well as passive DOAS. The IO column densities seen at both active LP-DOAS light paths are almost the same. Thus it can be concluded that coastal IO is almost exclusively located in the intertidal area, where we detected mixing ratios of up to 35±7.7 ppt (equivalent to pmol/mol). Nucleation events with particle concentrations of 106 cm−3 particles were observed each day correlating with high IO mixing ratios. Therefore we feel that our detected IO concentrations confirm the results of model studies, which state that in order to explain such particle bursts, IO mixing ratios of 50 to 100 ppt in so called "hot-spots" are required.


2019 ◽  
Vol 12 (11) ◽  
pp. 5959-5977 ◽  
Author(s):  
André Seyler ◽  
Andreas C. Meier ◽  
Folkard Wittrock ◽  
Lisa Kattner ◽  
Barbara Mathieu-Üffing ◽  
...  

Abstract. This study describes a novel application of an “onion-peeling” approach to multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of shipping emissions aiming at investigating the strong horizontal inhomogeneities in NO2 over a shipping lane. To monitor ship emissions on the main shipping route towards the port of Hamburg, a two-channel (UV and visible) MAX-DOAS instrument was deployed on the island Neuwerk in the German Bight, 6–7 km south of the main shipping lane. Utilizing the fact that the effective light path length in the atmosphere depends systematically on wavelength, simultaneous measurements and DOAS retrievals in the UV and visible spectral ranges are used to probe air masses at different horizontal distances to the instrument to estimate two-dimensional pollutant distributions. Two case studies have been selected to demonstrate the ability to derive the approximate plume positions in the observed area. A situation with northerly wind shows high NO2 concentrations close to the measurement site and low values in the north of the shipping lane. The opposite situation with southerly wind, unfavorable for the on-site in situ instrumentation, demonstrates the ability to detect enhanced NO2 concentrations several kilometers away from the instrument. Using a Gaussian plume model, in-plume NO2 volume mixing ratios can be derived from the MAX-DOAS measurements. For validation, a comparison to airborne imaging DOAS measurements during the NOSE campaign in July 2013 is performed, showing good agreement between the approximate plume position derived from the onion-peeling MAX-DOAS and the airborne measurements as well as between the derived in-plume NO2 volume mixing ratios (VMRs).


2007 ◽  
Vol 7 (7) ◽  
pp. 1809-1833 ◽  
Author(s):  
T. Wagner ◽  
J. P. Burrows ◽  
T. Deutschmann ◽  
B. Dix ◽  
C. von Friedeburg ◽  
...  

Abstract. The results of a comparison exercise of radiative transfer models (RTM) of various international research groups for Multiple AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) viewing geometry are presented. Besides the assessment of the agreement between the different models, a second focus of the comparison was the systematic investigation of the sensitivity of the MAX-DOAS technique under various viewing geometries and aerosol conditions. In contrast to previous comparison exercises, box-air-mass-factors (box-AMFs) for different atmospheric height layers were modelled, which describe the sensitivity of the measurements as a function of altitude. In addition, radiances were calculated allowing the identification of potential errors, which might be overlooked if only AMFs are compared. Accurate modelling of radiances is also a prerequisite for the correct interpretation of satellite observations, for which the received radiance can strongly vary across the large ground pixels, and might be also important for the retrieval of aerosol properties as a future application of MAX-DOAS. The comparison exercises included different wavelengths and atmospheric scenarios (with and without aerosols). The strong and systematic influence of aerosol scattering indicates that from MAX-DOAS observations also information on atmospheric aerosols can be retrieved. During the various iterations of the exercises, the results from all models showed a substantial convergence, and the final data sets agreed for most cases within about 5%. Larger deviations were found for cases with low atmospheric optical depth, for which the photon path lengths along the line of sight of the instrument can become very large. The differences occurred between models including full spherical geometry and those using only plane parallel approximation indicating that the correct treatment of the Earth's sphericity becomes indispensable. The modelled box-AMFs constitute an universal data base for the calculation of arbitrary (total) AMFs by simple convolution with a given trace gas concentration profile. Together with the modelled radiances and the specified settings for the various exercises, they can serve as test cases for future RTM developments.


2010 ◽  
Vol 10 (5) ◽  
pp. 2117-2128 ◽  
Author(s):  
K. Seitz ◽  
J. Buxmann ◽  
D. Pöhler ◽  
T. Sommer ◽  
J. Tschritter ◽  
...  

