Variability and linkages of aerosol properties between sub-urban and high altitude environments in Northern India

Atmospheric aerosol particles are linked to visibility reduction and adverse health effects, and radiation balance of the Earth— directly by reflecting and absorbing solar radiation and indirectly by influencing the cloud properties and processes and, possi-bly, by changing the heterogeneous chemistry of reactive gaseous species. Atmospheric aerosols are the most uncertain driver of global climate change. The South‒Asian region has been increasingly recognized as one of the global hotspots of aerosols; and Indo Gangetic Plains (IGP) is one among them with complex geography, heterogeneity in sources and varying atmospheric dynamics. These factors make IGP’s aerosol and pollution very difficult to characterize. So far, long-term regional observations of aerosol properties have been scarce in this region, but argued necessary in order to bring the knowledge of regional and global distribution of aerosols further. In this context, regional studies of aerosol properties their dynamics and atmospheric processes are very important areas of investigation to better estimate the climatic importance of submicron aerosol particles. Moreover regional studies over IGP-Himalayas domain are inevitable to know how trans-Himalayan valleys are acting as conduits for aerosol and pollution transport from the plains to the Himalayas. Therefore, in this thesis we studied these issues by applying basic to state-of-the-art instrumentation in two different envi-ronments, plains—Gual Pahari, and Himalayan foothills— Mukteshwar; to obtain physical and optical properties of submi-cron particles. Additionally, we used meteorological parameters, emissions and process modelling to determine local and region-al scale transport of atmospheric aerosols. The work carried out as part of the thesis infers four main conclusions, 1) Simultaneous long-term measurements at both the environments in Northern India region are useful to establish linkages between sub-urban environment and high altitude sites. One site represents a source region, while another characterize as a receiver site of atmospheric pollutants; 2) A distinct cycle of aerosol properties, both seasonal and diurnal, is present and provides information of driving factors of aerosol variability at both the sites; 3) The contribution of regional sources seem to dominate over the local /sub-urban sources, in the IGP region bounda-ry layer; 4) Aerosol properties and specific humidity “passive tracer” based analysis clearly reveal that the mountainous terrain sites are under the influence of air from the plains due to convective transport processes enhanced by local and mesoscale topography. The results presented in this thesis are particularly useful, first, when examining the linkages of aerosol properties variability between two different environments. The second, in determining for instance local versus regional influences, and pollutants reaching high altitude sites which can be explained by boundary layer dynamics processes, especially in the mountain terrain where the modelled mixing layer depths have uncertainties. This work outlines future direction of multi-points measurements on vertical profile of atmospheric particles and local boundary layer over mountainous terrain where the atmospheric structure becomes much more complicated. Additionally, investigations including isotope-based analysis and modelling work over the Himalayan region are desirable to be able to describe better the transport of atmospheric aerosols from IGP to high altitudes and further up to Himalayan ice-pack and glaciers where aerosol deposition could have serious environmental impacts

Light-absorption of dust and elemental carbon in snow in the Indian Himalayas and the Finnish Arctic

Light-absorbing impurities (LAIs) deposited in snow have the potential to substantially affect the snow radiation budget, with subsequent implications for snow melt. To more accurately quantify the snow albedo, the contribution from different LAIs needs to be assessed. Here we estimate the main LAI components, elemental carbon (EC) (as a proxy for black carbon) and mineral dust in snow from the Indian Himalayas and paired the results with snow samples from Arctic Finland. The impurities are collected onto quartz filters and are analyzed thermal-optically for EC, as well as with an additional optical measurement to estimate the light-absorption of dust separately on the filters. Laboratory tests were conducted using substrates containing soot and mineral particles, especially prepared to test the experimental setup. Analyzed ambient snow samples show EC concentrations that are in the same range as presented by previous research, for each respective region. In terms of the mass absorption cross section (MAC) our ambient EC surprisingly had about half of the MAC value compared to our laboratory standard EC (chimney soot), suggesting a less light absorptive EC in the snow, which has consequences for the snow albedo reduction caused by EC. In the Himalayan samples, larger contributions by dust (in the range of 50% or greater for the light absorption caused by the LAI) highlighted the importance of dust acting as a light absorber in the snow. Moreover, EC concentrations in the Indian samples, acquired from a 120 cm deep snow pit (possibly covering the last five years of snow fall), suggest an increase in both EC and dust deposition. This work emphasizes the complexity in determining the snow albedo, showing that LAI concentrations alone might not be sufficient, but additional transient effects on the light-absorbing properties of the EC need to be considered and studied in the snow. Equally as imperative is the confirmation of the spatial and temporal representativeness of these data by comparing data from several and deeper pits explored at the same time.Peer reviewe

Exhaust particle number and composition for diesel and gasoline passenger cars under transient driving conditions : Real-world emissions down to 1.5 nm

