Title: Parameterization retrieval of trace gas volume mixing ratios from Airborne MAX-DOAS

Abstract

We present a parameterization retrieval of volume mixing ratios (VMRs) from differential slant column density (dSCD) measurements by Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS). The method makes use of the fact that horizontally recorded limb spectra (elevation angle 0°) are strongly sensitive to the atmospheric layer at instrument altitude. These limb spectra are analyzed using reference spectra that largely cancel out column contributions from above and below the instrument, so that the resulting limb dSCDs, i.e., the column integrated concentration with respect to a reference spectrum, are almost exclusively sensitive to the atmospheric layers around instrument altitude. The conversion of limb dSCDs into VMRs is then realized by calculating box air mass factors (Box-AMFs) for a Rayleigh atmosphere and applying a scaling factor constrained by O₄ dSCDs to account for aerosol extinction. An iterative VMR retrieval scheme corrects for trace gas profile shape effects. Benefits of this method are (1) a fast conversion that only requires the computation of Box-AMFs in a Rayleigh atmosphere; (2) neither local aerosol extinction nor the slant column density in the DOAS reference (SCD_ref) needs to be known; and (3) VMRs can be retrieved for every measurement point along a flight track, thus increasing statistics and addingmore » flexibility to capture concentration gradients. Sensitivity studies are performed for bromine monoxide (BrO), iodine monoxide (IO) and nitrogen dioxide (NO₂), using (1) simulated dSCD data for different trace gas and aerosol profiles and (2) field measurements from the Tropical Ocean tRoposphere Exchange of Reactive halogen species and Oxygenated VOC (TORERO) field experiment. For simulated data in a Rayleigh atmosphere, the agreement between the VMR from the parameterization method (VMR_para) and the true VMR (VMR_true) is excellent for all trace gases. Offsets, slopes and R² values for the linear fit of VMR_para over VMR_true are, respectively (0.008 ± 0.001) pptv, 0.988 ± 0.001, 0.987 for BrO; (-0.0066 ± 0.0001) pptv, 1.0021 ± 0.0003, 0.9979 for IO; (-0.17 ± 0.03) pptv, 1.0036 ± 0.0001, 0.9997 for NO₂. The agreement for atmospheres with aerosol shows comparable R² values to the Rayleigh case, but slopes deviate a bit more from one: (0.093 ± 0.002) pptv, 0.933 ± 0.002, 0.907 for BrO; (0.0021 ± 0.0004) pptv, 0.887 ± 0.001, 0.973 for IO; (8.5 ± 0.1) pptv, 0.8302 ± 0.0006, 0.9923 for NO₂. VMR_para from field data are further compared with optimal estimation retrievals (VMR_OE). Least orthogonal distance fit of the data give the following equations: BrO_para = (0.1 ± 0.2) pptv + (0.95 ± 0.14) × BrO_OE; IO_para = (0.01 ± 0.02) pptv + (1.00 ± 0.12) × IO_OE; NO_2para = (3.9 ± 2.5) pptv + (0.87 ± 0.15) × NO_2OE. Overall, we conclude that the parameterization retrieval is accurate with an uncertainty of 20 % for IO, 30 % for BrO and NO₂, but not better than 0.05 pptv IO, 0.5 pptv BrO and 10 pptv NO₂. Finally, the retrieval is applicable over a wide range of atmospheric conditions and measurement geometries and not limited to the interpretation of vertical profile measurements in the remote troposphere.« less

Authors:

Dix, Barbara ^[1]; Koenig, Theodore K. ^[2]; Volkamer, Rainer  ^[2]

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+ Show Author Affiliations

1. Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry
2. Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES)

Publication Date:

Mon Nov 28 00:00:00 EST 2016

Research Org.:

Univ. of Colorado, Boulder, CO (United States)

Sponsoring Org.:

USDOE

OSTI Identifier:

1430260

Grant/Contract Number:  

SC0006080; EPP27450/C13049; EP-P32238/C14974

Resource Type:

Accepted Manuscript

Journal Name:

Atmospheric Measurement Techniques (Online)

Additional Journal Information:

Journal Name: Atmospheric Measurement Techniques (Online); Journal Volume: 9; Journal Issue: 11; Journal ID: ISSN 1867-8548

Publisher:

European Geosciences Union

Country of Publication:

United States

Language:

English

Subject:

54 ENVIRONMENTAL SCIENCES