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A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.

Aerosol retrieval using ozone lidars in the ultraviolet spectral region is challenging but necessary for correcting aerosol interference in ozone retrieval and for studying the ozone–aerosol correlations. This study describes the aerosol retrieval algorithm for a tropospheric ozone lidar, quantifies the retrieval error budget, and intercompares the aerosol retrieval products at 299 nm with those at 532 nm from a high spectral resolution lidar (HSRL) and with those at 340 nm from an AErosol RObotic NETwork radiometer. After the cloud-contaminated data are filtered out, the aerosol backscatter or extinction coefficients at 30 m and 10 min resolutions retrieved by the ozone lidar are highly correlated with the HSRL products, with a coefficient of 0.95 suggesting that the ozone lidar can reliably measure aerosol structures with high spatiotemporal resolution when the signal-to-noise ratio is sufficient. The actual uncertainties of the aerosol retrieval from the ozone lidar generally agree with our theoretical analysis. The backscatter color ratio (backscatter-related exponent of wavelength dependence) linking the coincident data measured by the two instruments at 299 and 532 nm is 1.34±0.11, while the Ångström (extinction-related) exponent is 1.49±0.16 for a mixture of urban and fire smoke aerosols within the troposphere above Huntsville, AL, USA.

The NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) project included goals related to aerosol particle life cycle in convective regimes. Using the University of Wisconsin High Spectral Resolution Lidar system at Huntsville, Alabama, USA, and the NASA DC-8 research aircraft, we investigate the altitude dependence of aerosol, water vapor and Altocumulus (Ac) properties in the free troposphere from a canonical 12 August 2013 convective storm case as a segue to a presentation of a mission-wide analysis. It stands to reason that any moisture detrainment from convection must have an associated aerosol layer. Modes of covariability between aerosol, water vapor and Ac are examined relative to the boundary layer entrainment zone, 0 ∘C level, and anvil, a region known to contain Ac clouds and a complex aerosol layering structure (Reid et al., 2017). Multiple aerosol layers in regions warmer than 0 ∘C were observed within the planetary boundary layer entrainment zone. At 0 ∘C there is a proclivity for aerosol and water vapor detrainment from storms, in association with melting level Ac shelves. Finally, at temperatures colder than 0 ∘C, weak aerosol layers were identified above Cumulus congestus tops (∼0 and ∼-20 ∘C). Stronger aerosol signals return in association with anvil outflow. In situ data suggest that detraining particles undergo aqueous-phase or heterogeneous chemical or microphysical transformations, while at the same time larger particles are being scavenged at higher altitudes leading to enhanced nucleation. We conclude by discussing hypotheses regarding links to aerosol emissions and potential indirect effects on Ac clouds.

Multiband downwelling thermal measurements of zenith sky radiance, along with cloud boundary heights, were used in a retrieval algorithm to estimate cloud optical depth and effective particle diameter of thin ice clouds in the Canadian High Arctic. Ground-based thermal infrared (IR) radiances for 150 semitransparent ice clouds cases were acquired at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut, Canada (80° N, 86° W). We analyzed and quantified the sensitivity of downwelling thermal radiance to several cloud parameters including optical depth, effective particle diameter and shape, water vapor content, cloud geometric thickness and cloud base altitude. A lookup table retrieval method was used to successfully extract, through an optimal estimation method, cloud optical depth up to a maximum value of 2.6 and to separate thin ice clouds into two classes: (1) TIC1 clouds characterized by small crystals (effective particle diameter ≤ 30 µm), and (2) TIC2 clouds characterized by large ice crystals (effective particle diameter > 30 µm). The retrieval technique was validated using data from the Arctic High Spectral Resolution Lidar (AHSRL) and Millimeter Wave Cloud Radar (MMCR). Inversions were performed over three polar winters and results showed a significant correlation (R2 = 0.95) for cloud optical depth retrievals and an overall accuracy of 83 % for the classification of TIC1 and TIC2 clouds. A partial validation relative to an algorithm based on high spectral resolution downwelling IR radiance measurements between 8 and 21 µm was also performed. It confirms the robustness of the optical depth retrieval and the fact that the broadband thermal radiometer retrieval was sensitive to small particle (TIC1) sizes.

Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2–O2 collision complexes (O4) were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2–0.55 pptv IO and 32–36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and aircraft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6° N; 101.2 to 97.4° W). At 14.5 km, 5–10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12–20 degrees of freedom (DoF) and up to 500 m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 × 1013 molec cm−2 (RF12) and at least 0.5 × 1013 molec cm−2 (RF17, 0–10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 × 1012 molec cm−2 (RF12) and 2.5 × 1012 molec cm−2 (RF17) and glyoxal VCDs of 2.6 × 1014 molec cm−2 (RF12) and 2.7 × 1014 molec cm−2 (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 ± 5%, 0.1–0.2 pptv; glyoxal: 52 ± 5%, 3–20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

We use retrievals of aerosol extinction from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard the CALIPSO satellite to examine the vertical, horizontal and temporal variability of tropospheric Arctic aerosols during the period 2006–2012. We develop an empirical method that takes into account the difference in sensitivity between daytime and nighttime retrievals over the Arctic. Comparisons of the retrieved aerosol extinction to in situ measurements at Barrow (Alaska) and Alert (Canada) show that CALIOP reproduces the observed seasonal cycle and magnitude of surface aerosols to within 25 %. In the free troposphere, we find that daytime CALIOP retrievals will only detect the strongest aerosol haze events, as demonstrated by a comparison to aircraft measurements obtained during NASA's ARCTAS mission during April 2008. This leads to a systematic underestimate of the column aerosol optical depth by a factor of 2–10. However, when the CALIOP sensitivity threshold is applied to aircraft observations, we find that CALIOP reproduces in situ observations to within 20% and captures the vertical profile of extinction over the Alaskan Arctic. Comparisons with the ground-based high spectral resolution lidar (HSRL) at Eureka, Canada, show that CALIOP and HSRL capture the evolution of the aerosol backscatter vertical distribution from winter to spring, but a quantitative comparison is inconclusive as the retrieved HSRL backscatter appears to overestimate in situ observations by a factor of 2 at all altitudes. In the High Arctic (>70° N) near the surface (−1), followed by a sharp decline and a minimum in May–September (1–4 Mm−1), thus providing the first pan-Arctic view of Arctic haze seasonality. The European and Asian Arctic sectors display the highest wintertime extinctions, while the Atlantic sector is the cleanest. Over the Low Arctic (60–70° N) near the surface, CALIOP extinctions reach a maximum over land in summer due to boreal forest fires. During summer, we find that smoke aerosols reach higher altitudes (up to 4 km) over eastern Siberia and North America than over northern Eurasia, where they remain mostly confined below 2 km. In the free troposphere, the extinction maximum over the Arctic occurs in March–April at 2–5 km altitude and April–May at 5–8 km. This is consistent with transport from the midlatitudes associated with the annual maximum in cyclonic activity and blocking patterns in the Northern Hemisphere. A strong gradient in aerosol extinction is observed between 60° N and 70° N in the summer. This is likely due to efficient stratocumulus wet scavenging at high latitudes combined with the poleward retreat of the polar front. Interannual variability in the middle and upper troposphere is associated with biomass burning events (high extinctions observed by CALIOP in spring 2008 and summer 2010) and volcanic eruptions (Kasatochi in August 2008 and Sarychev in June 2009). CALIOP displays below-average extinctions observed from August 2009 through May 2010, which appear to be linked with a strongly negative Arctic Oscillation index.

Numerical simulations were carried out in a high-resolution two-dimensional framework to increase our understanding of aerosol indirect effects in mixed-phase stratiform clouds. Aerosol characteristics explored include insoluble particle type, soluble mass fraction, influence of aerosol-induced freezing point depression and influence of aerosol number concentration. Simulations were analyzed with a focus on the processes related to liquid phase microphysics, and ice formation was limited to droplet freezing. Of the aerosol properties investigated, aerosol insoluble mass type and its associated freezing efficiency was found to be most relevant to cloud lifetime. Secondary effects from aerosol soluble mass fraction and number concentration also alter cloud characteristics and lifetime. These alterations occur via various mechanisms, including changes to the amount of nucleated ice, influence on liquid phase precipitation and ice riming rates, and changes to liquid droplet nucleation and growth rates. Alteration of the aerosol properties in simulations with identical initial and boundary conditions results in large variability in simulated cloud thickness and lifetime, ranging from rapid and complete glaciation of liquid to the production of long-lived, thick stratiform mixed-phase cloud.

