Numerical Modeling of Ozone Loss in the Exceptional Arctic Stratosphere Winter–Spring of 2020

Dynamical processes and changes in the ozone layer in the Arctic stratosphere during the winter of 2019–2020 were analyzed using numerical experiments with a chemistry-transport model (CTM) and reanalysis data. The results of numerical calculations using CTM with Dynamic parameters specified from the Modern Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) reanalysis data, carried out according to several scenarios of accounting for the chemical destruction of ozone, demonstrated that both Dynamic and chemical processes contribute significantly to ozone changes over the selected World Ozone and Ultraviolet Radiation Data Centre network stations, both in the Eastern and in the Western hemispheres. Based on numerical experiments with the CTM, the specific Dynamic conditions of winter–spring 2019–2020 described a decrease in ozone up to 100 Dobson Units (DU) in the Eastern Hemisphere and over 150 DU in the Western Hemisphere. In this case, the photochemical destruction of ozone in both the Western and Eastern Hemispheres at a maximum was about 50 DU with peaks in April in the Eastern Hemisphere and in March and April in the Western Hemisphere. Heterogeneous activation of halogen gases on the surface of polar stratospheric clouds, on the one hand, led to a sharp increase in the destruction of ozone in chlorine and bromine catalytic cycles, and, on the other hand, decreased its destruction in nitrogen catalytic cycles. Analysis of wave activity using 3D Plumb fluxes showed that the enhancement of upward wave activity propagation in the middle of March over the Gulf of Alaska was observed during the development stage of the minor sudden stratospheric warming (SSW) event that led to displacement of the stratospheric polar vortex to the north of Canada and decrease of polar stratospheric clouds’ volume.

Retrieval of O3, NO2, BrO and OClO Columns from Ground-Based Zenith Scattered Light DOAS Measurements in Summer and Autumn over the Northern Tibetan Plateau

Ground-based zenith scattered light differential optical absorption spectroscopy (DOAS) measurements were performed in summer and autumn (27 May–30 November) 2020 at Golmud (94°54′ E, 36°25′ N; 2807.6 m altitude) to investigate the abundances and temporal variations of ozone (O3) and its depleting substances over the northern Tibetan Plateau (TP). The differential slant column densities (dSCDs) of O3, nitrogen dioxide (NO2), bromine monoxide (BrO), and chlorine dioxide (OClO) were simultaneously retrieved from scattered solar spectra in the zenith direction during the twilight period. The O3 vertical column densities (VCDs) were derived by applying the Langley plot method, for which we investigated the sensitivities to the chosen wavelength, the a-priori O3 profile and the aerosol extinction profile used in O3 air mass factor (AMF) simulation as well as the selected solar zenith angle (SZA) range. The mean O3 VCDs from June to November 2020 are 7.21 × 1018 molec·cm−2 and 7.18 × 1018 molec·cm−2 at sunrise and sunset, respectively. The derived monthly variations of the O3 VCDs, ranging from a minimum of 6.9 × 1018 molec·cm−2 in October to 7.5 × 1018 molec·cm−2 in November, well matched the OMI satellite product, with a correlation coefficient R = 0.98. The NO2 VCDs at SZA = 90°, calculated by a modified Langley plot method, were systematically larger at sunset than at sunrise as expected with a pm/am ratio of ~1.56. The maximum of the monthly NO2 VCDs, averaged between sunrise and sunset, was 3.40 × 1015 molec·cm−2 in July. The overall trends of the NO2 VCDs were gradually decreasing with the time and similarly observed by the ground-based zenith DOAS and OMI. The average level of the BrO dSCD90°–80° (i.e., dSCD between 90° and 80° SZA) was 2.06 × 1014 molec·cm−2 during the period of June–November 2020. The monthly BrO dSCD90°–80° presented peaks in August and July for sunrise and sunset, respectively, and slowly increased after October. During the whole campaign period, the OClO abundance was lower than the detection limit of the instrument. This was to be expected because during that season the stratospheric temperatures were above the formation temperature of polar stratospheric clouds. Nevertheless, this finding is still of importance, because it indicates that the OClO analysis works well and is ready to be used during periods when enhanced OClO abundances can be expected. As a whole, ground-based zenith DOAS observations can serve as an effective way to measure the columns of O3 and its depleting substances over the TP. The aforementioned results are helpful in investigating stratospheric O3 chemistry over the third pole of the world.

