scholarly journals The Heidelberg Airborne Imaging DOAS Instrument (HAIDI) – a novel imaging DOAS device for 2-D and 3-D imaging of trace gases and aerosols

2014 ◽  
Vol 7 (10) ◽  
pp. 3459-3485 ◽  
Author(s):  
S. General ◽  
D. Pöhler ◽  
H. Sihler ◽  
N. Bobrowski ◽  
U. Frieß ◽  
...  
Keyword(s):  
Trace Gases ◽  
Tropospheric Chemistry ◽  
Optical Absorption Spectroscopy ◽  
Sources And Sinks ◽  
Volcanic Plumes ◽  
New Instrument ◽  
First Results ◽  
Mt Etna ◽  
Airborne Imaging ◽  
Ccd Detectors

Abstract. Many relevant processes in tropospheric chemistry take place on rather small scales (e.g., tens to hundreds of meters) but often influence areas of several square kilometer. Thus, measurements of the involved trace gases with high spatial resolution are of great scientific interest. In order to identify individual sources and sinks and ultimately to improve chemical transport models, we developed a new airborne instrument, which is based on the well established Differential Optical Absorption Spectroscopy (DOAS) method. The Heidelberg Airborne Imaging DOAS Instrument (HAIDI) is a passive imaging DOAS spectrometer, which is capable of recording horizontal and vertical trace gas distributions with a resolution of better than 100 m. Observable species include NO2, HCHO, C2H2O2, H2O, O3, O4, SO2, IO, OClO and BrO. Here we give a technical description of the instrument including its custom-built spectrographs and CCD detectors. Also first results from measurements with the new instrument are presented. These comprise spatial resolved SO2 and BrO in volcanic plumes, mapped at Mt. Etna (Sicily, Italy), NO2 emissions in the metropolitan area of Indianapolis (Indiana, USA) as well as BrO and NO2 distributions measured during arctic springtime in context of the BRomine, Ozone, and Mercury EXperiment (BROMEX) campaign, which was performed 2012 in Barrow (Alaska, USA).

scholarly journals The Heidelberg Airborne Imaging DOAS Instrument (HAIDI) – a novel Imaging DOAS device for 2-D and 3-D imaging of trace gases and aerosols

2014 ◽  
Vol 7 (3) ◽  
pp. 2187-2257 ◽  
Author(s):  
S. General ◽  
D. Pöhler ◽  
H. Sihler ◽  
N. Bobrowski ◽  
U. Frieß ◽  
...  
Keyword(s):  
Trace Gases ◽  
Tropospheric Chemistry ◽  
Passive Imaging ◽  
Sources And Sinks ◽  
Volcanic Plumes ◽  
New Instrument ◽  
First Results ◽  
Mt Etna ◽  
Airborne Imaging ◽  
Ccd Detectors

Abstract. Many relevant processes in tropospheric chemistry take place on rather small scales (e.g. tens to hundreds of meters) but often influence areas of several square kilometer. Thus, measurements of the involved trace gases with high spatial resolution are of great scientific interest. In order to identify individual sources and sinks and ultimately to improve chemical transport models, we developed a new airborne instrument, which is based on the well established DOAS method. The Heidelberg Airborne Imaging Differential Optical Absorption Spectrometer Instrument (HAIDI) is a passive imaging DOAS spectrometer, which is capable of recording horizontal and vertical trace gas distributions with a resolution of better than 100 m. Observable species include NO2, HCHO, C2H2O2, H2O, O3, O4, SO2, IO, OClO and BrO. Here we report a technical description of the instrument including its custom build spectrographs and CCD detectors. Also first results from measurements with the new instrument are presented. These comprise spatial resolved SO2 and BrO in volcanic plumes, mapped at Mt. Etna (Sicily, Italy), NO2 emissions in the metropolitan area of Indianapolis (Indiana, USA) as well as BrO and NO2 distributions measured during arctic springtime in context of the BROMEX campaign, which was performed 2012 in Barrow (Alaska, USA).