Recent recommendations given by WHO include systematic measurements of ambient particle number concentration and black carbon (BC) concentrations. In India and several other highly polluted areas, the air quality problems are severe and the need for air quality related information is urgent. This study focuses on particle number emissions and BC emissions of passenger cars that are technologically relevant from an Indian perspective. Particle number and BC were investigated under real-world conditions for driving cycles typical for Indian urban environments. Two mobile laboratories and advanced aerosol and trace gas instrumentation were utilized. Our study shows that passenger cars without exhaust particle filtration can emit in real-world conditions large number of particles, and especially at deceleration a significant fraction of particle number can be even in 1.5–10 nm particle sizes. The mass concentration of exhaust plume particles was dominated by BC that was emitted especially at acceleration conditions. However, exhaust particles contained also organic compounds, indicating the roles of engine oil and fuel in exhaust particle formation. In general, our study was motivated by serious Indian air quality problems, by the recognized lack of emission information related to Indian traffic, and by the recent WHO air quality guidance; our results emphasize the importance of monitoring particle number concentrations and BC also in Indian urban areas and especially in traffic environments where people can be significantly exposed to fresh exhaust emissions.Peer reviewe

Nitrogen Challenges and Opportunities for Agricultural and Environmental Science in India

In the last six decades, the consumption of reactive nitrogen (Nr) in the form of fertilizer in India has been growing rapidly, whilst the nitrogen use efficiency (NUE) of cropping systems has been decreasing. These trends have led to increasing environmental losses of Nr, threatening the quality of air, soils, and fresh waters, and thereby endangering climate-stability, ecosystems, and human-health. Since it has been suggested that the fertilizer consumption of India may double by 2050, there is an urgent need for scientific research to support better nitrogen management in Indian agriculture. In order to share knowledge and to develop a joint vision, experts from the UK and India came together for a conference and workshop on “Challenges and Opportunities for Agricultural Nitrogen Science in India.” The meeting concluded with three core messages: (1) Soil stewardship is essential and legumes need to be planted in rotation with cereals to increase nitrogen fixation in areas of limited Nr availability. Synthetic symbioses and plastidic nitrogen fixation are possibly disruptive technologies, but their potential and implications must be considered. (2) Genetic diversity of crops and new technologies need to be shared and exploited to reduce N losses and support productive, sustainable agriculture livelihoods. (3) The use of leaf color sensing shows great potential to reduce nitrogen fertilizer use (by 10–15%). This, together with the usage of urease inhibitors in neem-coated urea, and better management of manure, urine, and crop residues, could result in a 20–25% improvement in NUE of India by 2030

An Improved Version of the Prewhitening Method for Trend Analysis in the Autocorrelated Time Series

Nonparametric trend detection tests like the Mann–Kendall (MK) test require independent observations, but serial autocorrelation in the datasets inflates/deflates the variance and alters the Type-I and Type-II errors. Prewhitening (PW) techniques help address this issue by removing autocorrelation prior to applying MK. We evaluate several PW schemes—von Storch (PW-S), Slope-corrected PW (PW-Cor), trend-free prewhitening (TFPW) proposed by Yue (TFPW-Y), iterative TFPW (TFPW-WS), variance-corrected TFPW (VCTFPW), and newly proposed detrended prewhitened with modified trend added (DPWMT). Through Monte Carlo simulations, we constructed a lag-1 autoregressive (AR(1)) time series and systematically assessed the performance of different PW methods relative to sample size, autocorrelation, and trend slope. Results indicate that all methods tend to overestimate weak trends in small samples (n < 40). For moderate/high trends, the slopes estimated from the VCTFPW and DPWMT series close (within a ± 20% range) to the actual trend. VCTFPW shows slightly lower RMSE than DPWMT at mid-range lag-1 autocorrelation (ρ1 = 0.3 to 0.6) but fluctuates for ρ1 ≥ 0.7. Original series and TFPW-Y fail to control Type-I error with increasing ρ1, while VCTFPW and DPWMT maintained Type-I errors below the significance level (α = 0.05) for large samples. Apart from TFPW-Y, all PW methods resulted in weak power of the test for weak trends and small samples. TFPW-WS showed high power of the test but only for strong autocorrelated data combined with strong trends. In contrast, VCTFPW failed to preserve the power of the test at high autocorrelation (≥0.7) due to slope underestimation. DPWMT restores the power of the test for 0.1 ≤ ρ1 ≤ 0.9 for moderate/strong trends. Overall, the proposed DPWMT approach demonstrates clear advantages, providing unbiased slope estimates, reasonable Type-I error control, and sufficient power in detecting linear trends in the AR(1) series

Assessment of carbonaceous aerosols at Mukteshwar: A high-altitude (~2200 m amsl) background site in the foothills of the Central Himalayas

