Emission Perturbations Research Articles

Energy Gain Kernel for Climate Feedbacks. Part I: Formulation and Physical Understanding

Abstract This paper introduces a climate feedback kernel, referred to as the “energy gain kernel” (EGK). EGK allows for separating the net longwave radiative energy perturbations given by a Planck feedback matrix explicitly into thermal energy emission perturbations of individual layers and thermal radiative energy flux convergence perturbations at individual layers resulting from the coupled atmosphere–surface temperature changes in response to the unit forcing in individual layers. The former is represented by the diagonal matrix of a Planck feedback matrix and the latter by EGK. Elements of EGK are all positive, representing amplified energy perturbations at a layer where forcing is imposed and energy gained at other layers, both of which are achieved through radiative thermal coupling within an atmosphere–surface column. Applying EGK to input energy perturbations, whether external or internal due to responses of nontemperature feedback processes to external energy perturbations, such as water vapor and albedo feedbacks, yields their total energy perturbations amplified through radiative thermal coupling within an atmosphere–surface column. As the strength of EGK depends exclusively on climate mean states, it offers a solution for effectively and objectively separating control climate state information from climate perturbations for climate feedback studies. Given that an EGK comprises critical climate mean state information on mean temperature, water vapor, clouds, and surface pressure, we envision that the diversity of EGK across different climate models could provide insight into the inquiry of why, under the same anthropogenic greenhouse gas increase scenario, different models yield varying degrees of global mean surface warming. Significance Statement The wide range of 2.5°–4.0°C in global warming projections by climate models hinders our ability to predict its impacts. The newly introduced energy gain kernel (EGK) provides critical information for climate mean infrared opacity, which is collectively determined by climate mean temperature, water vapor, clouds, and surface pressure fields. EGK is directly derived from physical principles without additional definition. EGK captures the temperature feedback’s amplification of energy perturbations initiated from both external forcing and internal nontemperature feedback processes. EGK allows for disentangling positive and negative aspects of temperature feedback, rectifying the common misconception in existing temperature kernels that portray temperature feedback as predominantly negative. The diversity of EGK across different climate models may help explain their varying global warming degrees.

Revisiting day-of-week ozone patterns in an era of evolving US air quality

Abstract. Past work has shown that traffic patterns in the USA and resulting NOx emissions vary by day of week, with NOx emissions typically being higher on weekdays than weekends. This pattern of emissions leads to different levels of ozone on weekends versus weekdays and can be leveraged to understand how local ozone formation changes in response to NOx emission perturbations in different urban areas. Specifically, areas with lower NOx but higher ozone on the weekends (the weekend effect) can be characterized as NOx-saturated and areas with both lower NOx and ozone on weekends (the weekday effect) can be characterized as NOx-limited. In this analysis, we assess maximum daily 8 h average (MDA8) ozone weekend–weekday differences across 51 USA nonattainment areas using 18 years of observed and modeled data from 2002–2019, using the following two metrics: mean MDA8 ozone and percentage of days with MDA8 ozone > 70 ppb (parts per billion). In addition, we quantify the modeled and observed trends in these weekend–weekday differences across this period of substantial NOx emission reductions in the USA. The model assessment is carried out using U.S. Environmental Protection Agency (EPA)'s Air QUAlity TimE Series Project (EQUATES) Community Multiscale Air Quality (CMAQ) model dataset. We identify three types of MDA8 ozone trends occurring across the USA, namely transitioning chemical regime, disappearing weekday effect, and no trend. The transitioning chemical regime trend occurs in a subset of large urban areas that were NOx-saturated (i.e., volatile organic compound (VOC)-limited) at the beginning of the analysis period but transitioned to mixed chemical regimes or NOx-limited conditions by the end of the analysis period. Nine areas have strong transitioning chemical regime trends using both modeled and observed data and with both metrics indicating strong agreement that they are shifting to more NOx-limited conditions: Milwaukee, Houston, Phoenix, Denver, the Northern Wasatch Front, the Southern Wasatch Front, Las Vegas, Los Angeles – San Bernardino County, Los Angeles – South Coast, and San Diego. The disappearing weekday effect was identified for multiple rural and agricultural areas of California which were NOx-limited for the entire analysis period but appear to become less influenced by local day-of-week emission patterns in more recent years. Finally, we discuss a variety of reasons why there are no trends in certain areas including complex impacts of heterogeneous source mixes and stochastic impacts of meteorology. Overall, this assessment finds that the EQUATES modeling simulations indicate more NOx-saturated conditions than the observations but do a good job of capturing year-to-year changes in weekend–weekday MDA8 ozone patterns.