scholarly journals Direct observation of two dimensional trace gas distribution with an airborne Imaging DOAS instrument

2008 ◽  
Vol 8 (3) ◽  
pp. 11879-11907 ◽  
Author(s):  
K.-P. Heue ◽  
T. Wagner ◽  
S. P. Broccardo ◽  
D. Walter ◽  
S. J. Piketh ◽  
...  
Keyword(s):  
Power Plants ◽  
Trace Gases ◽  
Tropospheric Chemistry ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Small Scale ◽  
Two Dimensional ◽  
Gas Distribution ◽  
Dimensional Distribution ◽  
Airborne Imaging

Abstract. In many investigations of tropospheric chemistry information about the two dimensional distribution of trace gases on a small scale (e.g. tens to hundreds of meters) is highly desirable. An airborne instrument based on imaging Differential Optical Absorption Spectroscopy has been built to map the 2-D distribution of a series of relevant trace gases including NO2, HCHO, C2H2O2, H2O, O4, SO2, and BrO on a scale of 100 m. Here we report on the first tests of the novel aircraft instrument over the industrialised South African Highveld, where large variations in NO2 column densities in the immediate vicinity of several sources e.g. power plants or steel works, were measured. The observed patterns in the trace gas distribution are interpreted with respect to flux estimates, and it is seen that the fine resolution of the measurements allows separate sources in close proximity to one another to be distinguished.

scholarly journals Direct observation of two dimensional trace gas distributions with an airborne Imaging DOAS instrument

2008 ◽  
Vol 8 (22) ◽  
pp. 6707-6717 ◽  
Author(s):  
K.-P. Heue ◽  
T. Wagner ◽  
S. P. Broccardo ◽  
D. Walter ◽  
S. J. Piketh ◽  
...  
Keyword(s):  
Power Plants ◽  
Trace Gases ◽  
Tropospheric Chemistry ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Small Scale ◽  
Two Dimensional ◽  
Dimensional Distribution ◽  
Airborne Imaging ◽  
Fine Resolution

Abstract. In many investigations of tropospheric chemistry information about the two dimensional distribution of trace gases on a small scale (e.g. tens to hundreds of metres) is highly desirable. An airborne instrument based on imaging Differential Optical Absorption Spectroscopy has been built to map the two dimensional distribution of a series of relevant trace gases including NO2, HCHO, C2H2O2, H2O, O4, SO2, and BrO on a scale of 100 m. Here we report on the first tests of the novel aircraft instrument over the industrialised South African Highveld, where large variations in NO2 column densities in the immediate vicinity of several sources e.g. power plants or steel works, were measured. The observed patterns in the trace gas distribution are interpreted with respect to flux estimates, and it is seen that the fine resolution of the measurements allows separate sources in close proximity to one another to be distinguished.

scholarly journals MAX-DOAS measurements of NO<sub>2</sub>, SO<sub>2</sub>, HCHO, and BrO at the Mt. Waliguan WMO GAW global baseline station in the Tibetan Plateau

2020 ◽  
Vol 20 (11) ◽  
pp. 6973-6990 ◽  
Author(s):  
Jianzhong Ma ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Junli Jin ◽  
Siyang Cheng ◽  
...  
Keyword(s):  
Tibetan Plateau ◽  
Trace Gases ◽  
Elevation Angle ◽  
Lower Troposphere ◽  
Statistical Error ◽  
Tropospheric Chemistry ◽  
Ozone Production ◽  
Optical Absorption Spectroscopy ◽  
The Tibetan Plateau ◽  
Mixing Ratios

