Sachin S Gunthe

This study provides baseline information about indoor-outdoor PM concentrations, size-resolved bioaerosol concentration, size distribution and diversity, I/O ratios of PM and bioaerosol, indoor bioaerosol emissions for five locations such as laboratory, students’ office, air-conditioned room, eatery, and residence. While most of the indoor air quality studies reported so far emphasized on a distinct type of indoor environment at a time, this study provides a first-hand account about PM and bioaerosols simultaneously measured and compared from diverse yet commonly encountered indoor locations of southern Indian region. PM2.5 and PM10 was found to have similar concentration distributions at all locations. Elevated cooking activity and human induced floor resuspensions led to the highest indoor-outdoor number concentration of PM at eatery. The I/O mass concentration ratios indicated the influence of outdoor PM on indoor environment of laboratory. Presence of distinct sources that contributed to significant PM mass variations at indoor and outdoor environments were substantiated with ANOVA and chi-square test results. Human occupancy and potted plants was found contributing to the elevated indoor bacterial concentrations (>800 CFU m−3). Fine to coarse bioaerosol fractions implied the abundant presence of coarse mode bacteria and fungi amounting to >80% of total cultivable bioaerosol load across all locations. Bacilli and Gammaproteobacteria dominated the bacterial aerosols while Cladosporium and Aspergillus dominated the fungal aerosols. Fungi contributed highest to the mass fraction of PM10 in comparison to bacteria, both indoor and outdoor. Highest bacterial emission rates were observed at air-conditioned room (4.85 × 105 CFU/h/person) and fungal emissions at laboratory (4.60 × 105 CFU/h/person).

Size-resolved measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted over a full seasonal cycle at the remote Amazon Tall Tower Observatory (ATTO, March 2014-February 2015). In a preceding companion paper, we presented annually and seasonally averaged data and parametrizations (Part 1; Pöhlker et al., 2016a). In the present study (Part 2), we analyze key features and implications of aerosol and CCN properties for the following characteristic atmospheric conditions: Empirically pristine rain forest (PR) conditions, where no influence of pollution was detectable, as observed during parts of the wet season from March to May. The PR episodes are characterized by a bimodal aerosol size distribution (strong Aitken mode with DAit ≈ 70nm and NAit ≈ 160cm-3, weak accumulation mode with Dacc ≈ 160nm and Nacc ≈ 90cm-3), a chemical composition dominated by organic compounds, and relatively low particle hygroscopicity (ΚAit ≈ 0.12, Κacc ≈ 0.18). Long-range-transport (LRT) events, which frequently bring Saharan dust, African biomass smoke, and sea spray aerosols into the Amazon Basin, mostly during February to April. The LRT episodes are characterized by a dominant accumulation mode (DAit ≈ 80nm, NAit ≈ 120cm-3 vs. Dacc ≈ 180nm, Nacc ≈ 310cm-3), an increased abundance of dust and salt, and relatively high hygroscopicity (ΚAit ≈ 0.18, Κacc ≈ 0.35). The coarse mode is also significantly enhanced during these events. Biomass burning (BB) conditions characteristic for the Amazonian dry season from August to November. The BB episodes show a very strong accumulation mode (DAit ≈ 70nm, NAit ≈ 140cm-3 vs. Dacc ≈ 170nm, Nacc ≈ 3400cm-3), very high organic mass fractions (∼ 90%), and correspondingly low hygroscopicity (ΚAit ≈ 0.14, Κacc ≈ 0.17). Mixed-pollution (MPOL) conditions with a superposition of African and Amazonian aerosol emissions during the dry season. During the MPOL episode presented here as a case study, we observed African aerosols with a broad monomodal distribution (D ≈ 130nm, NCN, 10 ≈ 1300cm-3), with high sulfate mass fractions (∼ 20%) from volcanic sources and correspondingly high hygroscopicity (Κ < 100 nm ≈ 0.14, Κ > 100 nm ≈ 0.22), which were periodically mixed with fresh smoke from nearby fires (D ≈ 110nm, NCN, 10 ≈ 2800cm-3) with an organic-dominated composition and sharply decreased hygroscopicity (Κ < 150 nm ≈ 0.10, Κ > 150 nm ≈ 0.20). Insights into the aerosol mixing state are provided by particle hygroscopicity (Κ) distribution plots, which indicate largely internal mixing for the PR aerosols (narrow Κ distribution) and more external mixing for the BB, LRT, and MPOL aerosols (broad Κ distributions). The CCN spectra (CCN concentration plotted against water vapor supersaturation) obtained for the different case studies indicate distinctly different regimes of cloud formation and microphysics depending on aerosol properties and meteorological conditions. The measurement results suggest that CCN activation and droplet formation in convective clouds are mostly aerosol-limited under PR and LRT conditions and updraft-limited under BB and MPOL conditions. Normalized CCN efficiency spectra (CCN divided by aerosol number concentration plotted against water vapor supersaturation) and corresponding parameterizations (Gaussian error function fits) provide a basis for further analysis and model studies of aerosol-cloud interactions in the Amazon. .