Response of PM2.5 and O3 to Emission Reductions in Nanjing Based on Random Forest Algorithm

High levels of fine particulate matter (PM2.5) and ozone (O3) in ambient air affect climate change and also endanger human health and ecosystems. Air pollution in Nanjing has been improving since the implementation of the "Air Pollution Prevention and Control Action Plan" in 2013. However, Nanjing still faces PM2.5 and O3 pollution. Evaluating the response of pollutant concentrations to the reductions in precursor emissions is helpful to obtain effective strategies of emission reduction to improve pollution levels. The sensitive simulations of emission perturbation in atmospheric chemistry models directly demonstrate the response of pollution to the reductions in emissions. Nevertheless, these sensitive simulations are limited in computing time and resources. The random forest algorithm was trained by using the simulation results of the atmospheric chemical transport model (GEOS-Chem) in 2015. The changes in daily PM2.5 and daily maximum eight-hour O3 (MDA8 O3) concentrations in Nanjing in 2019 were efficiently predicted under different reduction scenarios of anthropogenic emissions. The simulations showed that the seasonal average of ρ(PM2.5) in Nanjing would decrease by 2-4 μg·m-3 with the reduction in anthropogenic emissions of 10% in 2019 in China. In the case of controlling only local emissions in Nanjing, the concentrations of PM2.5 in Nanjing decreased significantly without local anthropogenic emissions. Additionally, the simulations showed that the annual average of ρ(PM2.5) in Nanjing could be lower than the national secondary limit (35 μg·m-3) when the anthropogenic emission reduction in China was higher than 20% in 2019. For ozone, the equal proportional emission reductions in nitrogen oxides (NOx) and volatile organic pollutants (VOCs) of O3 precursors in China likely led to the increase in seasonal average concentrations of O3 in Nanjing. For the proportional reduction of anthropogenic emissions by 10%-50% in China, the seasonal average of ρ(MDA8 O3) in Nanjing in 2019 would increase by 1-3 μg·m-3 in spring, 1-4 μg·m-3 in autumn, and 3-11 μg·m-3 in winter, respectively, compared with that in the base simulation. With the reduction in anthropogenic NOx emission by 10% and VOCs by 20%, the seasonal average of ρ(MDA8 O3) in Nanjing would decrease by 3-6 μg·m-3. On this basis, further increasing the proportion (30%) of VOCs emission reduction could reduce the annual average of ρ(MDA8 O3) in Nanjing by 7 μg·m-3. However, the annual average of ρ(MDA8 O3) of Nanjing in 2019 increased by 1 μg·m-3, with the local emission reduction of NOx by 10% and VOCs by 30%. Therefore, this showed that the key to alleviate ozone pollution in Nanjing is a reasonable control ratio of ozone precursor emissions and the implementation of regional joint prevention and control. In order to effectively reduce the O3 pollution in Nanjing, the emission reduction ratio of NOx and VOCs in China should be less than 1:2. The response of pollutant concentrations to reductions in precursor emissions were efficiently obtained by the random forest algorithm and GEOS-Chem model. The simulations would provide the scientific basis for the emission control strategy to alleviate air pollution.

Emissions Background, Climate, and Season Determine the Impacts of Past and Future Pandemic Lockdowns on Atmospheric Composition and Climate

AbstractCOVID‐19 pandemic responses affected atmospheric composition and climate. These effects depend on the background emissions, climate, and season in which they occur. Although using multiple scenarios is common in explorations of long‐term climate change, they are rarely used to explore atmospheric composition or climate changes in response to transient emission perturbations on the scale of COVID‐19 lockdowns. We used the ModelE Earth system model to evaluate how atmospheric and climate impacts depend on the decade and season in which lockdowns occurred. Global COVID‐19‐related anomalies in aerosols and trace gases differed by up to an order of magnitude or more when comparing lockdowns in 1980, 2008, 2020, and 2051. Regional atmospheric composition anomalies tended to be largest when emissions were near a historical peak: 1980 in Europe and temperate North America, 2008 or 2020 in eastern Asia, and 2051 in south Asia. Regional aerosol direct effect anomalies were almost always less than 0.1 W m−2 during the first pandemic year, but over 0.1 W m−2 in Europe and exceeded 0.2 W m−2 in Europe and temperate North America in 1980, generally changing in tandem with regional emissions. In contrast, direct effect anomalies in Asia were positive in 1980 and negative in 2008, suggesting they may be primarily determined by exogenous emission anomalies. Shifting COVID‐19 onset in 2020 by 3, 6, or 9 months also altered atmospheric composition on the order of 2%–25% globally. In all scenarios, changes in surface temperature or precipitation appeared unrelated to local atmospheric compositional changes.