Abstract. We present investigations of the reactive iodine species (RIS) IO, OIO and I2 in a coastal region from a field campaign simultaneously employing active long path differential optical absorption spectroscopy (LP-DOAS) as well as passive multi-axis differential optical absorption spectroscopy (MAX-DOAS). The campaign took place at the Martin Ryan Institute (MRI) in Carna, County Galway at the Irish West Coast about 6 km south-east of the atmospheric research station Mace Head in summer 2007. In order to study the horizontal distribution of the trace gases of interest, we established two almost parallel active LP-DOAS light paths, the shorter of 1034 m length just crossing the intertidal area, whereas the longer one of 3946 m length also crossed open water during periods of low tide. In addition we operated two passive Mini-MAX-DOAS instruments with the same viewing direction. While neither OIO nor I2 could be unambiguously identified with any of the instruments, IO could be detected with active as well as passive DOAS. The IO column densities seen at both active LP-DOAS light paths are almost the same. Thus it can be concluded that coastal IO is almost exclusively located in the intertidal area, where we detected mixing ratios of up to 29±8.8 ppt (equivalent to pmol/mol). Nucleation events with particle concentrations of 106 cm−3 particles were observed each day correlating with high IO mixing ratios. Therefore we feel that our detected IO concentrations confirm the results of model studies, which state that in order to explain such particle bursts, IO mixing ratios of 50 to 100 ppt in so called "hot-spots" are required.


2006 ◽  
Vol 6 (5) ◽  
pp. 9823-9876 ◽  
Author(s):  
T. Wagner ◽  
J. P. Burrows ◽  
T. Deutschmann ◽  
B. Dix ◽  
C. von Friedeburg ◽  
...  

Abstract. The results of a comparison exercise of radiative transfer models (RTM) of various international research groups for Multiple AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) viewing geometry are presented. In contrast to previous comparison exercises, box-air-mass-factors (box-AMFs) for various atmospheric height layers were modelled, which describe the sensitivity of the measurements as a function of altitude. In addition, radiances were calculated allowing the identification of potential errors, which might be overlooked if only AMFs are compared. Accurate modelling of radiances is also a prerequisite for the correct interpretation of satellite observations, for which the received radiance can strongly vary across the large ground pixels, and might be also important for the retrieval of aerosol properties as a future application of MAX-DOAS. The comparison exercises included different wavelengths and atmospheric scenarios (with and without aerosols). The results were systematically investigated with respect to their dependence on the telescope's elevation angle and the azimuth angle. For both dependencies, a strong and systematic influence of aerosol scattering was found indicating that from MAX-DOAS observations also information on atmospheric aerosols can be retrieved. During the various iterations of the exercises, the results from all models showed a substantial convergence, and the final data sets agreed for most cases within about 5%. Larger deviations were found for cases with low atmospheric optical depth, for which the photon path lengths along the line of sight of the instrument can become very large. The differences occurred between models including full spherical geometry and those using only plane parallel approximation indicating that the correct treatment of the Earth's sphericity becomes indispensable. The modelled box-AMFs constitute an universal data base for the calculation of arbitrary (total) AMFs by simple convolution with a given trace gas concentration profile. Together with the modelled radiances and the specified settings for the various exercises, they can serve as test cases for future RTM developments.


2008 ◽  
Vol 8 (24) ◽  
pp. 7595-7601 ◽  
Author(s):  
E. Frins ◽  
U. Platt ◽  
T. Wagner

Abstract. Topographic Target Light scattering – Differential Optical Absorption Spectroscopy (ToTaL-DOAS), also called Target-DOAS, is a novel experimental procedure to retrieve trace gas concentrations present in the low atmosphere. Scattered sunlight (diffuse or specular) reflected from natural or artificial targets located at different distances are analyzed to retrieve the spatial distribution of the concentration of different trace gases like NO2, SO2 and others. We report high spatial resolution measurements of NO2 mixing ratios in the city of Montevideo (Uruguay) observing three buildings as targets with a Mini-DOAS instrument. Our instrument was 146 m, 196 m, and 280 m apart from three different buildings located along a main Avenue. We obtain temporal variation of NO2 mixing ratios between 30 ppb and 65 ppb from measurements of November 2007 and mixing ratios up to 50 ppb from measurements of August and September 2008. Our measurements demonstrate that ToTaL-DOAS observations can be made over relative short distances. In polluted air masses, the retrieved absorption signal was found to be sufficiently strong to allow measurements over distances in the range of several tens of meters.


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