Abstract

Abstract. Monitoring CO2 from space is essential to characterize the spatiotemporal distribution of this major greenhouse gas and quantify its sources and sinks. The mixing ratio of CO2 to dry air can be derived from the CO2∕O2 column ratio. The O2 column is usually derived from its absorption signature on the solar reflected spectra over the O2 A band (e.g. Orbiting Carbon Observatory-2 (OCO-2), Thermal And Near infrared Sensor for carbon Observation (TANSO)/Greenhouse Gases Observing Satellite (GOSAT), TanSat). As a result of atmospheric scattering, the atmospheric path length varies with the aerosols' load, their vertical distribution, and their optical properties. The spectral distance between the O2 A band (0.76 µm) and the CO2 absorption band (1.6 µm) results in significant uncertainties due to the varying spectral properties of the aerosols over the globe. There is another O2 absorption band at 1.27 µm with weaker lines than in the A band. As the wavelength is much closer to the CO2 and CH4 bands, there is less uncertainty when using it as a proxy of the atmospheric path length to the CO2 and CH4 bands. This O2 band is used by the Total Carbon Column Observing Network (TCCON) implemented for the validation of space-based greenhouse gas (GHG) observations. However, this absorption band is contaminated by the spontaneous emission of the excited molecule O2*, which is produced by the photo-dissociation of O3 molecules in the stratosphere and mesosphere. From a satellite looking nadir, this emission has a similar shape to the absorption signal that is used. In the frame of the CNES (Centre National d'Études Spatiales – the French National Centre for Space Studies) MicroCarb project, scientific studies have been performed in 2016–2018 to explore the problems associated with this O2* airglow contamination and methods to correct it. A theoretical synthetic spectrum of the emission was derived from an approach based on A21 Einstein coefficient information contained in the line-by-line high-resolution transmission molecular absorption (HITRAN) 2016 database. The shape of our synthetic spectrum is validated when compared to O2* airglow spectra observed by the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY)/Envisat in limb viewing. We have designed an inversion scheme of SCIAMACHY limb-viewing spectra, allowing to determine the vertical distribution of the volume emission rate (VER) of the O2* airglow. The VER profiles and corresponding integrated nadir intensities were both compared to a model of the emission based on the Reactive Processes Ruling the Ozone Budget in the Stratosphere (REPROBUS) chemical transport model. The airglow intensities depend mostly on the solar zenith angle (both in model and data), and the model underestimates the observed emission by ∼15 %. This is confirmed with SCIAMACHY nadir-viewing measurements over the oceans: in such conditions, we have disentangled and retrieved the nadir O2* emission in spite of the moderate spectral resolving power (∼860) and found that the nadir SCIAMACHY intensities are mostly dictated by solar zenith angle (SZA) and are larger than the model intensities by a factor of ∼1.13. At a fixed SZA, the model airglow intensities show very little horizontal structure, in spite of ozone variations. It is shown that with the MicroCarb spectral resolution power (25 000) and signal-to-noise ratio (SNR), the contribution of the O2* emission at 1.27 µm to the observed spectral radiance in nadir viewing may be disentangled from the lower atmosphere/ground absorption signature with a great accuracy. Indeed, simulations with 4ARCTIC radiative transfer inversion tool have shown that the CO2 mixing ratio may be retrieved with the accuracy required for quantifying the CO2 natural sources and sinks (pressure-level error ≤1 hPa; XCO2 accuracy better than 0.4 ppmv) with the O2 1.27 µm band only as the air proxy (without the A band). As a result of these studies (at an intermediate phase), it was decided to include this band (B4) in the MicroCarb design, while keeping the O2 A band for reference (B1). Our approach is consistent with the approach of Sun et al. (2018), who also analysed the potential of the O2 1.27 µm band and concluded favourably for GHG monitoring from space. We advocate for the inclusion of this O2 band on other GHG monitoring future space missions, such as GOSAT-3 and EU/European Space Agency (ESA) CO2-M missions, for a better GHG retrieval.

Highlights

  • Carbon dioxide (CO2) is recognized as the main driver of human-induced climate change

  • We have reported the results of a 3 years (2016– 2018) scientific research effort to revisit the use of the O2 absorption band at 1.27 μm in the problem of greenhouse gas (GHG) retrieval from space observations of the detailed spectrum of the solar radiation scattered by aerosols, atmosphere and surface

  • We used the limb-viewing observations of SCIAMACHY in this band, which are not contaminated by atmosphere/aerosols scattering of solar radiation when looking above ∼ 30 km altitude

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Summary

Introduction

Carbon dioxide (CO2) is recognized as the main driver of human-induced climate change. We have used this formulation to transform an absorption spectrum by O2 that can be computed with Line-ByLine Radiative Transfer Model (LBLRTM) software (see details in Appendix A) into a synthetic emission spectrum This method of construction of a synthetic emission spectrum was the basis of our work on three topics: a satisfactory comparison with the observed spectra of SCIAMACHY (see below); retrieving the airglow intensity from SCIAMACHY nadir data over low-albedo regions; retrieving the surface pressure from simulations at high spectral resolution. Both model and data nadir emissions are obtained by vertical integration of the VER, respectively, in the airglow model and in the SCIAMACHY-derived VER vertical profile This nadir emission is directly relevant to the GHG observations since, from an orbiter and nadir viewing, this signal is superimposed on the solar back-scattered emission from which the columns of GHG gases and O2 must be retrieved. The second element is an airglow model operated offline, which extracts from REPROBUS (for one location and one precise time and date) the information necessary for the computation of the relevant VER profile

REPROBUS 3-D simulations
Some examples of model results
Comparison of SCIAMACHY data with REPROBUS-derived airglow model
Comparison of VER vertical profiles
The MicroCarb mission
Overview
Airglow inversion in nadir SCIAMACHY spectra
Algorithm used in the LATMOS inversion breadboard
Conclusions
Simulation of Psurf retrievals
Spectroscopy: the various electronic states of the O2 molecule
Observations on Venus and Mars
Computation of the airglow detailed line-by-line intensity
Practical method to produce a synthetic emission spectrum
The case with no absorption: the onion-peeling technique
The case with absorption: a modified onion-peeling technique
Comparison of methods used by others
Nighttime ozone profiles
Findings
Daytime ozone profiles

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