Optimal emission reduction scheme aimed at eliminating PM2.5 city pollution days within North China during a haze episode

Economic development is accompanied by pollutant emissions, and environmental management plans should be urgently formulated to maximize air quality improvement under the premise of minimizing total amount of precursor emissions. The purpose of this study was to establish an optimal emission reduction system through a linear programming method based on source analysis, fine particulate matter (PM2.5) sensitivity, emission status, and pollution conditions to readjust the industrial layout within China and to achieve the goal of eliminating PM2.5 city pollution days (PMCPDs) during a PM2.5 pollution episode in North China. The WRF-NAQPMS simulations showed that the total PM2.5 sensitivity (the impact of unit precursor emission on air quality) increased with increasing precursor emission perturbation, and the order of each precursor was primary PM2.5 > NOx > SO2 > NH3 > volatile organic compounds (VOCs) in most receptors. Compared to the equal proportion (EP) scenario, not only were the emission reduction ratios of primary PM2.5, SO2, NOx, NH3, and VOCs in North China approximately 7.27%, 9.78%, 10.27%, 5.09%, and 26.34% lower, respectively, but the air quality improvement was also greater under the optimal proportion (OP) scenario. North China could achieve the goal of eliminating PMCPDs under the OP scenario, while the number increased by thirteen in Northwest China. Through technological upgrading in industrial transfer from North China to Northwest China (OPTU scenario), the number of PMCPDs in North China could not only be eliminated but a zero-increase relative to the business as usual (BAU) scenario could also be achieved in Northwest China.

The Impact of Volatile Chemical Products, Other VOCs, and NOx on Peak Ozone in the Lake Michigan Region

AbstractHigh concentrations of ozone along the coastline of Lake Michigan are a persistent air quality management challenge. Complementing observations during the 2017 Lake Michigan Ozone Study (LMOS 2017), WRF‐Chem modeling was used to quantify sensitivity of modeled ozone (O3) to anthropogenic nitrogen oxides (NOx) and volatile organic compound (VOC) emissions, including to changes in volatile chemical product (VCP). The daily maximum 8 hr average (MDA8) over the high ozone region of Lake Michigan decreased by 2.7 ppb with exclusion of VCP from the inventory, and was sensitive to both NOx and VOC changes, with greater sensitivity to NOx. Close to urban centers, MDA8 ozone was VOC‐sensitive. Clusters of coastal receptor sites were identified based on similarity in response to emission perturbations, with most clusters being NOx‐sensitive and NOx‐sensitivity increasing with distance from major emission sources. The 2 June 2017 ozone event, which has received considerable focus, is shown to be atypical due to unusually strong and spatially extended VOC‐sensitive behavior. WRF‐Chem integrated reaction rate analysis was used to compute radical termination rates due to NOx (LNOx) and to radical‐radical reactions (LROx). LROx/LNOx and formaldehyde to NO2 ratio (FNR) were shown to be predictive of modeled MDA8 ozone sensitivity, but with variation in predictive power as a function of time of day, which has implications for air quality management use of FNR from geostationary satellites.

Using Ice Cores to Evaluate CMIP6 Aerosol Concentrations Over the Historical Era

AbstractThe radiative effect of anthropogenic aerosols is one of the largest uncertainties in Earth's energy budget over the industrial period. This uncertainty is in part due to sparse observations of aerosol concentrations in the pre‐satellite era. To address this lack of measurements, ice cores can be used, which contain the aerosol concentration record. To date, these observations have been under‐utilized for comparison to aerosol concentrations found in state‐of‐the‐art Earth system models (ESMs). Here we compare long term trends in concentrations of sulfate and black carbon (BC) between 15 ice cores and 11 ESMs over nine regions around the world during the period 1850–2000. We find that for sulfate concentration trends model results generally agree with ice core records, whereas for BC concentration the model trends differ from the records. Absolute concentrations of both investigated species are overestimated by the models, probably in part due to representation errors. However, we assume that biases in relative trends are not altered by these errors. Ice cores in the European Alps and Greenland record a maximum BC concentration before 1950, while most ESMs used in this study agree on a post‐1950 maximum. We source this bias to an error in BC emission inventories in Europe. Emission perturbation experiments using NorESM2‐LM support the observed finding that BC concentrations in Northern Greenland ice cores are recording European emissions. Errors in BC emission inventories have implications for all future and past studies where Coupled Model Intercomparison Project Phase 6 historical simulations are compared to observations relevant to aerosol forcing.

