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Social distancing to combat the COVID-19 pandemic has led to widespread reductions in air pollutant emissions. Quantifying these changes requires a business-as-usual counterfactual that accounts for the synoptic and seasonal variability of air pollutants. We use a machine learning algorithm driven by information from the NASA GEOS-CF model to assess changes in nitrogen dioxide (NO2) and ozone (O3) at 5756 observation sites in 46 countries from January through June 2020. Reductions in NO2 coincide with the timing and intensity of COVID-19 restrictions, ranging from 60 % in severely affected cities (e.g., Wuhan, Milan) to little change (e.g., Rio de Janeiro, Taipei). On average, NO2 concentrations were 18 (13–23) % lower than business as usual from February 2020 onward. China experienced the earliest and steepest decline, but concentrations since April have mostly recovered and remained within 5 % of the business-as-usual estimate. NO2 reductions in Europe and the US have been more gradual, with a halting recovery starting in late March. We estimate that the global NOx (NO + NO2) emission reduction during the first 6 months of 2020 amounted to 3.1 (2.6–3.6) TgN, equivalent to 5.5 (4.7–6.4) % of the annual anthropogenic total. The response of surface O3 is complicated by competing influences of nonlinear atmospheric chemistry. While surface O3 increased by up to 50 % in some locations, we find the overall net impact on daily average O3 between February–June 2020 to be small. However, our analysis indicates a flattening of the O3 diurnal cycle with an increase in nighttime ozone due to reduced titration and a decrease in daytime ozone, reflecting a reduction in photochemical production. The O3 response is dependent on season, timescale, and environment, with declines in surface O3 forecasted if NOx emission reductions continue.

Magnetic resonance spectroscopy is one of the most important tools in chemical and bio-medical research. However, sensitivity limitations typically restrict imaging resolution to ~ 10 µm. Here we bring quantum control to the detection of chemical systems to demonstrate high-resolution electron spin imaging using the quantum properties of an array of nitrogen-vacancy centres in diamond. Our electron paramagnetic resonance microscope selectively images electronic spin species by precisely tuning a magnetic field to bring the quantum probes into resonance with the external target spins. This provides diffraction limited spatial resolution of the target spin species over a field of view of 50 × 50 µm 2 with a spin sensitivity of 10 4 spins per voxel or ∼100 zmol. The ability to perform spectroscopy and dynamically monitor spin-dependent redox reactions at these scales enables the development of electron spin resonance and zepto-chemistry in the physical and life sciences. Electron paramagnetic resonance spectroscopy has important scientific and medical uses but improving the resolution of conventional methods requires cryogenic, vacuum environments. Simpson et al. show nitrogen vacancy centres can be used for sub-micronmetre imaging with improved sensitivity in ambient conditions.

Toxic nitrogen oxides produced by high temperature combustion are prevalent in urban environments, contributing to a significant health burden. Nitrogen oxides such as NO2 and HONO in pollution are important for hydroxyl radical (OH) production and overall oxidative capacity in urban environments; however, current mechanisms cannot explain high daytime levels of HONO observed in many urban and rural locations around the world. Here we present HONO, NO2 and aerosol extinction vertical distributions retrieved from multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements in suburban Melbourne, which are the first MAX-DOAS results from the Australian continent. Using the optimal estimation algorithm HEIPRO we show that vertical profiles for NO2 and HONO can be calculated with a low dependence on the retrieval forward model and a priori parameters, despite a lack of independent co-located aerosol or trace gas measurements. Between December 2016 and April 2017 average peak NO2 values of 8±2 ppb indicated moderate traffic pollution levels, and high daytime peak values of HONO were frequently detected, averaging 220±30 ppt in the middle of the day. HONO levels measured in Melbourne were typically lower than those recorded in the morning in other places around the world, indicating minimal overnight accumulation, but peaked in the middle of the day to be commensurate with midday concentrations in locations with much higher NO2 pollution. Regular midday peaks in the diurnal cycle of HONO surface concentrations have only previously been reported in rural locations. The HONO measured implies a daytime source term 1 ppb h−1 above the predicted photostationary state (PSS) concentration and represents an OH radical source up to 4 times stronger than from ozone photolysis alone in the lowest 500 m of the troposphere. The dependence of the high midday HONO levels on soil moisture, combined with the observed diurnal and vertical profiles, provides evidence for a strong photoactivated and ground-based daytime HONO source.

