The role of biomass burning as derived from the tropospheric CO vertical profiles measured by IAGOS aircraft in 2002–2017

This study investigates the role of biomass burning and long-range transport in the anomalies of carbon monoxide (CO) regularly observed along the tropospheric vertical profiles measured in the framework of the In-service Aircraft for a Global Observing System (IAGOS). Considering the high interannual variability of biomass burning emissions and the episodic nature of long-range pollution transport, one strength of this study is the amount of data taken into account, namely 30 000 vertical profiles at nine clusters of airports in Europe, North America, Asia, India and southern Africa over the period 2002-2017. As a preliminary, a brief overview of the spatiotemporal variability, latitudinal distribution, interannual variability and trends of biomass burning CO emissions from 14 regions is provided. The distribution of CO mixing ratios at different levels of the troposphere is also provided based on the entire IAGOS database (125 million CO observations). This study focuses on the free troposphere (altitudes above 21(m) where the long-range transport of pollution is favoured. Anomalies at a given airport cluster are here defined as departures from the local seasonally averaged climatological vertical profile. The intensity of these anomalies varies significantly depending on the airport, with maximum (minimum) CO anomalies of 110-150 (48) ppbv in Asia (Europe). Looking at the seasonal variation of the frequency of occurrence, the 25 % strongest CO anomalies appear reasonably well distributed throughout the year, in contrast to the 5 % or 1 % strongest anomalies that exhibit a strong seasonality with, for instance, more frequent anomalies during sum- mertime in the northern United States, during winter/spring in Japan, during spring in south-east China, during the nonmonsoon seasons in south-east Asia and south India, and during summer/fall in Windhoek, Namibia. Depending on the location, these strong anomalies are observed in different parts of the free troposphere. In order to investigate the role of biomass burning emissions in these anomalies, we used the SOFT-IO (SOft attribution using FlexparT and carbon monoxide emission inventories for In-situ Observation database) v1.0 IAGOS added-value products that consist of FLEXible PARTicle dispersion model (FLEXPART) 20-day backward simulations along all IAGOS aircraft trajectories, coupled with anthropogenic Monitoring Atmospheric Composition and Climate (MACC)/CityZEN EU projects (MACCity) and biomass burning Global Fire Assimilation System (GFAS) CO emission inventories and vertical injections. SOFT-IO estimates the contribution (in ppbv) of the recent (less than 20 days) primary worldwide CO emissions, tagged per source region. Biomass burning emissions are found to play an important role in the strongest CO anomalies observed at most airport clusters. The regional tags indicate a large contribution from boreal regions at airport clusters in Europe and North America during the summer season. In both Japan and south India, the anthropogenic emissions dominate all throughout the year, except for the strongest summertime anomalies observed in Japan that are due to Siberian fires. The strongest CO anomalies at airport clusters located in south-east Asia are induced by fires burning during spring in south-east Asia and during fall in equatorial Asia. In southern Africa, the Windhoek airport was mainly impacted by fires in Southern Hemisphere Africa and South America. To our knowledge, no other studies have used such a large dataset of in situ vertical profiles for deriving a climatology of the impact of biomass burning versus anthropogenic emissions on the strongest CO anomalies observed in the troposphere, in combination with information on the source regions. This study therefore provides both qualitative and quantitative information for interpreting the highly variable CO vertical distribution in several regions of interest.