Changes in the Relative Importance of Biogenic Isoprene and Soil NOx Emissions on Ozone Concentrations in Nonattainment Areas of the United States

AbstractReductions in anthropogenic emissions have drawn increasing attention to the role of the biosphere in O3 production chemistry in U.S. cities. We report the results of chemical transport model sensitivity simulations exploring the relative impacts of biogenic isoprene and soil nitrogen oxides (NOx) emissions on O3 and its temporal variability. We compare scenarios with high and low anthropogenic NOx emissions representing the reductions that have occurred in recent decades. As expected, summertime O3 concentrations become less sensitive to perturbations in biogenic isoprene emissions as anthropogenic NOx emissions decline. However, we demonstrate for the first time that across policy relevant O3 nonattainment areas of the United States, O3 becomes more sensitive to perturbations in soil NOx emissions than to identical perturbations in isoprene emissions. We show that interannual variability in soil NOx emissions may now have larger impacts on interannual O3 variability than isoprene emissions in many areas where the latter would have dominated in the recent past.

Direct measurements of ozone response to emissions perturbations in California

Abstract. A new technique was used to directly measure O3 response to changes in precursor NOx and volatile organic compound (VOC) concentrations in the atmosphere using three identical Teflon smog chambers equipped with UV lights. One chamber served as the baseline measurement for O3 formation, one chamber added NOx, and one chamber added surrogate VOCs (ethylene, m-xylene, n-hexane). Comparing the O3 formation between chambers over a 3-hour UV cycle provides a direct measurement of O3 sensitivity to precursor concentrations. Measurements made with this system at Sacramento, California, between April–December 2020 revealed that the atmospheric chemical regime followed a seasonal cycle. O3 formation was VOC-limited (NOx-rich) during the early spring, transitioned to NOx-limited during the summer due to increased concentrations of ambient VOCs with high O3 formation potential, and then returned to VOC-limited (NOx-rich) during the fall season as the concentrations of ambient VOCs decreased and NOx increased. This seasonal pattern of O3 sensitivity is consistent with the cycle of biogenic emissions in California. The direct chamber O3 sensitivity measurements matched semi-direct measurements of HCHO/NO2 ratios from the TROPOspheric Monitoring Instrument (TROPOMI) aboard the Sentinel-5 Precursor (Sentinel-5P) satellite. Furthermore, the satellite observations showed that the same seasonal cycle in O3 sensitivity occurred over most of the entire state of California, with only the urban cores of the very large cities remaining VOC-limited across all seasons. The O3-nonattainment days (MDA8 O3>70 ppb) have O3 sensitivity in the NOx-limited regime, suggesting that a NOx emissions control strategy would be most effective at reducing these peak O3 concentrations. In contrast, a large portion of the days with MDA8 O3 concentrations below 55 ppb were in the VOC-limited regime, suggesting that an emissions control strategy focusing on NOx reduction would increase O3 concentrations. This challenging situation suggests that emissions control programs that focus on NOx reductions will immediately lower peak O3 concentrations but slightly increase intermediate O3 concentrations until NOx levels fall far enough to re-enter the NOx-limited regime. The spatial pattern of increasing and decreasing O3 concentrations in response to a NOx emissions control strategy should be carefully mapped in order to fully understand the public health implications.

Assessing the importance of nonlinearity for aircraft emissions' impact on O3 and PM2.5

