Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher.
Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?
Some links on this page may take you to non-federal websites. Their policies may differ from this site.
-
Abstract. Reactive halogen chemistry in the springtime Arctic causes ozone depletion events and alters the rate of pollution processing. There are still many uncertainties regarding this chemistry, including the multiphase recycling of halogens and how sea ice impacts the source strength of reactive bromine. Adding to these uncertainties are the impacts of a rapidly warming Arctic. We present observations from the CHACHA (CHemistry in the Arctic: Clouds, Halogens, and Aerosols) field campaign based out of Utqiaġvik, Alaska, from mid-February to mid-April of 2022 to provide information on the vertical distribution of bromine monoxide (BrO), which is a tracer for reactive bromine chemistry. Data were gathered using the Heidelberg Airborne Imaging DOAS (differential optical absorption spectroscopy) Instrument (HAIDI) on the Purdue University Airborne Laboratory for Atmospheric Research (ALAR) and employing a unique sampling technique of vertically profiling the lower atmosphere with the aircraft via “porpoising” maneuvers. Observations from HAIDI were coupled to radiative transfer model calculations to retrieve mixing ratio profiles throughout the lower atmosphere (below 1000 m), with unprecedented vertical resolution (50 m) and total information gathered (average of 17.5 degrees of freedom) for this region. A cluster analysis was used to categorize 245 retrieved BrO mixing ratio vertical profiles into four common profile shapes. We often found the highest BrO mixing ratios at the Earth's surface with a mean of nearly 30 pmol mol−1 in the lowest 50 m, indicating an important role for multiphase chemistry on the snowpack in reactive bromine production. Most lofted-BrO profiles corresponded with an aerosol profile that peaked at the same altitude (225 m above the ground), suggesting that BrO was maintained due to heterogeneous reactions on particle surfaces aloft during these profiles. A majority (11 of 15) of the identified lofted-BrO profiles occurred on a single day, 19 March 2022, over an area covering more than 24 000 km2, indicating that this was a large-scale lofted-BrO event. The clustered BrO mixing ratio profiles should be particularly useful for some MAX-DOAS (multi-axis DOAS) studies, where a priori BrO profiles and their uncertainties, used in optimal estimation inversion algorithms, are not often based on previous observations. Future MAX-DOAS studies (and past reanalyses) could rely on the profiles provided in this work to improve BrO retrievals.more » « less
-
Abstract The Chemistry in the Arctic: Clouds, Halogens, and Aerosols (CHACHA) field project aimed to advance the understanding of coupled meteorological and chemical processes in the atmospheric boundary layer during the seasonal increase in sea ice fracturing in spring. CHACHA sought to understand the interactions between this changing snow-covered surface, surface-coupled clouds, sea spray aerosols, multiphase halogen chemistry, and impacts of emissions from oil and gas extraction on atmospheric chemistry. The project measured greenhouse gases, reactive gases, size-resolved aerosol number concentrations, cloud microphysical properties, and meteorological conditions in real time, while also collecting particles for offline analysis. Two instrumented aircraft were deployed: the Purdue University Airborne Laboratory for Atmospheric Research and the University of Wyoming King Air. Flights were conducted out of Utqiaġvik, Alaska, between 21 February and 16 April 2022, sampling air over snow-covered and newly frozen sea ice in the Beaufort and Chukchi Seas, over open leads, and over the snow-covered tundra of the North Slope of Alaska, including the oil and gas extraction region near Prudhoe Bay. Observations showed that reactive bromine gases generally peaked near the snow-covered surface and decayed rapidly within the lowest few hundred meters where ozone was depleted, with concentrations reduced by nitrogen oxides emitted from oil fields. Cloud microphysical measurements revealed that thin clouds over and downwind of leads grew in vertical extent after contact with open water. Results from dropsondes indicated that convective boundary layers developed over leads, with depths ranging from 250 to 850 m depending on the fetch.more » « lessFree, publicly-accessible full text available November 1, 2026
An official website of the United States government