Global shipping fuel sulphur content regulations introduced in 2020 reduced the radiative cooling effects of sulfate aerosol over the ocean. Here we use the WRF-Chem model to estimate the effect these regulations have had on aerosols, clouds and solar radiation at the Great Barrier Reef, where climate change is increasing the frequency of mass coral bleaching events. During February 2022, the build-up to a La Niña mass coral bleaching event, we find 11 Wm −2 extra daytime downwards shortwave radiation reaches the reef post-sulfate regulation, compared to the control pre-regulation scenario. The enhancement is dominated by clear-sky-only forcing changes and less severe in cloudier and windier periods. Persistent incoming shortwave radiation enhancements on the order of 5-11 Wm −2 likely lead to sea-surface temperature increases of 0.05-0.15 °C, implying that during bleaching-conducive conditions, 5-10% additional thermal stress is felt by GBR corals now than before the regulation of ship sulfate emissions. Reduced sulfate aerosols due to ship fuel regulation may increase shortwave radiation on the Great Barrier Reef, exacerbating the impact of marine heatwaves on coral bleaching, according to model analysis of ship emission impacts on aerosols, clouds and solar radiation.

Nitrogen oxides (NOx≡NO+NO2) in the NOx-limited upper troposphere (UT) are long-lived and so have a large influence on the oxidizing capacity of the troposphere and formation of the greenhouse gas ozone. Models misrepresent NOx in the UT, and observations to address deficiencies in models are sparse. Here we obtain a year of near-global seasonal mean mixing ratios of NO2 in the UT (450–180 hPa) at 1∘×1∘ by applying cloud-slicing to partial columns of NO2 from TROPOMI. This follows refinement of the cloud-slicing algorithm with synthetic partial columns from the GEOS-Chem chemical transport model. TROPOMI, prior to cloud-slicing, is corrected for a 13 % underestimate in stratosphericNO2 variance and a 50 % overestimate in free-tropospheric NO2 determined by comparison to Pandora total columns at high-altitude free-tropospheric sites at Mauna Loa, Izaña, and Altzomoni and MAX-DOAS and Pandora tropospheric columns at Izaña. Two cloud-sliced seasonal mean UTNO2 products for June 2019 to May 2020 are retrieved from corrected TROPOMI total columns using distinct TROPOMI cloud products that assume clouds are reflective boundaries (FRESCO-S) or water droplet layers (ROCINN-CAL). TROPOMI UT NO2 typically ranges from 20–30 pptv over remote oceans to >80 pptv over locations with intense seasonal lightning. Spatial coverage is mostly in the tropics and subtropics with FRESCO-S and extends to the midlatitudes and polar regions with ROCINN-CAL, due to its greater abundance of optically thick clouds and wider cloud-top altitude range. TROPOMI UT NO2 seasonal means are spatially consistent (R=0.6–0.8) with an existing coarser spatial resolution (5∘ latitude × 8∘ longitude) UT NO2 product from the Ozone Monitoring Instrument (OMI). UT NO2 from TROPOMI is 12–26 pptv more than that from OMI due to increase in NO2 with altitude from the OMI pressure ceiling (280 hPa) to that for TROPOMI (180 hPa), but possibly also due to altitude differences in TROPOMI and OMI cloud products andNO2 retrieval algorithms. The TROPOMI UT NO2 product offers potential to evaluate and improve representation of UT NOx in models and supplement aircraft observations that are sporadic and susceptible to large biases in the UT.