In this study we utilize the Decoupled Direct Method (HDDM-3D) as implemented in the Community Multiscale Air Quality Model (CMAQ) to calculate first and second order sensitivity coefficients of O 3 and PM 2.5 concentrations with respect to aviation emissions during landing and takeoff (LTO) cycles at ten individual airports; five located in regions of attainment of O 3 and PM 2.5 NAAQS: Boston Logan (BOS), Kansas City (MCI), Raleigh-Durham (RDU), Seattle-Tacoma (SEA), and Tucson (TUS); and five airports in current nonattainment areas: Chicago O'Hare (ORD), Hartsfield- Jackson Atlanta (ATL), New York John F. Kennedy (JFK), Los Angeles (LAX), and Charlotte- Douglas (CLT). We utilize these coefficients in an attainment/nonattainment emission decrease/increase analysis to determine the importance of including second order sensitivity coefficients for quantifying O 3 and PM 2.5 concentration responses to LTO aircraft emission reductions near the airport. Sensitivity coefficients help to determine distinct chemical regimes, NO X -limited versus NO X -inhibited for the case of O 3 formation, and NH 3 -rich versus NH 3 -poor for the case of PM 2.5 formation. Overall, we find that NO X LTO emissions are the largest contributor to any potential nonlinearity in O 3 and PM 2.5 formation through LTO emissions. However, when utilizing Taylor series expansions to estimate O 3 and PM 2.5 concentration responses under LTO emission perturbation scenarios, differences in responses calculated using only first order coefficients and responses calculated using both first and second order coefficients were less than 1% for LTO emission perturbations less than 100%. Hence, we find from the results in this study that first order sensitivity coefficients are sufficient for constructing accurate LTO emissions perturbation scenarios. This study also demonstrates through the analyses performed, an illustration of how HDDM-based sensitivity calculations can be used to assess sector-specific impacts on attainment designations. • Sensitivities can help to determine distinct chemical regimes. • Aircraft NOx emissions contribute most to nonlinear chemistry. • Higher order sensitivities not needed for aircraft emission reduction strategies. • Novel approach to determine emissions sector contribution to attainment designations.

Bias in CMIP6 models as compared to observed regional dimming and brightening

Abstract. Anthropogenic aerosol emissions have increased considerably over the last century, but climate effects and quantification of the emissions are highly uncertain as one goes back in time. This uncertainty is partly due to a lack of observations in the pre-satellite era, making the observations we do have before 1990 additionally valuable. Aerosols suspended in the atmosphere scatter and absorb incoming solar radiation and thereby alter the Earth's surface energy balance. Previous studies show that Earth system models (ESMs) do not adequately represent surface energy fluxes over the historical era. We investigated global and regional aerosol effects over the time period 1961–2014 by looking at surface downwelling shortwave radiation (SDSR). We used observations from ground stations as well as multiple experiments from eight ESMs participating in the Coupled Model Intercomparison Project Version 6 (CMIP6). Our results show that this subset of models reproduces the observed transient SDSR well in Europe but poorly in China. We suggest that this may be attributed to missing emissions of sulfur dioxide in China, sulfur dioxide being a precursor to sulfate, which is a highly reflective aerosol and responsible for more reflective clouds. The emissions of sulfur dioxide used in the models do not show a temporal pattern that could explain observed SDSR evolution over China. The results from various aerosol emission perturbation experiments from DAMIP, RFMIP and AerChemMIP show that only simulations containing anthropogenic aerosol emissions show dimming, even if the dimming is underestimated. Simulated clear-sky and all-sky SDSR do not differ greatly, suggesting that cloud cover changes are not a dominant cause of the biased SDSR evolution in the simulations. Therefore we suggest that the discrepancy between modeled and observed SDSR evolution is partly caused by erroneous aerosol and aerosol precursor emission inventories. This is an important finding as it may help interpret whether ESMs reproduce the historical climate evolution for the right or wrong reason.

Constraining the Twomey effect from satellite observations: issues and perspectives

Abstract. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

Assessing the manageable portion of ground-level ozone in the contiguous United States

ABSTRACT Regional air quality models are widely being used to understand the spatial extent and magnitude of the ozone non-attainment problem and to design emission control strategies needed to comply with the relevant ozone standard through direct emission perturbations. In this study, we examine the manageable portion of ground-level ozone using two simulations of the Community Multiscale Air Quality (CMAQ) model for the year 2010 and a probabilistic analysis approach involving 29 years (1990–2018) of historical ozone observations. The modeling results reveal that the reduction in the peak ozone levels from total elimination of anthropogenic emissions within the model domain is around 13–21 ppb for the 90th−100th percentile range of the daily maximum 8-hr ozone concentrations across the contiguous United States (CONUS). Large reductions in the 4th highest 8-hr ozone are seen in the regions of West (interquartile range (IQR) of 17–33%), South (IQR 22–34%), Central (IQR 19–31%), Southeast (IQR 25–34%), and Northeast (IQR 24–37%). However, sites in the western portion of the domain generally show smaller reductions even when all anthropogenic emissions are removed, possibly due to the strong influence of global background ozone, including sources such as intercontinental ozone transport, stratospheric ozone intrusions, wildfires, and biogenic precursor emissions. Probabilistic estimates of the exceedances for several hypothetical thresholds of the 4th highest 8-hr ozone indicate that, in some areas, exceedances of such hypothetical thresholds may occur even with no anthropogenic emissions due to the ever-present atmospheric stochasticity and the current global tropospheric ozone burden. Implications: Because air pollution is intricately linked to adverse health effects, National Ambient Air Quality Standards (NAAQS) have been established for criteria pollutants to safeguard human health and the environment. Areas not in compliance with the relevant standards are required to develop plans and policies to reduce their air pollution levels. Regional-scale air quality models are currently being used routinely to inform policies to identify the emissions reduction required to meet and maintain the NAAQS throughout the country. This paper examines the feasibility of the 4th highest ozone, which is used to derive the ozone design value for NAAQS, complying with various current and hypothetical 8-hr ozone thresholds over CONUS based on the information embedded in 29 years of historical ozone observations and two modeling scenarios with and without anthropogenic emissions loading.