Abstract. Mt. Waliguan Observatory (WLG) is a World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) global baseline station in China. WLG is located at the northeastern part of the Tibetan Plateau (36∘17′ N, 100∘54′ E, 3816 m a.s.l.) and is representative of the pristine atmosphere over the Eurasian continent. We made long-term ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements at WLG during the period 2012–2015. In this study, we retrieve the differential slant column densities (dSCDs) and estimate the tropospheric background mixing ratios of different trace gases, including NO2, SO2, HCHO, and BrO, using the measured spectra at WLG. Averaging of 10 original spectra is found to be an “optimum option” for reducing both the statistical error of the spectral retrieval and systematic errors in the analysis. The dSCDs of NO2, SO2, HCHO, and BrO under clear-sky and low-aerosol-load conditions are extracted from measured spectra at different elevation angles at WLG. By performing radiative transfer simulations with the model TRACY-2, we establish approximate relationships between the trace gas dSCDs at 1∘ elevation angle and the corresponding average tropospheric background volume mixing ratios. Mixing ratios of these trace gases in the lower troposphere over WLG are estimated to be in a range of about 7 ppt (January) to 100 ppt (May) for NO2, below 0.5 ppb for SO2, between 0.4 and 0.9 ppb for HCHO, and lower than 0.3 ppt for BrO. The chemical box model simulations constrained by the NO2 concentration from our MAX-DOAS measurements show that there is a little net ozone loss (−0.8 ppb d−1) for the free-tropospheric conditions and a little net ozone production (0.3 ppb d−1) for the boundary layer conditions over WLG during summertime. Our study provides valuable information and data sets for further investigating tropospheric chemistry in the background atmosphere and its links to anthropogenic activities.

scholarly journals Observations of Atmospheric NO2 Using a New Low-Cost MAX-DOAS System

Atmosphere ◽  
2020 ◽  
Vol 11 (2) ◽  
pp. 129 ◽  
Author(s):  
Adrian Roşu ◽  
Daniel-Eduard Constantin ◽  
Mirela Voiculescu ◽  
Maxim Arseni ◽  
Alexis Merlaud ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Optical Absorption ◽  
Low Cost ◽  
Trace Gases ◽  
Elevation Angle ◽  
Local Source ◽  
Optical Absorption Spectroscopy ◽  
Optic System ◽  
First Results ◽  
Spectroscopy System

This article describes the prototype of a new MAX-DOAS (multi-axis differential optical absorption spectroscopy) system built at “Dunarea de Jos” University of Galati (UGAL), Romania, and the first results of its use to observe NO2 content over Galati city (45.42° N, 28.04° E). The new equipment is a ground-based MAX-DOAS system capable of measuring the spatial distribution of DSCD (differential slant column densities) of several trace gases using horizontal and vertical observations. The new optic system, named UGAL-2-DOAS, is an in-house, low-cost, solution in comparison to the existing market of the MAX-DOAS systems. This paper describes the technical design and capabilities of the new MAX-DOAS instrument. The UGAL-2D-DOAS system was tested in April and June 2017 in Galati city. Measurements over three days were selected for the present manuscript. Full azimuthal (0–360°), local celestial meridian observations and other elevation angle sequence measurements (e.g., E–W) were performed. We found that the new MAX-DOAS system is able to detect diurnal variation and the local source emissions of NO2 from the urban environment. Also, we present concomitant zenith-sky car-DOAS observations measurements around the location of the new MAX-DOAS instrument. Comparing the horizontal scanning sequence of the new developed instrument with the mobile DOAS observations, we found that both systems can indicate and detect the same NO2 sources.

scholarly journals OClO and BrO observations in the volcanic plume of Mt. Etna – implications on the chemistry of chlorine and bromine species in volcanic plumes

2014 ◽  
Vol 14 (18) ◽  
pp. 25213-25280
Author(s):  
J. Gliß ◽  
N. Bobrowski ◽  
L. Vogel ◽  
U. Platt
Keyword(s):  
Early Morning ◽  
Optical Absorption Spectroscopy ◽  
Volcanic Plume ◽  
Plume Dispersion ◽  
Strong Indication ◽  
Volcanic Plumes ◽  
Mixing Ratios ◽  
Rate Of Increase ◽  
Mt Etna ◽  
The Impact