Macrofungi have long been investigated for various scientific purposes including their food and medicinal characteristics. Their role in aerobiology as a fraction of the primary biological aerosol particles (PBAPs), however, has been poorly studied. In this study, we present a source of macrofungi with two different but interdependent objectives: (i) to characterize the macrofungi from a tropical dry evergreen biome in southern India using advanced molecular techniques to enrich the database from this region, and (ii) to assess whether identified species of macrofungi are a potential source of atmospheric PBAPs. From the DNA analysis, we report the diversity of the terrestrial macrofungi from a tropical dry evergreen biome robustly supported by the statistical analyses for diversity conclusions. A total of 113 macrofungal species belonging to 54 genera and 23 families were recorded, with Basidiomycota and Ascomycota constituting 96% and 4% of the species, respectively. The highest species richness was found in the family Agaricaceae (25.3%) followed by Polyporaceae (15.3%) and Marasmiaceae (10.8%). The difference in the distribution of commonly observed macrofungal families over this location was compared with other locations in India (Karnataka, Kerala, Maharashtra, and West Bengal) using two statistical tests. The distributions of the terrestrial macrofungi were distinctly different in each ecosystem. We further attempted to demonstrate the potential role of terrestrial macrofungi as a source of PBAPs in ambient air. In our opinion, the findings from this ecosystem of India will enhance our understanding of the distribution, diversity, ecology, and biological prospects of terrestrial macrofungi as well as their potential to contribute to airborne fungal aerosols.

An ultraviolet aerodynamic particle sizer (UV-APS) was continuously operated for the first time during two seasons to sample the contrasting winds during monsoon and winter to characterize the properties of fluorescent biological aerosol particles (FBAPs), at a high-Altitude site in India. Averaged over the entire monsoon campaign (1 June-21 August 2014), the arithmetic mean number and mass concentrations of coarse-mode (>ĝ€1ĝ€μm) FBAPs were 0.02ĝ€cmĝ'3 and 0.24ĝ€μgĝ€mĝ'3, respectively, which corresponded to ĝ1/4 ĝ€2 and 6ĝ€% of total aerosol loading, respectively. Average FBAP number size distribution exhibited a peak at ĝ1/4 ĝ€3ĝ€μm, which is attributed to the fungal spores, as supported by scanning electron microscope (SEM) images, and these results are consistent with previous studies made for FBAPs. During 11 weeks of measurements the variability of the total coarse-mode particle number (TAP) concentration was high compared to that observed in FBAP number concentrations. The TAP and FBAP number concentrations measured at this site were strongly dependent on changes in wind direction and rainfall. During periods of westerly/southwesterly winds with heavy persistent rainfall, the TAP and FBAP concentrations exhibited very low values (1.3 and 0.005ĝ€cmĝ'3, respectively) with no significant diurnal variations, whereas during periods of northerly winds with scattered rainfall FBAPs exhibited relatively high concentration values (0.05ĝ€cmĝ'3) with pronounced diurnal variations, which were strongly coupled with diurnal variations in meteorological parameters. The campaign-Averaged FBAP number concentrations were shown to correlate with daily patterns of meteorological parameters and were positively correlated with relative humidity (RH; R2ĝ€ Combining double low line ĝ€0.58) and negatively with temperature (R2ĝ€ Combining double low line ĝ€0.60) and wind speed (R2ĝ€ Combining double low line ĝ€0.60). We did not observe any significant positive correlation with precipitation as reported by previous researchers from selected areas. These measurement results confirm the fact that the ratio of PBAPs to TAP is strongly dependent on particle size and location and thus may constitute a significant proportion of total aerosol particles.

We evaluate numerical simulations of surface ozone mixing ratios over the south Asian region during the pre-monsoon season, employing three different emission inventories in the Weather Research and Forecasting model with Chemistry (WRF-Chem) with the second-generation Regional Acid Deposition Model (RADM2) chemical mechanism: the Emissions Database for Global Atmospheric Research - Hemispheric Transport of Air Pollution (EDGAR-HTAP), the Intercontinental Chemical Transport Experiment phase B (INTEX-B) and the Southeast Asia Composition, Cloud, Climate Coupling Regional Study (SEAC4RS). Evaluation of diurnal variability in modelled ozone compared to observational data from 15 monitoring stations across south Asia shows the model ability to reproduce the clean, rural and polluted urban conditions over this region. In contrast to the diurnal average, the modelled ozone mixing ratios during noontime, i.e. hours of intense photochemistry (11:30-16:30gIST - Indian Standard Time - UTC +5:30), are found to differ among the three inventories. This suggests that evaluations of the modelled ozone limited to 24gh average are insufficient to assess uncertainties associated with ozone buildup. HTAP generally shows 10-30gppbv higher noontime ozone mixing ratios than SEAC4RS and INTEX-B, especially over the north-west Indo-Gangetic Plain (IGP), central India and southern India. The HTAP simulation repeated with the alternative Model for Ozone and Related Chemical Tracers (MOZART) chemical mechanism showed even more strongly enhanced surface ozone mixing ratios due to vertical mixing of enhanced ozone that has been produced aloft. Our study indicates the need to also evaluate the O3 precursors across a network of stations and the development of high-resolution regional inventories for the anthropogenic emissions over south Asia accounting for year-to-year changes to further reduce uncertainties in modelled ozone over this region.