South-eastern Australia has been identified by modelling studies as a hotspot of biogenic volatile organic compound (VOC) emissions; however, long-term observational VOC studies are lacking in this region. Here, 2.5 years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) formaldehyde (HCHO) measurements in Australasia are presented, from Broadmeadows, in northern Melbourne, Australia, and from Lauder, a rural site in the South Island of New Zealand. Across the measurement period from December 2016 to November 2019, the mean formaldehyde columns measured by the MAX-DOAS were 2.50±0.61×1015 molec. cm−2 at Lauder and 5.40±1.59×1015 molec. cm−2 at Broadmeadows. In both locations, the seasonal cycle showed a pronounced peak in Austral summer (December–January–February) consistent with temperature-dependent formaldehyde production from biogenic precursor gases. The amplitude of the seasonal cycle was 0.7×1015 molec. cm−2 at Lauder, and it was 2.0×1015 molec. cm−2 at Broadmeadows. The Lauder MAX-DOAS HCHO measurements are compared with 27 months of co-located Fourier transform infrared (FTIR) observations. The seasonal variation of Lauder MAX-DOAS HCHO, smoothed by the FTIR averaging kernels, showed good agreement with the FTIR measurements, with a linear regression slope of 1.03 and an R2 of 0.66 for monthly averaged formaldehyde partial columns (0–4 km). In addition to ground-based observations, a clear way to address the VOC measurement gap in areas such as Australasia is with satellite measurements. Here, we demonstrate that the TROPOspheric Monitoring Instrument (TROPOMI) can be used to distinguish formaldehyde hotspots in forested and agricultural regions of south-eastern Australia. The MAX-DOAS measurements are also compared to TROPOMI HCHO vertical columns at Lauder and Melbourne; very strong monthly average agreement is found for Melbourne (regression slope of 0.61 and R2 of 0.95) and a strong agreement is found at Lauder (regression slope of 0.73 and R2 of 0.61) for MAX-DOAS vs. TROPOMI between May 2018 and November 2019. This study, the first long-term satellite comparison study using MAX-DOAS in the Southern Hemisphere, highlights the improvement offered by TROPOMI's high resolution over previous satellite products and provides the groundwork for future studies using ground-based and satellite DOAS for studying VOCs in Australasia.

Recent temperature records have triggered debate about whether global warming is accelerating. Here, we examine for acceleration and explore possible causes for regional differences using gridded surface temperature data. We find that global and regional warming is accelerating, and on average, regions with low Human Development Index (HDI) experienced much higher accelerated warming in comparison to regions with high HDI. However, some regions of low HDI with a large population experienced slow acceleration due to high local aerosol emissions. Since aerosol negative forcing impacts are short‐lived and localized, rapid future reduction of aerosol emissions without a concurrent reduction in GHG emissions could have major compounding impacts. Such a pathway, similar to most 21st century scenarios, could expose a large fraction of the world's most vulnerable people to sudden warming acceleration and heat stress associated impacts. These results call for targeted climate adaptation strategies directing attention to low‐socioeconomic aerosol masked regions. Plain Language Summary The issue of whether climate change is accelerating has sparked heated debate in recent months. Here, we examine for acceleration in warming rates and explore possible causes for regional differences. We find, the rate of global warming is accelerating, and show that regions with large population and low socioeconomic development experience reduced acceleration due to high local aerosol emissions. As we transition to clean‐energy alternatives, rapid reduction in aerosol emissions without a concurrent reduction in greenhouse gas emissions could expose a large fraction of the world's most vulnerable people to a sudden acceleration of warming. This would also increase exposure to more intense and frequent heat extremes for highly vulnerable populations. These results call for targeted climate adaptation strategies that direct attention to low‐socioeconomic aerosol masked regions. Key Points The globe and most locations have experienced acceleration of warming over the last century Regions which imposed clean air acts in the late twentieth century have experienced a greater increase in warming trends over time Highly populated urban areas with low human development index have experienced lower acceleration linked with high local aerosol emissions