Abstract. Spatial and temporal profiles of chlorine dioxide (OClO), bromine monoxide (BrO) and sulphur dioxide (SO2) were measured in the plume of Mt. Etna, Italy, in September 2012 using Multi-Axis-Differential-Optical-Absorption-Spectroscopy (MAX-DOAS). OClO (BrO) was detected in 119 (452) individual measurements covering plume ages up to 6 (23) minutes. The retrieved slant column densities (SCDs) reached values up to 2.0 × 1014 molecules cm−2 (OClO) and 1.1 × 1015 molecules cm−2 (BrO). In addition, the spectra were analysed for signatures of IO, OIO and OBrO, none of these species could be detected. The corresponding detection limits for IO / SO2, OIO / SO2 and OBrO / SO2 were 1.8 × 10−6, 2.0 × 10−5 and 1.1 × 10−5 respectively. The measurements were performed at plume ages (τ) from zero to 23 min downwind the emission source. The chemical variability of BrO and OClO in the plume was studied analysing the OClO / SO2 and BrO / SO2-ratio. A marked increase of both ratios was observed in the young plume (τ < 3 min) and a levelling off at larger plume ages (τ > 3 min) with mean abundances of 3.17 × 10−5 (OClO / SO2), 1.55 × 10−4 (BrO / SO2) and 0.16 (OClO / BrO). Furthermore, enhanced BrO/SO2-ratios were found at the plume edges (by ~30–37%) and a strong indication of enhanced OClO / SO2-ratios as well (~10–250%). A measurement performed in the early morning (05:20–06:20 UTC, sunrise: 04:40 UTC) showed an BrO / SO2-ratio increasing with time until 05:35 UTC and a constant ratio afterwards. Observing this increase was only possible due to a correction for stratospheric BrO signals in the plume spectra. The corresponding OClO / SO2-ratio showed a similar trend stabilising around 06:13 UTC, approximately 40 min later than BrO. This is another strong indication for the photochemical nature of the reactions involved in the formation of oxidised halogens in volcanic plumes. In particular, these findings support the current understanding of the underlying chemistry, namely, that BrO is formed in an autocatalytic reaction mechanism in literature often referred to as "bromine explosion" and that OClO is formed in the "BrO + ClO"-reaction. BrO and OClO concentrations were estimated from the measured SCDs assuming a circular plume shape. In addition, mixing ratios of ClO were determined from the retrieved OClO and BrO-SCDs assuming chemical equilibrium between formation of OClO (BrO + ClO) and its destruction (photolysis). Mean abundances in the young plume (τ<4 min) were BrO = 1.35 ppb, OClO = 300 ppt and ClO = 139 ppt with peak values of 600 ppt (OClO), 2.7 ppb (BrO) and 235 ppt (ClO) respectively. The prevailing Cl-atom concentrations in the plume could be estimated from the rate of increase of OClO and BrO in the young plume and the determined ClO and OClO concentrations. Values between 5.1 × 106 cm−3 (at 40 ppb O3) and 2.1 × 108 cm−3 (at 1 ppb O3) were found. Based on that, a potential – chlorine induced – depletion of tropospheric methane (CH4) in the plume was investigated. CH4-lifetimes between 13 h (at 1 ppb O3) and 23 days (at 40 ppb O3) were found. These are considerably small compared to the atmospheric lifetime of CH4. However, the impact of gaseous chlorine on the CH4-budget in the plume environment was assessed to be relatively small, mainly due to plume dispersion (decrease of Cl number densities) and permanent mixing of the plume with the surrounding atmosphere (net supply of O3 and CH4).