Bioaerosols abundantly found in the atmosphere can potentially influence the climate by acting as ice nuclei and thus profoundly influencing the hydrological cycle. As the first attempt over India, we report the diversity, abundance, and ice nucleating ability of bacteria present in the rainwater collected at Chennai, during summer and two contrasting monsoon seasons. Diverse bacterial communities were present in all the twenty rainwater samples and predominantly belonged to Actinobacteria (6%), Alpha proteobacter (9%), Bacilli (29%), Betaproterobacteria (14%), Flavobacteria (3%), and Gammaproteobacteria (39%). The most efficient ice nucleating bacteria such as Pseudomonas sp. and Pantoea sp. were present in our precipitation samples and they contributed to 8.4% and 9.4% of the total cultivable bacterial species obtained. The relative abundance of Pseudomonas was highest during the south-west monsoon (75%) whereas Pantoea was abundant in the north-east monsoon (51.8%). The dominant bacteria belonging to the known ice nucleating genera Pseudomonas, Pantoea, and Bacillus were chosen for the determination of their freezing temperatures using tube freeze assay technique. The onset freezing temperature of species belonging to Pseudomonas and Pantoea was recorded as −12 °C and for those species belonging to Bacillus it was found to be −14 °C. Further, the number of bacterial cells making up an ice nucleus was estimated at the temperatures ranging from −18 °C to −12 °C for all the ice nucleating bacteria and it was found to vary from 106 to 109 (cells/nucleus).

Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.

Fungal spores play important role in the health of humans, animals, and plants by constituting a class of the primary biological aerosol particles (PBAPs). Additionally, these could mediate the hydrological cycle by acting as nuclei for ice and cloud formation (IN and CCN respectively). Various processes in the biosphere and the variations in the meteorological conditions control the releasing mechanism of spores through active wet and dry discharge. In the present paper, we simulate the concentration of fungal spores over the Indian region during three distinct meteorological seasons by combining a numerical model (WRF-Chem) with the fungal spore emissions based on land-use type. Maiden high-resolution regional simulations revealed large spatial gradient and strong seasonal dependence in the concentration of fungal spores over the Indian region. The fungal spore concentrations are found to be the highest during winter (0-70 μg m-3 in December), moderately higher during summer (0-35 μg m-3 in May) and lowest during the monsoon (0-25 μg m-3 in July). The elevated concentrations during winter are attributed to the shallower boundary layer trapping the emitted fungal spores in smaller volume. In contrast, the deeper boundary layer mixing in May and stronger monsoonal-convection in July distribute the fungal spores throughout the lower troposphere (~5 km). We suggest that the higher fungal spore concentrations during winter could have potential health impacts. While, stronger vertical mixing could enable fungal spores to influence the cloud formation during summer and monsoon. Our study provides the first information about the distribution and seasonal variation of fungal spores over the densely populated and observationally sparse Indian region.

The relationship between surface-level observations of daily maxima in ozone (O3max) volume mixing ratio and ambient air temperature (Tmax) has been studied at an urban site, i.e. Pune (18.4°N, 73.8°E), India during 2003-04. The mixing ratios of O3max were found to be highest during winter to pre-monsoon period and lowest in the monsoon season. The dependence of O3max levels on Tmax has been quantified using the linear regression fit for the different seasons. However, except for the monsoon season, reasonably good correlations between O3max and Tmax were noticed. The correlation between daily O3max concentration and minimum NOx (NOxmin) concentration was also studied to assess the importance of photochemical mechanism mainly reduction in the loss due to titration. Overall, the strong dependencies of O3max on Tmax and NOxmin signify the role of both meteorological and photochemical processes during most months of a year. The positive slopes of ΔO3max/ΔTmax and ΔO3max/ΔNOxmin clearly indicate the role of significant production and accumulation of O3 under high temperature and low NOx conditions respectively, during winter and premonsoon seasons. The statistical analysis of O3 in relation with the key meteorological and chemical parameters is important to understand the sensitivity of secondary pollutants on various controlling factors.

Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations - exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol-cloud interactions in various environments.