New Insights into Polar Stratospheric Clouds

New satellite observations of polar stratospheric clouds have advanced our understanding of how, when, and where they form, their composition, and their role in ozone depletion.

Investigation and amelioration of long-term instrumental drifts in water vapor and nitrous oxide measurements from the Aura Microwave Limb Sounder (MLS) and their implications for studies of variability and trends

The Microwave Limb Sounder (MLS), launched on NASA's Aura spacecraft in 2004, measures vertical profiles of the abundances of key atmospheric species from the upper troposphere to the mesosphere with daily near-global coverage. We review the first 15 years of the record of H2O and N2O measurements from the MLS 190 GHz subsystem (along with other 190 GHz information), with a focus on their long-term stability, largely based on comparisons with measurements from other sensors. These comparisons generally show signs of an increasing drift in the MLS “version 4” (v4) H2O record starting around 2010. Specifically, comparisons with v4.1 measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) indicate a ∼ 2 %–3 % per decade drift over much of the stratosphere, increasing to as much as ∼ 7 % per decade around 46 hPa. Larger drifts, of around 7 %–11 % per decade, are seen in comparisons to balloon-borne frost point hygrometer measurements in the lower stratosphere. Microphysical calculations considering the formation of polar stratospheric clouds in the Antarctic winter stratosphere corroborate a drift in MLS v4 water vapor measurements in that region and season. In contrast, comparisons with the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on NASA's Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED) mission, and with ground-based Water Vapor Millimeter-wave Spectrometer (WVMS) instruments, do not show statistically significant drifts. However, the uncertainty in these comparisons is large enough to encompass most of the drifts identified in other comparisons. In parallel, the MLS v4 N2O product is shown to be generally decreasing over the same period (when an increase in stratospheric N2O is expected, reflecting a secular growth in emissions), with a more pronounced drift in the lower stratosphere than that found for H2O. Comparisons to ACE-FTS and to MLS N2O observations in a different spectral region, with the latter available from 2004 to 2013, indicate an altitude-dependent drift, growing from 5 % per decade or less in the mid-stratosphere to as much as 15 % per decade in the lower stratosphere. Detailed investigations of the behavior of the MLS 190 GHz subsystem reveal a drift in its “sideband fraction” (the relative sensitivity of the 190 GHz receiver to the two different parts of the microwave spectrum that it observes). Our studies indicate that sideband fraction drift accounts for much of the observed changes in the MLS H2O product and some portion of the changes seen in N2O. The 190 GHz sideband fraction drift has been corrected in the new “version 5” (v5) MLS algorithms, which have now been used to reprocess the entire MLS record. As a result of this correction, the MLS v5 H2O record shows no statistically significant drifts compared to ACE-FTS. However, statistically significant drifts remain between MLS v5 and frost point measurements, although they are reduced. Drifts in v5 N2O are about half the size of those in v4 but remain statistically significant. Scientists are advised to use MLS v5 data in all future studies. Quantification of interregional and seasonal to annual changes in MLS H2O and N2O will not be affected by the drift. However, caution is advised in studies using the MLS record to examine long-term (multiyear) variability and trends in either of these species, especially N2O; such studies should only be undertaken in consultation with the MLS team. Importantly, this drift does not affect any of the MLS observations made in other spectral regions such as O3, HCl, CO, ClO, or temperature.

Redistribution of total reactive nitrogen in the lowermost Arctic stratosphere during the cold winter 2015/2016