Comprehensive analyses of source sensitivities and apportionments of PM<sub>2.5</sub> and ozone over Japan via multiple numerical techniques

Abstract. Source sensitivity and source apportionment are two major indicators representing source–receptor relationships, which serve as essential information when considering effective strategies to accomplish improved air quality. This study evaluated source sensitivities and apportionments of ambient ozone and PM2.5 concentrations over Japan with multiple numerical techniques embedded in regional chemical transport models, including a brute-force method (BFM), a high-order decoupled direct method (HDDM), and an integrated source apportionment method (ISAM), to update the source–receptor relationships considering stringent emission controls recently implemented in Japan and surrounding countries. We also attempted to understand the differences among source sensitivities and source apportionments calculated by multiple techniques. While a part of ozone concentrations was apportioned to domestic sources, their sensitivities were small or even negative; ozone concentrations were exclusively sensitive to transport from outside Japan. Although the simulated PM2.5 concentrations were significantly lower than those reported by previous studies, their sensitivity to transport from outside Japan was still relatively large, implying that there has been a reduction in Japanese emissions, similar to surrounding countries including China, due to implementation of stringent emission controls. HDDM allowed us to understand the importance of the non-linear responses of PM2.5 concentrations to precursor emissions. Apportionments derived by ISAM were useful in distinguishing various direct and indirect influences on ozone and PM2.5 concentrations by combining with sensitivities. The results indicate that ozone transported from outside Japan plays a key role in exerting various indirect influences on the formation of ozone and secondary PM2.5 components. While the sensitivities come closer to the apportionments when perturbations in emissions are larger in highly non-linear relationships – including those between NH3 emissions and NH4+ concentrations, NOx emissions and NO3- concentrations, and NOx emissions and ozone concentrations – the sensitivities did not reach the apportionments because there were various indirect influences including other sectors, complex photochemical reactions, and gas–aerosol partitioning. It is essential to consider non-linear influences to derive strategies for effectively suppressing concentrations of secondary pollutants.

Derivation and Validation of Sensor Brightness Temperatures for Advanced Microwave Sounding Unit-A Instruments

In this article, we first present a generalized methodology for deriving sensor brightness temperature sensor data records (SDR) from antenna temperature data records (TDR) applicable for Advanced Microwave Sounding Unit-A (AMSU-A) instruments. It includes corrections for antenna sidelobe contributions, antenna emission, and radiation perturbation due to the difference of Earth radiance in the main beam and that in the sidelobes that lie outside the main beam but within the Earth disk. For practical purposes, we simplify the methodology by neglecting the components other than the antenna sidelobe contributions to establish a consistent formulation with the legacy AMSU-A antenna pattern correction (APC) formula. The simplified formulation is then applied to the final AMSU-A instrument onboard the Metop-C satellite that was launched in November 2018, in order to compute APC coefficients for deriving SDR from TDR data. Furthermore, the performance of the calculated correction coefficients is validated by calculating the differences between the daily averaged AMSU-A (TDR and SDR) observations against radiative transfer model (O–B) simulations under clear sky conditions, and over open oceans. The validation results show that the derived temperature corrections are channel and scan position dependent, and can add 0.2–1.6 K to the antenna temperatures. In addition, the derived SDR O-B results exhibit a reduced and more symmetric scan angle-dependent bias when compared with corresponding TDR antenna temperatures.

