Search

This study focuses on the distribution of hydrogen peroxide (H 2 O 2) 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 no clear trend in the 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 to the tropical storm Florence (later developing into a hurricane). The observed H 2 O 2 distribution suggests that mixing ratios in the upper troposphere seem to be far less dependent on latitude than assumed previously and the corresponding factors influencing the photochemical production and loss of H 2 O 2. The observed levels of H 2 O 2 in the upper troposphere indicate the influence of convective transport processes on the distribution of the species not only in the tropical but also in the subtropical regions. The measurements are compared to observation-based photostationary steady-state (PSS) calculations and numerical simulations by the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model. North of the ITCZ, PSS calculations produce mostly lower H 2 O 2 mixing ratios relative to the observations. The observed mixing ratios tend to exceed the PSS calculations by up to a factor of 2. With the exception of local events, the comparison between the calculated PSS values and the observations indicates enhanced H 2 O 2 mixing ratios relative to the expectations based on PSS calculations in the north of the ITCZ. On the other hand, PSS calculations tend to overestimate the H 2 O 2 mixing ratios in most of the sampled area in the 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 sampled region. Simulations performed by the EMAC model also overestimate hydrogen peroxide levels particularly in the Southern Hemisphere, most likely due to underestimated cloud scavenging. EMAC simulations and PSS calculations both indicate a latitudinal gradient from the Equator towards the subtropics. In contrast, the measurements show no clear gradient with latitude in the mixing ratios of H 2 O 2 in the upper troposphere with a slight decrease from the ITCZ towards the subtropics, indicating a relatively low dependency on the solar radiation intensity and the corresponding photolytic activity. The largest model 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]

The supereruption of Los Chocoyos (14.6 ∘ N, 91.2 ∘ W) in Guatemala ∼84 kyr ago was one of the largest volcanic events of the past 100 000 years. Recent petrologic data show that the eruption released very large amounts of climate-relevant sulfur and ozone-destroying chlorine and bromine gases (523±94 Mt sulfur, 1200±156 Mt chlorine, and 2±0.46 Mt bromine). Using the Earth system model (ESM) of the Community Earth System Model version 2 (CESM2) coupled with the Whole Atmosphere Community Climate Model version 6 (WACCM6), we simulated the impacts of the sulfur- and halogen-rich Los Chocoyos eruption on the preindustrial Earth system. Our simulations show that elevated sulfate burden and aerosol optical depth (AOD) persists for 5 years in the model, while the volcanic halogens stay elevated for nearly 15 years. As a consequence, the eruption leads to a collapse of the ozone layer with global mean column ozone values dropping to 50 DU (80 % decrease) and leading to a 550 % increase in surface UV over the first 5 years, with potential impacts on the biosphere. The volcanic eruption shows an asymmetric-hemispheric response with enhanced aerosol, ozone, UV, and climate signals over the Northern Hemisphere. Surface climate is impacted globally due to peak AOD of >6 , which leads to a maximum surface cooling of >6 K, precipitation and terrestrial net primary production decrease of >25 %, and sea ice area increases of 40 % in the first 3 years. Locally, a wetting (>100 %) and strong increase in net primary production (NPP) (>700 %) over northern Africa is simulated in the first 5 years and related to a southward shift of the Intertropical Convergence Zone (ITCZ) to the southern tropics. The ocean responds with pronounced El Niño conditions in the first 3 years that shift to the southern tropics and are coherent with the ITCZ change. Recovery to pre-eruption ozone levels and climate takes 15 years and 30 years, respectively. The long-lasting surface cooling is sustained by an immediate increase in the Arctic sea ice area, followed by a decrease in poleward ocean heat transport at 60 ∘ N which lasts up to 20 years. In contrast, when simulating Los Chocoyos conventionally by including sulfur and neglecting halogens, we simulate a larger sulfate burden and AOD, more pronounced surface climate changes, and an increase in column ozone. By comparing our aerosol chemistry ESM results to other supereruption simulations with aerosol climate models, we find a higher surface climate impact per injected sulfur amount than previous studies for our different sets of model experiments, since the CESM2(WACCM6) creates smaller aerosols with a longer lifetime, partly due to the interactive aerosol chemistry. As the model uncertainties for the climate response to supereruptions are very large, observational evidence from paleo archives and a coordinated model intercomparison would help to improve our understanding of the climate and environment response. [ABSTRACT FROM AUTHOR]