The present study examined the equivalent black carbon (eBC) mass concentrations measured over 10.5 years (September 2005–March 2016) using a 7-wavelength Aethalometer (AE-31) at Mukteshwar, a high-altitude and regional background site in the foothills of Indian central Himalayas. The total spectral absorption coefficient (babs) was divided into three categories: black carbon (BC) and brown carbon (BrC); fossil fuels (FF) and wood/biomass burning (WB/BB); and primary and secondary sources. At the wavelength of 370 nm, a significant BrC contribution (25 %) to the total babs is identified, characterized by a pronounced seasonal variation with winter (December–January-February) maxima (31 %) and post-monsoon (October and November) minima (20 %); whereas, at 660 nm, the contribution of BrC is dramatically less (9 %). Climatologically, the estimated BCFF at 880 nm ranges from 0.25 ± 0.19 μg m−3 in July to 1.17 ± 0.80 μg m−3 in May with the annual average of 0.67 ± 0.63 μg m−3, accounting for 79 % of the BC mass. The maximum BCFF/BC fraction reaches its peak value during the monsoon (July and August, 85 %), indicating the dominance of local traffic emissions due to tourism activities. Further, the highest BCWB concentration observed during pre-monsoon (March–May) suggests the influence of local forest fires along with long-range transported aerosols from the low-altitude plains. The increased contribution of BrC (26 % at 370 nm) and WB absorption (61 % at 370 nm) to the total absorption at the shorter wavelengths suggests that wood burning is one of the major sources of BrC emissions. Secondary BrC absorption accounts for 24 % [91 %] of the total absorption [BrC absorption] at 370 nm, implying the dominance of secondary sources in BrC formation. A trend analysis for the measured BC concentration shows a statistically significant increasing trend with a slope of 0.02 μgm−3/year with a total increase of about 22 % over the study period. A back trajectory-based receptor model, potential source contribution function (PSCF), was used to identify the potential regional source region of BC. The main source regions of BC are the northwest states of India in the IGP region and the northeast Pakistan region

Chemical Composition and Source Apportionment of Total Suspended Particulate in the Central Himalayan Region

The present study analyzes data from total suspended particulate (TSP) samples collected during 3 years (2005–2008) at Nainital, central Himalayas, India and analyzed for carbonaceous aerosols (organic carbon (OC) and elemental carbon (EC)) and inorganic species, focusing on the assessment of primary and secondary organic carbon contributions (POC, SOC, respectively) and on source apportionment by positive matrix factorization (PMF). An average TSP concentration of 69.6 ± 51.8 µg m−3 was found, exhibiting a pre-monsoon (March–May) maximum (92.9 ± 48.5 µg m−3) due to dust transport and forest fires and a monsoon (June–August) minimum due to atmospheric washout, while carbonaceous aerosols and inorganic species expressed a similar seasonality. The mean OC/EC ratio (8.0 ± 3.3) and the good correlations between OC, EC, and nss-K+ suggested that biomass burning (BB) was one of the major contributing factors to aerosols in Nainital. Using the EC tracer method, along with several approaches for the determination of the (OC/EC)pri ratio, the estimated SOC component accounted for ~25% (19.3–29.7%). Furthermore, TSP source apportionment via PMF allowed for a better understanding of the aerosol sources in the Central Himalayan region. The key aerosol sources over Nainital were BB (27%), secondary sulfate (20%), secondary nitrate (9%), mineral dust (34%), and long-range transported mixed marine aerosol (10%). The potential source contribution function (PSCF) and concentration weighted trajectory (CWT) analyses were also used to identify the probable regional source areas of resolved aerosol sources. The main source regions for aerosols in Nainital were the plains in northwest India and Pakistan, polluted cities like Delhi, the Thar Desert, and the Arabian Sea area. The outcomes of the present study are expected to elucidate the atmospheric chemistry, emission source origins, and transport pathways of aerosols over the central Himalayan region

Chemical Composition and Source Apportionment of Total Suspended Particulate in the Central Himalayan Region

The present study analyzes data from total suspended particulate (TSP) samples collected during 3 years (2005–2008) at Nainital, central Himalayas, India and analyzed for carbonaceous aerosols (organic carbon (OC) and elemental carbon (EC)) and inorganic species, focusing on the assessment of primary and secondary organic carbon contributions (POC, SOC, respectively) and on source apportionment by positive matrix factorization (PMF). An average TSP concentration of 69.6 ± 51.8 µg m−3 was found, exhibiting a pre-monsoon (March–May) maximum (92.9 ± 48.5 µg m−3) due to dust transport and forest fires and a monsoon (June–August) minimum due to atmospheric washout, while carbonaceous aerosols and inorganic species expressed a similar seasonality. The mean OC/EC ratio (8.0 ± 3.3) and the good correlations between OC, EC, and nss-K+ suggested that biomass burning (BB) was one of the major contributing factors to aerosols in Nainital. Using the EC tracer method, along with several approaches for the determination of the (OC/EC)pri ratio, the estimated SOC component accounted for ~25% (19.3–29.7%). Furthermore, TSP source apportionment via PMF allowed for a better understanding of the aerosol sources in the Central Himalayan region. The key aerosol sources over Nainital were BB (27%), secondary sulfate (20%), secondary nitrate (9%), mineral dust (34%), and long-range transported mixed marine aerosol (10%). The potential source contribution function (PSCF) and concentration weighted trajectory (CWT) analyses were also used to identify the probable regional source areas of resolved aerosol sources. The main source regions for aerosols in Nainital were the plains in northwest India and Pakistan, polluted cities like Delhi, the Thar Desert, and the Arabian Sea area. The outcomes of the present study are expected to elucidate the atmospheric chemistry, emission source origins, and transport pathways of aerosols over the central Himalayan region.</jats:p