Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NO_x). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NO_x and temperature, and we compared this to previous observational studies. Under high-NO_x conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NO_x emissions. CB05 and RADM2 simulated more NO_x-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of O_x production; the net influence of peroxy nitrates increased net O_x production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NO_x emissions would be required to offset the additional ozone production due to an increase in temperature in the future.

Fine particulate matter (PM_2.5, aerodynamic diameter ≤2.5 µm) impacts the climate, reduces visibility and severely influences human health. The Indo-Gangetic Plain (IGP), home to about one-seventh of the world’s total population and a hotspot of aerosol loading, observes strong enhancements in the PM_2.5 concentrations towards winter. We performed high-resolution (12 km × 12 km) atmospheric chemical transport modeling (WRF-Chem) for the post-monsoon to winter transition to unravel the underlying dynamics and influences of regional emissions over the region. Model, capturing the observed variations to an extent, reveals that the spatial distribution of PM_2.5 having patches of enhanced concentrations (≥100 µgm⁻³) during post-monsoon, evolves dramatically into a widespread enhancement across the IGP region during winter. A sensitivity simulation, supported by satellite observations of fires, shows that biomass-burning emissions over the northwest IGP play a crucial role during post-monsoon. Whereas, in contrast, towards winter, a large-scale decline in the air temperature, significantly shallower atmospheric boundary layer, and weaker winds lead to stagnant conditions (ventilation coefficient lower by a factor of ~4) thereby confining the anthropogenic influences closer to the surface. Such changes in the controlling processes from post-monsoon to winter transition profoundly affect the composition of the fine aerosols over the IGP region. The study highlights the need to critically consider the distinct meteorological processes of west-to-east IGP and changes in dominant sources from post-monsoon to winter in the formulation of future pollution mitigation policies.

Surface-based measurements from the EMEP and Airbase networks are used to estimate the changes in surface ozone levels during the 1995–2014 period over Europe. We find significant ozone enhancements (0.20–0.59 µg m⁻³ yr⁻¹ for the annual means; P-value < 0.01 according to an F-test) over the European suburban and urban stations during 1995–2012 based on the Airbase sites. For European background ozone observed at EMEP sites, it is shown that a significantly decreasing trend in the 95th percentile ozone concentrations has occurred, especially at noon (0.9 µg m⁻³ yr⁻¹; P-value < 0.01), while the 5th percentile ozone concentrations continued to increase with a trend of 0.3 µg m⁻³ yr⁻¹ (P-value < 0.01) during the study period. With the help of numerical simulations performed with the global chemistry-climate model EMAC, the importance of anthropogenic emissions changes in determining these changes over background sites are investigated. The EMAC model is found to successfully capture the observed temporal variability in mean ozone concentrations, as well as the contrast in the trends of 95th and 5th percentile ozone over Europe. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels and that background ozone levels have been influenced by hemispheric transport, while climate variability generally regulated the inter-annual variations of surface ozone in Europe.

The seasonal variability of black carbon (BC) aerosols in India is studied using high resolution (10 km) BC simulations conducted using the Weather Research and Forecasting Model coupled with Chemistry. The model reproduces the observed seasonality of surface BC fairly well over most parts of India but fails to capture the seasonality in the Himalayas and deviates from the observed BC magnitude at several sites. The errors in modeled BC are attributed to uncertainties in BC emissions and their diurnal cycle, planetary boundary layer height underestimation, and aerosol processes. Model results show distinct but opposite seasonality of BC in the lower (LT) and free troposphere (FT) with BC showing winter maximum and summer minimum in the LT and vice versa in the FT. Our analysis shows that BC seasonality is not driven by seasonality of the anthropogenic emissions but by changes in the regional meteorology through weakening of the horizontal transport and strengthening of the vertical transport of BC during summertime compared to winter. BC in both the LT and FT comes mostly from anthropogenic emissions followed by biomass burning emissions except during winter when long‐distant sources become more important in the FT. BC in the FT is significantly affected by anthropogenic emissions from all parts of India. The source‐receptor relationship changes seasonally, but the regional transport remains a significant contributor to BC loadings in the LT of India, highlighting the necessity of considering nonlocal sources along with local emissions when designing strategies for mitigating BC impacts on air quality.