Detailed examination of the impact of modern space launches on the Earth's atmosphere is crucial, given booming investment in the space industry and an anticipated space tourism era. We develop air pollutant emissions inventories for rocket launches and re‐entry of reusable components and debris in 2019 and for a speculative space tourism scenario based on the recent billionaire space race. This we include in the global GEOS‐Chem model coupled to a radiative transfer model to determine the influence on stratospheric ozone (O3) and climate. Due to recent surge in re‐entering debris and reusable components, nitrogen oxides from re‐entry heating and chlorine from solid fuels contribute equally to all stratospheric O3 depletion by contemporary rockets. Decline in global stratospheric O3 is small (0.01%), but reaches 0.15% in the upper stratosphere (∼5 hPa, 40 km) in spring at 60–90°N after a decade of sustained 5.6% a−1 growth in 2019 launches and re‐entries. This increases to 0.24% with a decade of emissions from space tourism rockets, undermining O3 recovery achieved with the Montreal Protocol. Rocket emissions of black carbon (BC) produce substantial global mean radiative forcing of 8 mW m−2 after just 3 years of routine space tourism launches. This is a much greater contribution to global radiative forcing (6%) than emissions (0.02%) of all other BC sources, as radiative forcing per unit mass emitted is ∼500 times more than surface and aviation sources. The O3 damage and climate effect we estimate should motivate regulation of an industry poised for rapid growth. Plain Language Summary It is imperative that we understand the current and future risks to Earth's atmosphere posed by pollution from rocket launches and re‐entry heating of reusable and discarded rocket parts and historical debris. Rockets, unlike other anthropogenic pollution sources, emit gaseous and solid chemicals directly into the upper atmosphere. We compile inventories of these chemicals from rocket launches in 2019 and projections of future growth and speculative space tourism activity. We incorporate these in a 3D atmospheric chemistry model to simulate the impact on climate and the protective stratospheric ozone layer. We find that loss of ozone due to current rockets is small, but that routine space tourism launches may undermine progress made by the Montreal Protocol in reversing ozone depletion in the Arctic springtime upper stratosphere. The BC (or soot) particles from rockets are also of great concern, as these are almost five hundred times more efficient at warming the atmosphere than all other sources of soot combined. These findings demonstrate an urgent need to develop environmental regulation to mitigate damage from this rapidly growing industry. Key Points Air pollutant emission inventory for current space sector and future tourism input to a coupled chemistry and radiative transfer model Upper stratospheric Arctic ozone loss from launch chlorine and re‐entry nitrogen oxide emissions undermines Montreal Protocol success Warming efficiency of space tourism (soot) emissions about 500‐times greater than surface and aircraft sources of soot

Routine observations of the vertical distribution of tropospheric nitrogen oxides (NOx ≡ NO + NO2) are severely lacking, despite the large influence of NOx on climate, air quality, and atmospheric oxidants. Here, we derive vertical profiles of global seasonal mean tropospheric NO2 by applying the cloud-slicing method to TROPOspheric Monitoring Instrument (TROPOMI) columns of NO2 retrieved above optically thick clouds. The resultant NO2 is provided at a horizontal resolution of 1° × 1° for multiple years (June 2018 to May 2022), covering five layers of the troposphere: two layers in the upper troposphere (180–320 hPa and 320–450 hPa), two layers in the middle troposphere (450–600 hPa and 600–800 hPa), and the marine boundary layer (800 hPa to the Earth's surface). NO2 in the terrestrial boundary layer is obtained as the difference between TROPOMI tropospheric columns and the integrated column of cloud-sliced NO2 in all layers above the boundary layer. Cloud-sliced NO2 typically ranges from 20–60 pptv throughout the free troposphere, and spatial coverage ranges from > 60 % in the mid-troposphere to < 20 % in the upper troposphere and boundary layer. When both datasets are abundant and sampling coverage is commensurate, our product is similar (within 10–15 pptv) to NO2 data from NASA DC-8 aircraft campaigns. However, such instances are rare. We use cloud-sliced NO2 to critique current knowledge of the vertical distribution of global NO2, as simulated by the GEOS-Chem chemical transport model, which has been updated to include peroxypropionyl nitrate (PPN) and aerosol nitrate photolysis, liberating NO2 in the lower troposphere and mid-troposphere for aerosol nitrate photolysis and in the upper troposphere for PPN. Multiyear GEOS-Chem and cloud-sliced means are compared to mitigate the influence of interannual variability. We find that for cloud-sliced NO2, interannual variability is ∼ 10 pptv over remote areas and ∼ 25 pptv over areas influenced by lightning and surface sources. The model consistently underestimates NO2 across the remote marine troposphere by ∼ 15 pptv. At the northern midlatitudes, GEOS-Chem overestimates mid-tropospheric NO2 by 20–50 pptv as NOx production per lightning flash is parameterised to be almost double that of the rest of the world. There is a critical need for in situ NO2 measurements in the tropical terrestrial troposphere to evaluate cloud-sliced NO2 there. The model and cloud-sliced NO2 discrepancies identified here need to be investigated further to ensure confident use of models to understand and interpret factors affecting the global distribution of tropospheric NOx, ozone, and other oxidants.