Local and remote mean and extreme temperature response to regional aerosol emissions reductions

Abstract. The climatic implications of regional aerosol and precursor emissions reductions implemented to protect human health are poorly understood. We investigate the mean and extreme temperature response to regional changes in aerosol emissions using three coupled chemistry–climate models: NOAA GFDL CM3, NCAR CESM1, and NASA GISS-E2. Our approach contrasts a long present-day control simulation from each model (up to 400 years with perpetual year 2000 or 2005 emissions) with 14 individual aerosol emissions perturbation simulations (160–240 years each). We perturb emissions of sulfur dioxide (SO2) and/or carbonaceous aerosol within six world regions and assess the statistical significance of mean and extreme temperature responses relative to internal variability determined by the control simulation and across the models. In all models, the global mean surface temperature response (perturbation minus control) to SO2 and/or carbonaceous aerosol is mostly positive (warming) and statistically significant and ranges from +0.17 K (Europe SO2) to −0.06 K (US BC). The warming response to SO2 reductions is strongest in the US and Europe perturbation simulations, both globally and regionally, with Arctic warming up to 1 K due to a removal of European anthropogenic SO2 emissions alone; however, even emissions from regions remote to the Arctic, such as SO2 from India, significantly warm the Arctic by up to 0.5 K. Arctic warming is the most robust response across each model and several aerosol emissions perturbations. The temperature response in the Northern Hemisphere midlatitudes is most sensitive to emissions perturbations within that region. In the tropics, however, the temperature response to emissions perturbations is roughly the same in magnitude as emissions perturbations either within or outside of the tropics. We find that climate sensitivity to regional aerosol perturbations ranges from 0.5 to 1.0 K (W m−2)−1 depending on the region and aerosol composition and is larger than the climate sensitivity to a doubling of CO2 in two of three models. We update previous estimates of regional temperature potential (RTP), a metric for estimating the regional temperature responses to a regional emissions perturbation that can facilitate assessment of climate impacts with integrated assessment models without requiring computationally demanding coupled climate model simulations. These calculations indicate a robust regional response to aerosol forcing within the Northern Hemisphere midlatitudes, regardless of where the aerosol forcing is located longitudinally. We show that regional aerosol perturbations can significantly increase extreme temperatures on the regional scale. Except in the Arctic in the summer, extreme temperature responses largely mirror mean temperature responses to regional aerosol perturbations through a shift of the temperature distributions and are mostly dominated by local rather than remote aerosol forcing.

The changing role of organic nitrates in the removal and transport of NO<sub><i>x</i></sub>

Abstract. A better understanding of the chemistry of nitrogen oxides (NOx) is crucial to effectively reducing air pollution and predicting future air quality. The response of NOx lifetime to perturbations in emissions or in the climate system is set in large part by whether NOx loss occurs primarily by the direct formation of HNO3 or through the formation of alkyl and multifunctional nitrates (RONO2). Using 15 years of detailed in situ observations, we show that in the summer daytime continental boundary layer the relative importance of these two pathways can be well approximated by the relative likelihood that OH will react with NO2 or instead with a volatile organic compound (VOC). Over the past decades, changes in anthropogenic emissions of both NOx and VOCs have led to a significant increase in the overall importance of RONO2 chemistry to NOx loss. We find that this shift is associated with a decreased effectiveness of NOx emissions reductions on ozone production in polluted areas and increased transport of NOx from source to receptor regions. This change in chemistry, combined with changes in the spatial pattern of NOx emissions, is observed to be leading to a flatter distribution of NO2 across the United States, potentially transforming ozone air pollution from a local issue into a regional one.

Evaluating climate emulation: fundamental impulse testing of simple climate models

Abstract. Simple climate models (SCMs) are numerical representations of the Earth's gas cycles and climate system. SCMs are easy to use and computationally inexpensive, making them an ideal tool in both scientific and decision-making contexts (e.g., complex climate model emulation, parameter estimation experiments, climate metric calculations, and probabilistic analyses). Despite their prolific use, the fundamental responses of SCMs are often not directly characterized. In this study, we use fundamental impulse tests of three chemical species (CO2, CH4, and black carbon – BC) to understand the fundamental gas cycle and climate system responses of several comprehensive (Hector v2.0, MAGICC 5.3, MAGICC 6.0) and idealized (FAIR v1.0, AR5-IR) SCMs. We find that while idealized SCMs are widely used, they fail to capture the magnitude and timescales of global mean climate responses under emissions perturbations, which can produce biased temperature results. Comprehensive SCMs, which have physically based nonlinear forcing and carbon cycle representations, show improved responses compared to idealized SCMs. Even the comprehensive SCMs, however, fail to capture the response timescales to BC emission perturbations seen recently in two general circulation models. Some comprehensive SCMs also generally respond faster than more complex models to a 4×CO2 concentration perturbation, although this was not evident for lower perturbation levels. These results suggest where improvements should be made to SCMs. Further, we demonstrate here a set of fundamental tests that we recommend as a standard evaluation suite for any SCM. Fundamental impulse tests allow users to understand differences in model responses and the impact of model selection on results.