During winter 2015/2016 the Arctic stratosphere was characterized by extraordinarily low temperatures in connection with the occurrence of extensive polar stratospheric clouds. From mid of December 2015 until mid of March 2016 the German research aircraft HALO (High Altitude and Long–Range Research Aircraft) was deployed to probe the lowermost stratosphere in the Arctic region within the POLSTRACC (Polar Stratosphere in a Changing Climate) mission. More than twenty flights have been conducted out of Kiruna/Sweden and Oberpfaffenhofen/Germany, covering the whole winter period. Besides total reactive nitrogen (NOy), observations of nitrous oxide, nitric acid, ozone and water were used for this study. Total reactive nitrogen and its partitioning between gas- and particle phase are key parameters for understanding processes controlling the ozone budget in the polar winter stratosphere. The redistribution of total reactive nitrogen was evaluated by using tracer–tracer correlations. In January air masses with extensive nitrification were encountered at altitudes between 12 and 15 km. The excess NOy amounted up to about 6 ppb. During several flights, along with gas–phase nitrification, indications for extensive occurrence of nitric acid containing particles at flight altitude were found. These observations support the assumption of sedimentation and subsequent evaporation of nitric acid containing particles leading to redistribution of total reactive nitrogen. Remnants of nitrified air masses have been observed until mid of March. Between end of February and mid of March also de-nitrified air masses have been observed in connection with high potential temperatures. Using tracer–tracer correlations, missing total reactive nitrogen was estimated to amount up to 6 ppb. This indicates the downward transport of air masses that have been denitrified during the earlier winter phase. Observations within POLSTRACC, at the bottom of the vortex, reflect heterogeneous processes from the overlying Arctic winter stratosphere. The comparison of the observations with CLaMS model simulations confirm and complete the picture arising from the present measurements. The simulations confirm, that the ensemble of all observations is representative for the vortex–wide vertical NOy-redistribution.

Earth Imaging From the Surface of the Moon With a DSCOVR/EPIC-Type Camera

The Earth Polychromatic Imaging Camera (EPIC) on the Deep Space Climate Observatory (DSCOVR) satellite observes the entire Sun-illuminated Earth from sunrise to sunset from the L1 Sun-Earth Lagrange point. The L1 location, however, confines the observed phase angles to ∼2°–12°, a nearly backscattering direction, precluding any information on the bidirectional surface reflectance factor (BRF) or cloud/aerosol phase function. Deploying an analog of EPIC on the Moon’s surface would offer a unique opportunity to image the full range of Earth phases, including observing ocean/cloud glint reflection for different phase angles; monitoring of transient volcanic clouds; detection of circum-polar mesospheric and stratospheric clouds; estimating the surface BRF and full phase-angle integrated albedo; and monitoring of vegetation characteristics for different phase angles.

Mountain-wave-induced polar stratospheric clouds and their representation in the global chemistry model ICON-ART

Polar stratospheric clouds (PSCs) are a driver for ozone depletion in the lower polar stratosphere. They provide surface for heterogeneous reactions activating chlorine and bromine reservoir species during the polar night. The large-scale effects of PSCs are represented by means of parameterisations in current global chemistry–climate models, but one process is still a challenge: the representation of PSCs formed locally in conjunction with unresolved mountain waves. In this study, we investigate direct simulations of PSCs formed by mountain waves with the ICOsahedral Nonhydrostatic modelling framework (ICON) with its extension for Aerosols and Reactive Trace gases (ART) including local grid refinements (nesting) with two-way interaction. Here, the nesting is set up around the Antarctic Peninsula, which is a well-known hot spot for the generation of mountain waves in the Southern Hemisphere. We compare our model results with satellite measurements of PSCs from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and gravity wave observations of the Atmospheric Infrared Sounder (AIRS). For a mountain wave event from 19 to 29 July 2008 we find similar structures of PSCs as well as a fairly realistic development of the mountain wave between the satellite data and the ICON-ART simulations in the Antarctic Peninsula nest. We compare a global simulation without nesting with the nested configuration to show the benefits of adding the nesting. Although the mountain waves cannot be resolved explicitly at the global resolution used (about 160 km), their effect from the nested regions (about 80 and 40 km) on the global domain is represented. Thus, we show in this study that the ICON-ART model has the potential to bridge the gap between directly resolved mountain-wave-induced PSCs and their representation and effect on chemistry at coarse global resolutions.

Climate change favours large seasonal loss of Arctic ozone

Chemical loss of Arctic ozone due to anthropogenic halogens is driven by temperature, with more loss occurring during cold winters favourable for formation of polar stratospheric clouds (PSCs). We show that a positive, statistically significant rise in the local maxima of PSC formation potential (PFPLM) for cold winters is apparent in meteorological data collected over the past half century. Output from numerous General Circulation Models (GCMs) also exhibits positive trends in PFPLM over 1950 to 2100, with highest values occurring at end of century, for simulations driven by a large rise in the radiative forcing of climate from greenhouse gases (GHGs). We combine projections of stratospheric halogen loading and humidity with GCM-based forecasts of temperature to suggest that conditions favourable for large, seasonal loss of Arctic column O3 could persist or even worsen until the end of this century, if future abundances of GHGs continue to steeply rise.