Search

Copyright of Perspektive Mediation is the property of Verlag Oesterreich GmbH and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

This study focuses on the distribution of hydrogen peroxide (H2O2) in the upper tropical troposphere at altitudes between 8 and 15 km based on in situ observations during the Chemistry of the Atmosphere - Field Experiment in Africa (CAFE-Africa) campaign conducted in August-September 2018 over the tropical Atlantic Ocean and western Africa. The measured hydrogen peroxide mixing ratios in the upper troposphere show a nearly uniform latitudinal distribution with locally increased levels (up to 1 ppbv) within the Intertropical Convergence Zone (ITCZ), over the African coastal area, as well as during measurements performed in proximity of the tropical storm Florence (later developing into a hurricane), indicating the influence of convective transport processes. The measurements are compared to observation-based photostationary steady-state (PSS) calculations and numerical simulations by the global EMAC model. North of the ITCZ, PSS calculations produce lower H2O2 mixing ratios relative to the observations. Here observed mixing ratios exceed the PSS calculations by up to a factor of 2. On the other hand, PSS calculations overestimate the H2O2 mixing ratios south of the ITCZ by a factor of up to 3. The significant influence of convection in the ITCZ and the enhanced presence of clouds towards the southern hemisphere indicate contributions of atmospheric transport and cloud scavenging in the probed region. Differences between H2O2 observations and simulations of local PSS indicate that convective transport in the ITCZ region and consequent redistribution of H2O2 towards the north and south impacts the spatial distribution of H2O2 in the upper troposphere. Simulations performed by EMAC analogously overestimate hydrogen peroxide levels particularly in the southern hemisphere, most likely due to underestimated cloud scavenging. Latitudinal distribution analysis indicates a gradient from the equator towards the subtropics both in the EMAC simulations and the PSS calculations. On the other hand, the measurements display nearly uniform mixing ratios of the species in the upper troposphere with a slight decrease from the ITCZ towards the subtropics, indicating a relatively low dependency on the solar radiation inclination and the corresponding photolytic activity. The highest deviations relative to the observations correspond with the underestimated hydrogen peroxide loss due to enhanced cloud presence, scavenging, and rainout in the ITCZ and towards the south. [ABSTRACT FROM AUTHOR]

Formaldehyde (HCHO) and hydrogen peroxide (H2O2) play a key role in atmospheric oxidation processes. They act as sources and sinks for HOx radicals (OH + HO2), with OH as the primary oxidant that governs the atmospheric self-cleaning capacity. Measurements of these species allow evaluation of global chemistry-transport models which need to account for multifarious source distributions, transport and mixing, complex photochemical reaction pathways and deposition processes. HCHO is an intermediate produced during the oxidation of VOCs and is an indicator of photochemical activity and combustion related emissions. Due to its many production pathways and its rather short lifetime of only several hours at noon, accurate modelling of this species is challenging. In this study, we use in situ observations in the marine boundary layer (MBL) to evaluate results of the general circulation model EMAC (ECHAM5/MESSy2 Atmospheric Chemistry). The dataset was obtained during the AQABA ship campaign around the Arabian Peninsula in summer 2017. This region is characterized by high mixing ratios of photochemical air pollution, high humidity and strong solar irradiation, especially in the area around the Suez Canal and the Arabian Gulf. We find that EMAC fails to predict absolute mixing ratios of HCHO, especially during high pollution events, but it reproduces most of the HCHO variability seen in the different regions, while it systematically overestimates H2O2. This is mainly attributed to missing primary VOC emissions and the overestimation of HOx radicals, and also related to the models coarse spatial resolution. [ABSTRACT FROM AUTHOR]