Long-term MAX-DOAS measurements of formaldehyde in the suburban area of London 

2021 ◽  
Author(s):  
Sebastian Donner ◽  
Steffen Dörner ◽  
Joelle Buxmann ◽  
Steffen Beirle ◽  
David Campbell ◽  
...  
Keyword(s):  
Trace Gases ◽  
Lower Troposphere ◽  
Anthropogenic Pollution ◽  
Tropospheric Chemistry ◽  
Atmospheric Composition ◽  
Optical Absorption Spectroscopy ◽  
Vertical Column ◽  
Pollution Levels ◽  
Measurement Site ◽  
Prevailing Wind Direction

&lt;p&gt;Multi-AXis (MAX)-Differential Optical Absorption Spectroscopy (DOAS) instruments record spectra of scattered sun light under different elevation angles. From such measurements tropospheric vertical column densities (VCDs) and vertical profiles of different atmospheric trace gases and aerosols can be determined for the lower troposphere. These measurements allow a simultaneous observation of multiple trace gases, e.g. formaldehyde (HCHO), glyoxal (CHOCHO) and nitrogen dioxide (NO&lt;sub&gt;2&lt;/sub&gt;), with the same measurement setup. Since November 2018, a MAX-DOAS instrument has been operating at Bayfordbury Observatory, which is located approximately 30 km north of London. This measurement site is operated by the University of Hertfordshire and equipped with an AERONET station, a LIDAR and multiple instruments to measure meteorological quantities and solar radiation. Depending on the prevailing wind direction the air masses at the measurement site can be dominated by the pollution of London (SE to SW winds) or rather pristine air (northerly winds).&lt;/p&gt;&lt;p&gt;First results already showed that the highest formaldehyde and glyoxal columns are observed for southerly to southeasterly winds indicating the influence of the anthropogenic emissions of London. However, the detailed patterns of the different trace gases were found to be more complex. Therefore, this measurement site is well suited to study the influence of anthropogenic pollution on the atmospheric composition and chemistry at a rather pristine location in the vicinity of London, a major European capital with about 10 million inhabitants and 4 major international airports.&lt;/p&gt;&lt;p&gt;In this study, trace gas and aerosol profiles are retrieved using the MAinz Profile Algorithm (MAPA) with a focus on tropospheric HCHO which plays an important role in tropospheric chemistry. The HCHO results are combined with the results of other trace species such as NO&lt;sub&gt;2&lt;/sub&gt;, CHOCHO and aerosols in order to identify pollution levels, emission sources and different chemical regimes.&lt;/p&gt;

scholarly journals OClO and BrO observations in the volcanic plume of Mt. Etna – implications on the chemistry of chlorine and bromine species in volcanic plumes

2015 ◽  
Vol 15 (10) ◽  
pp. 5659-5681 ◽  
Author(s):  
J. Gliß ◽  
N. Bobrowski ◽  
L. Vogel ◽  
D. Pöhler ◽  
U. Platt
Keyword(s):  
Heterogeneous Reaction ◽  
Early Morning ◽  
Optical Absorption Spectroscopy ◽  
Volcanic Plume ◽  
Plume Dispersion ◽  
Volcanic Plumes ◽  
Mixing Ratios ◽  
New Findings ◽  
Mt Etna ◽  
The Impact