A climatology of particle scattering properties in the wintertime High Arctic troposphere, including vertical distributions and effective radii, is presented. The measurements were obtained using a lidar and cloud radar located at Eureka, Nunavut Territory (80° N, 86° W). Four different particle groupings are considered: boundary-layer ice crystals, ice clouds, mixed-phase clouds, and aerosols. Two-dimensional histograms of occurrence probabilities against depolarization, radar/lidar colour ratio and height are given. Colour ratios are related to particle minimum dimensions (i.e., widths rather than lengths) using a Mie scattering model. Ice cloud crystals have effective radii spanning 25–220 µm, with larger particles observed at lower altitudes. Topographic blowing snow residuals in the boundary layer have the smallest crystals at 15–70 µm. Mixed-phase clouds have water droplets and ice crystal precipitation in the 5–40 µm and 40–220 µm ranges, respectively. Ice cloud crystals have depolarization decreasing with height. The depolarization trend is associated with the large ice crystal sub-population. Small crystals depolarize more than large ones in ice clouds at a given altitude, and show constant modal depolarization with height. Ice clouds in the mid-troposphere are sometimes observed to precipitate to the ground. Water clouds are constrained to the lower troposphere (0.5–3.5 km altitude). Aerosols are most abundant near the ground and are frequently mixed with the other particle types. The data are used to construct a classification chart for particle scattering in wintertime Arctic conditions.

Ice crystals, also known as diamond dust, are suspended in the boundary layer air under clear sky conditions during most of the Arctic winter in Northern Canada. Occasionally ice crystal events can produce significantly thick layers with optical depths in excess of 2.0 even in the absence of liquid water clouds. Four case studies of high optical depth ice crystal events at Eureka in the Nunavut Territory of Canada during the winter of 2006/07 are presented. They show that the measured ice crystal surface infrared downward radiative forcing ranged from 8 to 36 W m−2 in the wavelength band from 5.6 to 20 μm for 532 nm optical depths ranging from 0.2 to 1.7. MODIS infrared and visible images and the operational radiosonde wind profile were used to show that these high optical depth events were caused by surface snow being blown off 600 to 800 m high mountain ridges about 20 to 30 km North-West of Eureka and advected by the winds towards Eureka as they settled towards the ground within the highly stable boundary layer. This work presents the first study that demonstrates the important role that surrounding topography plays in determining the occurrence of high optical depth ice crystal events from residual blowing snow that becomes a source of boundary layer ice crystals distinct from the classical diamond dust phenomenon.

Summer 2004 saw severe forest fires in Alaska and the Yukon Territory that were mostly triggered by lightning strikes. The area burned (>2.7×106 ha) in the year 2004 was the highest on record to date in Alaska. Pollutant emissions from the fires lead to violation of federal standards for air quality in Fairbanks. This paper studies deep convection events that occurred in the burning regions at the end of June 2004. The convection was likely enhanced by the strong forest fire activity (so-called pyro-convection) and penetrated into the lower stratosphere, up to about 3 km above the tropopause. Emissions from the fires did not only perturb the UT/LS locally, but also regionally. POAM data at the approximate location of Edmonton (53.5° N, 113.5° W) show that the UT/LS aerosol extinction was enhanced by a factor of 4 relative to unperturbed conditions. Simulations with the particle dispersion model FLEXPART with the deep convective transport scheme turned on showed transport of forest fire emissions into the stratosphere, in qualitatively good agreement with the enhancements seen in the POAM data. A corresponding simulation with the deep convection scheme turned off did not result in such deep vertical transport. Lidar measurements at Wisconsin on 30 June also show the presence of substantial aerosol loading in the UT/LS, up to about 13 km. In fact, the FLEXPART results suggest that this aerosol plume originated from the Yukon Territory on 25 June.