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Abstract

Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly-averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN-MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tg yr-1) which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+13 %) and anthropogenic VOCs (-17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50° N, but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism. However, the top-down emissions are very sensitive to the bias correction of the observed columns. Furthermore, the use of different a priori emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. In regions with variable meteorology, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments.