Nitrogen oxides are essential for the formation of secondary atmospheric aerosols and of atmospheric oxidants such as ozone and the hydroxyl radical, which controls the self-cleansing capacity of the atmosphere. Nitric acid, a major oxidation product of nitrogen oxides, has traditionally been considered to be a permanent sink of nitrogen oxides. However, model studies predict higher ratios of nitric acid to nitrogen oxides in the troposphere than are observed. A 'renoxification' process that recycles nitric acid into nitrogen oxides has been proposed to reconcile observations with model studies, but the mechanisms responsible for this process remain uncertain. Here we present data from an aircraft measurement campaign over the North Atlantic Ocean and find evidence for rapid recycling of nitric acid to nitrous acid and nitrogen oxides in the clean marine boundary layer via particulate nitrate photolysis. Laboratory experiments further demonstrate the photolysis of particulate nitrate collected on filters at a rate more than two orders of magnitude greater than that of gaseous nitric acid, with nitrous acid as the main product. Box model calculations based on the Master Chemical Mechanism suggest that particulate nitrate photolysis mainly sustains the observed levels of nitrous acid and nitrogen oxides at midday under typical marine boundary layer conditions. Given that oceans account for more than 70 per cent of Earth's surface, we propose that particulate nitrate photolysis could be a substantial tropospheric nitrogen oxide source. Recycling of nitrogen oxides in remote oceanic regions with minimal direct nitrogen oxide emissions could increase the formation of tropospheric oxidants and secondary atmospheric aerosols on a global scale.

d. Open access institutional repositoriesThe AMS understands there is increasing demand for institutions to provide open access to the published research being produced by employees, such as faculty, of that institution. In recognition of this, the AMS grants permission to each of its authors to deposit the definitive version of that author's published AMS journal article in the repository of the author's institution provided all of the following conditions are met: The article lists the institution hosting the repository as the author's affiliation.  The copy provided to the repository is the final published PDF of the article (not the EOR version made available by AMS prior to formal publication; see section 6).  The repository does not provide access to the article until six months after the date of publication of the definitive version by the AMS.  The repository copy includes the AMS copyright notice. T he Deep Propagating Gravity Wave Experiment (DEEPWAVE) was the first comprehensive measurement program devoted to quantifying the evolution of gravity waves (GWs) arising from sources at lower altitudes as they propagate, interact with mean and other wave motions, and ultimately dissipate from Earth's surface into the mesosphere and lower thermosphere (MLT). Research goals motivating the DEEPWAVE measurement program are summarized in Table 1. To achieve our research goals, DEEPWAVE needed to sample regions having large horizontal extents because of large horizontal GW propagation distances for some GW sources. DEEPWAVE accomplished this goal through airborne and ground-based (GB) measurements that together provided sensitivity to multiple GW sources and their propagation to, and effects at, higher altitudes. DEEPWAVE was performed over and around the GW "hotspot" region of New Zealand (Fig.1, top) during austral winter, when strong vortex edge westerlies provide a stable environment for deep GW propagation into the MLT.DEEPWAVE airborne measurements employed two research aircraft during a core 6-week airborne field program based at Christchurch, New Zealand, from 6 June to 21 July 2014. The National Science 425MARCH 2016 AMERICAN METEOROLOGICAL SOCIETY | Foundation (NSF)/National Center for Atmospheric Research (NCAR) Gulfstream V (GV) provided in situ, dropsonde, and microwave temperature profiler (MTP) measurements extending from Earth's surface to ~20 km throughout the core field program (see Table 2). The GV also carried three new instruments designed specifically to address DEEPWAVE science goals: 1) a Rayleigh lidar measuring densities and temperatures from ~20 to 60 km, 2) a sodium resonance lidar measuring sodium densities and temperatures from ~75 to 100 km, and 3) an advanced mesosphere temperature mapper (AMTM) measuring temperatures in a horizontal plane at ~87 km with a field of view (FOV) of ~120 km along track and 80 km cross track. AMTM measurements were augmented by two side-viewing infrared (IR) airglow "wing" cameras also viewing an ~87-km altitude that extended the cross-track FOV to ...

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation and radiative processes, and their interactions. Projects between 2016 and 2018 used in-situ probes, radar, lidar and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN) and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase cloudsnucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF/NCAR G-V aircraft flying north-south gradients south of Tasmania, at Macquarie Island, and on the RV Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons.Results show a largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multi-layered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O 3 ), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O 3 and methane (CH 4 ) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10°N to 40°S), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O 3 . The observed BrO concentrations increase strongly with altitude (∼3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Br y ), or model overestimated Br y wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Br y source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O 3 needs to be considered when estimating past and future ozone radiative effects.atmospheric chemistry | oxidative capacity | halogens | heterogeneous chemistry | UTLS T ropospheric halogens catalytically destroy O 3 (1−3), oxidize atmospheric mercury (4, 5), and modify the oxidative capacity of the atmosphere (6). O 3 is a potent greenhouse gas (7), and an important precursor for hydroxyl (OH) radicals (6, 8) that determine the lifetime of CH 4 another important greenhouse gas. About 75% of the global tropospheric O 3 (3) and CH 4 (8) loss occurs at tropical latitudes, where O 3 radiative forcing is also most sensitive to changes in O 3 (9). Halogen chemistry is thought responsible for ∼10% of the tropical tropospheric O 3 column loss (3), yet atmospheric models remain essentially untested due to the lack of vertically resolved halogen radical measurements in the tropical troposphere. Column observations from ground and satellites (10−18), including measurements in the tropics (14, 16−18), point to the existence of a-possibly ubiquitous-tropospheric BrO background concentration of ∼1−2 parts per trillion by volume (pptv) that currently remains unexplained by models, and would be of significant relevance for O 3 , OH, and mercury oxidation (2−6, 8). Recently, corroborating evidence is emerging from a measurement in the tropical free troposphere (FT) (19). IO has been detected in the Northern Hemisphere (NH) FT (19−21), but there is currently no vertically resolved measurement of BrO or IO in the ...

The distributions of ice particles, precipitation embryos, and supercooled water are examined within updrafts in convective clouds in the Amazon and at Kwajalein, Marshall Islands, based on in situ measurements during two Tropical Rainfall Measuring Mission field campaigns. Composite vertical profiles of liquid water, small particle concentration, and updraft/downdraft magnitudes exhibit similar peak values for the two tropical regions. Updrafts were found to be favored locations for precipitation embryos in the form of liquid or frozen drizzle-sized droplets. Most updrafts glaciated rapidly, removing most of the liquid water between −5° and −17°C. However, occasional encounters with liquid water occurred in much colder updraft regions. The updraft magnitudes where liquid water was observed at cold (e.g., −16° to −19°C) temperatures do not appear to be stronger than updrafts without liquid water at similar temperatures, however. The concentrations of small spherical frozen particles in glaciated regions without liquid water are approximately one-half of the concentrations in regions containing liquid cloud droplets, suggesting that a substantial portion of the cloud droplets may be freezing at relatively warm temperatures. Further evidence for a possible new type of aggregate ice particle, a chain aggregate found at cloud midlevels, is given.