Abstract

Abstract. We perform observing system simulation experiments (OSSEs) with the GEOS-Chem adjoint model to test how well methane emissions over North America can be resolved using measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and similar high-resolution satellite sensors. We focus analysis on the impacts of (i) spatial errors in the prior emissions and (ii) model transport errors. Along with a standard scale factor (SF) optimization we conduct a set of inversions using alternative formalisms that aim to overcome limitations in the SF-based approach that arise for missing sources. We show that 4D-Var analysis of the TROPOMI data can improve monthly emission estimates at 25 km even with a spatially biased prior or model transport errors (42 %–93 % domain-wide bias reduction; R increases from 0.51 up to 0.73). However, when both errors are present, no single inversion framework can successfully improve both the overall bias and spatial distribution of fluxes relative to the prior on the 25 km model grid. In that case, the ensemble-mean optimized fluxes have a domain-wide bias of 77 Gg d−1 (comparable to that in the prior), with spurious source adjustments compensating for the transport errors. Increasing observational coverage through longer-timeframe inversions does not significantly change this picture. An inversion formalism that optimizes emission enhancements rather than scale factors exhibits the best performance for identifying missing sources, while an approach combining a uniform background emission with the prior inventory yields the best performance in terms of overall spatial fidelity – even in the presence of model transport errors. However, the standard SF optimization outperforms both of these for the magnitude of the domain-wide flux. For the common scenario in which prior errors are non-random, approximate posterior error reduction calculations (derived via gradient-based randomization) for the inversions reflect the sensitivity to observations but have no spatial correlation with the actual emission improvements. This demonstrates that such information content analysis can be used for general observing system characterization but does not describe the spatial accuracy of the posterior emissions or of the actual emission improvements. Findings here highlight the need for careful evaluation of potential missing sources in prior emission datasets and for robust accounting of model transport errors in inverse analyses of the methane budget.

Highlights

  • Increases in atmospheric methane since the pre-industrial era have enhanced global radiative forcing by 0.97 W m−2, making it the second-most important anthropogenic greenhouse gas after carbon dioxide (IPCC, 2013)

  • In this paper we examine three factors that limit the accuracy of top-down methane source estimates: (i) observational coverage, (ii) spatial inaccuracies in prior emission estimates, and (iii) model transport accuracy

  • We employ here a series of observing system simulation experiments (OSSEs) experiments to evaluate a range of inversion approaches in terms of their ability to spatially resolve methane emissions from high-coverage satellite sensors such as TROPOspheric Monitoring Instrument (TROPOMI) given the remaining limiting factors above

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Summary

Introduction

Increases in atmospheric methane since the pre-industrial era have enhanced global radiative forcing by 0.97 W m−2, making it the second-most important anthropogenic greenhouse gas after carbon dioxide (IPCC, 2013). Inverse analyses commonly employ Bayesian scale factor (SF) optimization to improve flux estimates based on model–measurement concentration mismatches (Chen et al, 2018, 2021; Deng et al, 2014; Hooghiemstra et al, 2012; Jacob et al, 2016; Li et al, 2019; Maasakkers et al, 2021; Turner et al, 2015; Wecht et al, 2014a; Yu et al, 2021a; Zhang et al, 2018) This approach fails where emissions are either missing entirely in the prior inventory or are too low to sufficiently adjust without incurring a prohibitive cost function penalty (Chen et al, 2018). In this context relative to the standard and widely used SF approach

Methods
TROPOMI observations
Chemical transport model and true state
Methane sources and sinks
Optimization framework
Inversions with spatially uniform prior biases
Inversions with spatially varying prior biases
Alternative approaches to mitigate impacts of spatially varying prior errors
Summary and ensemble inversion performance
Influence of inversion timeframe on solution accuracy
Findings
Conclusions and implications

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