An official website of the United States government
Abstract Marine cloud brightening (MCB) is proposed to offset global warming by emitting sea salt aerosols to the tropical marine boundary layer, which increases aerosol and cloud albedo. Sea salt aerosol is the main source of tropospheric reactive chlorine (Cly) and bromine (Bry). The effects of additional sea salt on atmospheric chemistry have not been explored. We simulate sea salt aerosol injections for MCB under two scenarios (212–569 Tg/a) in the GEOS‐Chem global chemical transport model, only considering their impacts as a halogen source. Globally, tropospheric Clyand Bryincrease (20–40%), leading to decreased ozone (−3 to −6%). Consequently, OH decreases (−3 to −5%), which increases the methane lifetime (3–6%). Our results suggest that the chemistry of the additional sea salt leads to minor total radiative forcing compared to that of the sea salt aerosol itself (~2%) but may have potential implications for surface ozone pollution in tropical coastal regions.
more »
« less
Anthropogenic Influence on Tropospheric Reactive Bromine Since the Pre‐industrial: Implications for Arctic Ice‐Core Bromine Trends
Abstract Tropospheric reactive bromine (Bry) influences the oxidation capacity of the atmosphere by acting as a sink for ozone and nitrogen oxides. Aerosol acidity plays a crucial role in Bryabundances through acid‐catalyzed debromination from sea‐salt‐aerosol, the largest global source. Bromine concentrations in a Russian Arctic ice‐core, Akademii Nauk, show a 3.5‐fold increase from pre‐industrial (PI) to the 1970s (peak acidity, PA), and decreased by half to 1999 (present day, PD). Ice‐core acidity mirrors this trend, showing robust correlation with bromine, especially after 1940 (r = 0.9). Model simulations considering anthropogenic emission changes alone show that atmospheric acidity is the main driver of Brychanges, consistent with the observed relationship between acidity and bromine. The influence of atmospheric acidity on Bryshould be considered in interpretation of ice‐core bromine trends.
more »
« less
- Award ID(s):
- 2202287
- PAR ID:
- 10492811
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Geophysical Research Letters
- Volume:
- 51
- Issue:
- 5
- ISSN:
- 0094-8276
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Snowpack emissions are recognized as an important source of gas‐phase reactive bromine in the Arctic and are necessary to explain ozone depletion events in spring caused by the catalytic destruction of ozone by halogen radicals. Quantifying bromine emissions from snowpack is essential for interpretation of ice‐core bromine. We present ice‐core bromine records since the pre‐industrial (1750 CE) from six Arctic locations and examine potential post‐depositional loss of snowpack bromine using a global chemical transport model. Trend analysis of the ice‐core records shows that only the high‐latitude coastal Akademii Nauk (AN) ice core from the Russian Arctic preserves significant trends since pre‐industrial times that are consistent with trends in sea ice extent and anthropogenic emissions from source regions. Model simulations suggest that recycling of reactive bromine on the snow skin layer (top 1 mm) results in 9–17% loss of deposited bromine across all six ice‐core locations. Reactive bromine production from below the snow skin layer and within the snow photic zone is potentially more important, but the magnitude of this source is uncertain. Model simulations suggest that the AN core is most likely to preserve an atmospheric signal compared to five Greenland ice cores due to its high latitude location combined with a relatively high snow accumulation rate. Understanding the sources and amount of photochemically reactive snow bromide in the snow photic zone throughout the sunlit period in the high Arctic is essential for interpreting ice‐core bromine, and warrants further lab studies and field observations at inland locations.more » « less
-
Abstract. Bromine radicals influence global tropospheric chemistryby depleting ozone and by oxidizing elemental mercury and reduced sulfurspecies. Observations typically indicate a 50 % depletion of sea saltaerosol (SSA) bromide relative to seawater composition, implying that SSAdebromination could be the dominant global source of tropospheric bromine.However, it has been difficult to reconcile this large source with therelatively low bromine monoxide (BrO) mixing ratios observed in the marineboundary layer (MBL). Here we present a new mechanistic description of SSAdebromination in the GEOS-Chem global atmospheric chemistry model with adetailed representation of halogen (Cl, Br, and I) chemistry. We show thatobserved levels of SSA debromination can be reproduced in a mannerconsistent with observed BrO mixing ratios. Bromine radical sinks from theHOBr + S(IV) heterogeneous reactions and from ocean emission ofacetaldehyde are critical in moderating tropospheric BrO levels. Theresulting HBr is rapidly taken up by SSA and also deposited. Observations of SSA debromination at southern midlatitudes in summer suggest that modeluptake of HBr by SSA may be too fast. The model provides a successfulsimulation of free-tropospheric BrO in the tropics and midlatitudes in summer,where the bromine radical sink from the HOBr + S(IV) reactions iscompensated for by more efficient HOBr-driven recycling in clouds compared toprevious GEOS-Chem versions. Simulated BrO in the MBL is generally muchhigher in winter than in summer due to a combination of greater SSA emissionand slower conversion of bromine radicals to HBr. An outstanding issue inthe model is the overestimate of free-tropospheric BrO in extratropicalwinter–spring, possibly reflecting an overestimate of the HOBr∕HBr ratiounder these conditions where the dominant HOBr source is hydrolysis ofBrNO3.more » « less
-
Abstract Bromine is a key halogen element in the quantification of volcanic volatiles, but analytical difficulties in measuring its very low abundances have prevented progress in understanding its behavior and its role in volcanic emissions. We present a new data set of bromine, chlorine, and fluorine concentrations in melt inclusions and matrix glasses for two rhyolitic super-eruptions from the Toledo and Valles calderas, New Mexico, USA. We show that before eruption, Br and Cl were efficiently partitioned from the gas-saturated magma into a separate fluid phase, and we calculate the mass of halogens in the fluid phase. We further demonstrate that syn-eruptive magma degassing was negligible during the super-eruptions, so that the main source of halogen emissions must have been the fluid phase. If the fluid phase were erupted, the large mass of Br and Cl could have severely impacted the atmospheric chemistry upon eruption.more » « less
-
Abstract The abundance and sources of ice‐nucleating particles, particles required for heterogeneous ice nucleation, are long‐standing sources of uncertainty in quantifying aerosol‐cloud interactions. In this study, we demonstrate near closure between immersion freezing ice‐nucleating particle number concentration (nINPs) observations andnINPscalculated from simulated sea spray aerosol and dust. The Community Atmospheric Model with constrained meteorology was used to simulate aerosol concentrations at the Mace Head Research Station (North Atlantic) and over the Southern Ocean to the south of Tasmania (Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign). Model‐predictednINPswere within a factor of 10 ofnINPsobserved with an off‐line ice spectrometer at Mace Head Research Station and Clouds, Aerosols, Precipitation, Radiation, and atmospherIc Composition Over the southeRN ocean campaign, for 93% and 69% of observations, respectively. Simulated vertical profiles ofnINPsreveal that transported dust may be critical tonINPsin remote regions and that sea spray aerosol may be the dominate contributor to primary ice nucleation in Southern Ocean low‐level mixed‐phase clouds.more » « less