Abstract. Spatial and temporal profiles of chlorine dioxide (OClO), bromine monoxide (BrO) and sulfur dioxide (SO2) of the volcanic plume at Mt. Etna, Italy, were investigated in September 2012 using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS). OClO was detected in 119 individual measurements covering plume ages up to 6 min. BrO could be detected in 452 spectra up to 23 min downwind. The retrieved slant column densities (SCDs) reached maximum values of 2.0 × 1014 molecules cm-2 (OClO) and 1.1 × 1015 molecules cm-2 (BrO). Mean mixing ratios of BrO and OClO were estimated assuming a circular plume cross section. Furthermore, ClO mixing ratios were derived directly from the BrO and OClO-SCDs. Average abundances of BrO = 1.35 ppb, OClO = 300 ppt and ClO = 139 ppt were found in the young plume (plume age τ < 4 min) with peak values of 2.7 ppb (BrO), 600 ppt (OClO) and 235 ppt (ClO) respectively. The chemical evolution of BrO and OClO in the plume was investigated in great detail by analysing the OClO/SO2 and BrO/SO2 ratios as a function of plume age τ. A marked increase of both ratios was observed in the young plume (τ < 142 s) and a levelling off at larger plume ages showing mean SO2 ratios of 3.17 × 10-5 (OClO/SO2) and 1.65 × 10-4 (BrO/SO2). OClO was less abundant in the plume compared to BrO with a mean OClO/BrO ratio of 0.16 at plume ages exceeding 3 min. A measurement performed in the early morning at low solar radiances revealed BrO/SO2 and OClO/SO2 ratios increasing with time. This observation substantiates the importance of photochemistry regarding the formation of BrO and OClO in volcanic plumes. These findings support the current understanding of the underlying chemistry, namely, that BrO is formed in an autocatalytic, heterogeneous reaction mechanism (in literature often referred to as "bromine explosion") and that OClO is formed in the reaction of OClO with BrO. These new findings, especially the very detailed observation of the BrO and OClO formation in the young plume, were used to infer the prevailing Cl-atom concentrations in the plume. Relatively small values ranging from [Cl] = 2.5 × 106 cm-3 (assuming 80 ppb background O3) to [Cl] = 2.0 × 108 cm-3 (at 1 ppb O3) were calculated at plume ages of about 2 min. Based on these Cl abundances, a potential – chlorine-induced – depletion of tropospheric methane (CH4) in the plume was investigated. CH4 lifetimes between 14 h (at 1 ppb O3) and 47 days (at 80 ppb O3) were derived. While these lifetimes are considerably shorter than the atmospheric lifetime of CH4, the impact of gaseous chlorine on the CH4 budget in the plume environment should nevertheless be relatively small due to plume dispersion (decreasing Cl concentrations) and ongoing mixing of the plume with the surrounding atmosphere (replenishing O3 and CH4). In addition, all spectra were analysed for signatures of IO, OIO and BrO. None of these species could be detected. Upper limits for IO/SO2, OIO/SO2 and OBrO/SO2 are 1.8 × 10-6, 2.0 × 10-5 and 1.1 × 10-5 respectively.

scholarly journals The CU 2-dimensional MAX-DOAS instrument – Part 1: Retrieval of NO<sub>2</sub> in 3 dimensions and azimuth dependent OVOC ratios

2014 ◽  
Vol 7 (11) ◽  
pp. 11653-11709 ◽  
Author(s):  
I. Ortega ◽  
T. Koenig ◽  
R. Sinreich ◽  
D. Thomson ◽  
R. Volkamer
Keyword(s):  
Boundary Layer ◽  
Trace Gases ◽  
Elevation Angle ◽  
Tropospheric Chemistry ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
High Time Resolution ◽  
Vertical Profiles ◽  
Near Surface

Abstract. We present an innovative instrument telescope, and describe a retrieval method to probe 3-D distributions of atmospheric trace gases that are relevant to air pollution and tropospheric chemistry. The University of Colorado (CU) two dimensional (2-D) Multi-AXis-Differential Optical Absorption Spectroscopy (CU 2D-MAX-DOAS) instrument measures nitrogen dioxide (NO2), formaldehyde (HCHO), glyoxal (CHOCHO), oxygen dimer (O2-O2, or O4) and water vapor (H2O); also nitrous acid (HONO), bromine monoxide (BrO), iodine monoxide (IO) among other gases can in principle be measured. Information about aerosols is derived through coupling with a radiative transfer model (RTM). The 2-D telescope has 3 modes of operation: (mode 1) measures solar scattered photons from any pair of elevation angle (−20° < EA < +90° or zenith; zero is to the horizon) and azimuth angle (−180° < AA < +180°; zero being North), (mode 2) measures any set of AA at constant EA (almucantar scans); and (mode 3) tracks the direct solar beam via a separate view port. Vertical profiles of trace gases are measured, and used to estimate planetary boundary layer height (PBL). Horizontal distributions are then derived using PBL and parameterization of RTM (Sinreich et al., 2013). NO2 is evaluated at different wavelengths (350, 450, and 560 nm), exploiting the fact that the effective path length varies systematically with wavelength. The area probed is constrained by O4 observations at nearby wavelengths, and has an effective radius of 7.5 to 20 km around the instrument location; i.e., up to 1250 km2 can be sampled near-instantaneously, and with high time resolution. The instrument was deployed as part of the Multi Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany from 7 June to 6 July 2013. We present first measurements (modes 1 and 2 only) and describe a four-step retrieval to derive (a) boundary layer vertical profiles of NO2 and PBL; (b) near-surface horizontal distributions of NO2; (c) range resolved NO2 horizontal distribution measurements using an "onion peeling" approach; and (d) the ratios HCHO-to-NO2 (RFN), CHOCHO-to-NO2 (RGN), and CHOCHO-to-HCHO (RGF) at 14 pre-set azimuth angles distributed over a 360° view. 2D-MAX-DOAS provides an innovative, regional perspective about trace gases, their spatial and temporal concentration gradients, and maximizes information to compare near-surface observations with atmospheric models and satellites.