Foreign influences on tropospheric ozone over East Asia through global atmospheric transport

Abstract. Tropospheric ozone in East Asia is influenced by the transport of ozone from foreign regions around the world. However, the magnitudes and variations in such influences remain unclear. This study was performed to investigate the influences using a global chemical transport model, GEOS-Chem, through the tagged ozone and emission perturbation simulations. The results show that foreign ozone is transported to East Asia (20–60∘ N, 95–150∘ E) mainly through the middle and upper troposphere. In East Asia, the influence of foreign ozone increases rapidly with altitude. In the middle and upper troposphere, the regional mean concentrations of foreign ozone range from 32 to 65 ppbv, being 0.8–4.8 times higher than its native counterpart (11–18 ppbv). Annually, ∼60 % of foreign ozone in the East Asian middle and upper troposphere comes from North America (5–13 ppbv) and Europe (5–7 ppbv), as well as from foreign oceanic regions (9–21 ppbv). Over the East Asian tropospheric columns, foreign ozone appears most in spring when ozone concentrations in the foreign regions are high and the westerlies are strong and least in summer when the South Asian High blocks eastward foreign ozone from reaching East Asia south of 35∘ N. At the East Asian surface, the annual mean of foreign ozone concentrations is ∼22.2 ppbv, which is comparable to its native counterpart of ∼20.4 ppbv. In the meantime, the annual mean of anthropogenic ozone concentrations from foreign regions is ∼4.7 ppbv, half of which comes from North America (1.3 ppbv) and Europe (1.0 ppbv). Seasonally, foreign ozone concentrations at the East Asian surface are highest in winter (27.1 ppbv) and lowest in summer (16.5 ppbv). This strong seasonality is largely modulated by the East Asian monsoon (EAM) via its influence on vertical motion. The large-scale subsidence prevailing during the East Asian winter monsoon (EAWM) favours the downdraft of foreign ozone to the surface, while widespread convection in the East Asian summer monsoon (EASM) blocks such transport. Interannually, the variation in foreign ozone at the East Asian surface is found to be closely related to the intensity of the EAM. Specifically, the stronger the EAWM is in a winter, the more ozone from North America and Europe reaches the East Asian surface because of the stronger subsidence behind the East Asian trough. In summer, ozone from South and South-east Asia is reduced in strong EASM years due to weakened south-westerly monsoon winds. This study suggests substantial foreign influences on ozone at the East Asian surface and in its tropospheric columns. It also underscores the importance of the EAM in the seasonal and interannual variations in foreign influences on surface ozone in East Asia.

Impact of West Asia, Tibetan Plateau and local dust emissions on intra-seasonal oscillations of the South Asian monsoon rainfall

In the present study, we examine the responses of South Asian Monsoon (SAM) rainfall at intra-seasonal scale to remote dust emissions from west Asia, Tibetan Plateau and local dust emissions from within south Asia using a state of the art coupled atmosphere-slab ocean model CESM1-SOM. A series of systematically designed idealized simulations are carried out in such a way that dust emissions from the selected source regions are either perpetually suppressed or enhanced from these source regions and the response of the intra-seasonal oscillations (ISOs) of SAM rainfall to such perturbations in dust emissions are investigated. It is noted that the intra-seasonal variability of SAM rainfall is dominated by three different ISOs with periodicities of 10–20 days, 30–60 days and 60–90 days. Modulations in the characteristics of each of these three ISOs are studied for each of the dust perturbation experiments. Statistically robust K–S test and F test performed on the results from various dust perturbation experiments suggest that the perpetual perturbations in dust emissions from remote sources as well as locally from south Asia can significantly modulate the spatial and temporal structure of the ISOs of rainfall across scales during the monsoon season. Substantial changes are also noted in the spatial scales and propagation characteristics of ISOs attributable to the dust emission changes made over local and remote source regions in our idealized simulations. Our results suggest that perturbations in dust emissions over remote locations can substantially modulate the depth and duration of active and break rainfall events in the south Asian monsoon region. Results presented here have implications for better understanding and predicting the SAM rainfall variability at the intra-seasonal scales or at shorter time scales (~ less than a season) under variable dust emissions from remote and local source regions.