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The ability to predict the trajectory of climate change requires a clear understanding of the emissions and uptake (i.e., surface fluxes) of long-lived greenhouse gases (GHGs). Furthermore, the development of climate policies is driving a need to constrain the budgets of anthropogenic GHG emissions. Inverse problems that couple atmospheric observations of GHG concentrations with an atmospheric chemistry and transport model have increasingly been used to gain insights into surface fluxes. Given the inherent technical challenges associated with their solution, it is imperative that objective approaches exist for the evaluation of such inverse problems. Because direct observation of fluxes at compatible spatiotemporal scales is rarely possible, diagnostics tools must rely on indirect measures. Here we review diagnostics that have been implemented in recent studies and discuss their use in informing adjustments to model setup. We group the diagnostics along a continuum starting with those that are most closely related to the scientific question being targeted, and ending with those most closely tied to the statistical and computational setup of the inversion. We thus begin with diagnostics based on assessments against independent information (e.g., unused atmospheric observations, largescale scientific constraints), followed by statistical diagnostics of inversion results, diagnostics based on sensitivity tests, and analyses of robustness (e.g., tests focusing on the chemistry and transport model, the atmospheric observations, or the statistical and computational framework), and close with the use of synthetic data experiments (i.e., observing system simulation experiments, OSSEs). We find that existing diagnostics provide a crucial toolbox for evaluating and improving flux estimates but, not surprisingly, cannot overcome the fundamental challenges associated with limited atmospheric observations or the lack of direct flux measurements at compatible scales. As atmospheric inversions are increasingly expected to contribute to national reporting of GHG emissions, the need for developing and implementing robust and transparent evaluation approaches will only grow.