scholarly journals The CU 2-D-MAX-DOAS instrument – Part 1: Retrieval of 3-D distributions of NO<sub>2</sub> and azimuth-dependent OVOC ratios

2015 ◽  
Vol 8 (6) ◽  
pp. 2371-2395 ◽  
Author(s):  
I. Ortega ◽  
T. Koenig ◽  
R. Sinreich ◽  
D. Thomson ◽  
R. Volkamer
Keyword(s):  
Trace Gases ◽  
Elevation Angle ◽  
Three Dimensional ◽  
Tropospheric Chemistry ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
High Time Resolution ◽  
Vertical Profiles ◽  
Near Surface

Abstract. We present an innovative instrument telescope and describe a retrieval method to probe three-dimensional (3-D) distributions of atmospheric trace gases that are relevant to air pollution and tropospheric chemistry. The University of Colorado (CU) two-dimensional (2-D) multi-axis differential optical absorption spectroscopy (CU 2-D-MAX-DOAS) instrument measures nitrogen dioxide (NO2), formaldehyde (HCHO), glyoxal (CHOCHO), oxygen dimer (O2–O2, or O4), and water vapor (H2O); nitrous acid (HONO), bromine monoxide (BrO), and iodine monoxide (IO) are among other gases that can in principle be measured. Information about aerosols is derived through coupling with a radiative transfer model (RTM). The 2-D telescope has three modes of operation: mode 1 measures solar scattered photons from any pair of elevation angle (−20° < EA < +90° or zenith; zero is to the horizon) and azimuth angle (−180° < AA < +180°; zero being north); mode 2 measures any set of azimuth angles (AAs) at constant elevation angle (EA) (almucantar scans); and mode 3 tracks the direct solar beam via a separate view port. Vertical profiles of trace gases are measured and used to estimate mixing layer height (MLH). Horizontal distributions are then derived using MLH and parameterization of RTM (Sinreich et al., 2013). NO2 is evaluated at different wavelengths (350, 450, and 560 nm), exploiting the fact that the effective path length varies systematically with wavelength. The area probed is constrained by O4 observations at nearby wavelengths and has a diurnal mean effective radius of 7.0 to 25 km around the instrument location; i.e., up to 1960 km2 can be sampled with high time resolution. The instrument was deployed as part of the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, from 7 June to 6 July 2013. We present first measurements (modes 1 and 2 only) and describe a four-step retrieval to derive (a) boundary layer vertical profiles and MLH of NO2; (b) near-surface horizontal distributions of NO2; (c) range-resolved NO2 horizontal distribution measurements using an "onion-peeling" approach; and (d) the ratios HCHO to NO2 (RFN), CHOCHO to NO2 (RGN), and CHOCHO to HCHO (RGF) at 14 pre-set azimuth angles distributed over a 360° view. Three-dimensional distribution measurements with 2-D-MAX-DOAS provide an innovative, regional perspective of trace gases as well as their spatial and temporal concentration gradients, and they maximize information to compare near-surface observations with atmospheric models and satellites.

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