NanoMap : Geographical mapping of atmospheric new-particle formation through analysis of particle number size distribution and trajectory data

Particle number size distributions at various field sites are used to identify atmospheric new-particle formation (NPF) event days. However, the spatial distribution of regionally extensive events is unknown. To remedy this situation, the NanoMap method has been developed to enable the estimation of where NPF occurs within 500 km from any field station using as input size distribution and meteorological trajectories only. Also, the horizontal extension of NPF can be determined. An open-source program to run NanoMap is available on the internet. NanoMap has been developed using as an example the Finnish field site at Hyytiala. It shows that there are frequent NPF events over the Baltic Sea, but not as frequent as over Finland for certain wind directions; hence NanoMap is able to pinpoint areas with a low or high occurrence of NPF events. The method should be applicable to almost any field site.Peer reviewe

Coupling an aerosol box model with one-dimensional flow : a tool for understanding observations of new particle formation events

Field observations of new particle formation and the subsequent particle growth are typically only possible at a fixed measurement location, and hence do not follow the temporal evolution of an air parcel in a Lagrangian sense. Standard analysis for determining formation and growth rates requires that the time-dependent formation rate and growth rate of the particles are spatially invariant; air parcel advection means that the observed temporal evolution of the particle size distribution at a fixed measurement location may not represent the true evolution if there are spatial variations in the formation and growth rates. Here we present a zero-dimensional aerosol box model coupled with one-dimensional atmospheric flow to describe the impact of advection on the evolution of simulated new particle formation events. Wind speed, particle formation rates and growth rates are input parameters that can vary as a function of time and location, using wind speed to connect location to time. The output simulates measurements at a fixed location; formation and growth rates of the particle mode can then be calculated from the simulated observations at a stationary point for different scenarios and be compared with the 'true' input parameters. Hence, we can investigate how spatial variations in the formation and growth rates of new particles would appear in observations of particle number size distributions at a fixed measurement site. We show that the particle size distribution and growth rate at a fixed location is dependent on the formation and growth parameters upwind, even if local conditions do not vary. We also show that different input parameters used may result in very similar simulated measurements. Erroneous interpretation of observations in terms of particle formation and growth rates, and the time span and areal extent of new particle formation, is possible if the spatial effects are not accounted for.Peer reviewe

The Detection of Bacteria in the Maxillary Sinus Secretion of Patients With Acute Rhinosinusitis Using an Electronic Nose : A Pilot Study

Objective: Detecting bacteria as a causative pathogen of acute rhinosinusitis (ARS) is a challenging task. Electronic nose technology is a novel method for detecting volatile organic compounds (VOCs) that has also been studied in association with the detection of several diseases. The aim of this pilot study was to analyze maxillary sinus secretion with differential mobility spectrometry (DMS) and to determine whether the secretion demonstrates a different VOC profile when bacteria are present. Methods: Adult patients with ARS symptoms were examined. Maxillary sinus contents were aspirated for bacterial culture and DMS analysis. k-Nearest neighbor and linear discriminant analysis were used to classify samples as positive or negative, using bacterial cultures as a reference. Results: A total of 26 samples from 15 patients were obtained. After leave-one-out cross-validation, k-nearest neighbor produced accuracy of 85%, sensitivity of 67%, specificity of 94%, positive predictive value of 86%, and negative predictive value of 84%. Conclusions: The results of this pilot study suggest that bacterial positive and bacterial negative sinus secretion release different VOCs and that DMS has the potential to detect them. However, as the results are based on limited data, further conclusions cannot be made. DMS is a novel method in disease diagnostics and future studies should examine whether the method can detect bacterial ARS by analyzing exhaled air.publishedVersionPeer reviewe

Differentiation of aspirated nasal air from room air using analysis with a differential mobility spectrometry-based electronic nose : a proof-of-concept study

Over the last few decades, breath analysis using electronic nose (eNose) technology has become a topic of intense research, as it is both non-invasive and painless, and is suitable for point-of-care use. To date, however, only a few studies have examined nasal air. As the air in the oral cavity and the lungs differs from the air in the nasal cavity, it is unknown whether aspirated nasal air could be exploited with eNose technology. Compared to traditional eNoses, differential mobility spectrometry uses an alternating electrical field to discriminate the different molecules of gas mixtures, providing analogous information. This study reports the collection of nasal air by aspiration and the subsequent analysis of the collected air using a differential mobility spectrometer. We collected nasal air from ten volunteers into breath collecting bags and compared them to bags of room air and the air aspirated through the device. Distance and dissimilarity metrics between the sample types were calculated and statistical significance evaluated with Kolmogorov-Smirnov test. After leave-one-day-out cross-validation, a shrinkage linear discriminant classifier was able to correctly classify 100% of the samples. The nasal air differed (p < 0.05) from the other sample types. The results show the feasibility of collecting nasal air by aspiration and subsequent analysis using differential mobility spectrometry, and thus increases the potential of the method to be used in disease detection studies.acceptedVersionPeer reviewe

Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

We use observations of total particle number concentration at 36 worldwide sites and a global aerosol model to quantify the primary and secondary sources of particle number. We show that emissions of primary particles can reasonably reproduce the spatial pattern of observed condensation nuclei (CN) (R2=0.51) but fail to explain the observed seasonal cycle at many sites (R2=0.1). The modeled CN concentration in the free troposphere is biased low (normalised mean bias, NMB=&#8722;88%) unless a secondary source of particles is included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=&#8722;25%). Simulated CN concentrations in the continental boundary layer (BL) are also biased low (NMB=&#8722;74%) unless the number emission of anthropogenic primary particles is increased or an empirical BL particle formation mechanism based on sulfuric acid is used. We find that the seasonal CN cycle observed at continental BL sites is better simulated by including a BL particle formation mechanism (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). Using sensitivity tests we derive optimum rate coefficients for this nucleation mechanism, which agree with values derived from detailed case studies at individual sites

Global observations of aerosol-cloud-precipitation-climate interactions: Global observations of aerosol-cloud-precipitation-climateinteractions

Cloud drop condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and, consequently, cloud albedo and the dynamic response of clouds to aerosol-induced changes to precipitation. This can modify the reflected solar radiation and the thermal radiation emitted to space. Measurements of tropospheric CCN and IN over large areas have not been possible and can be only roughly approximated from satellite-sensor-based estimates of optical properties of aerosols. Our lack of ability to measure both CCN and cloud updrafts precludes disentangling the effects ofmeteorology fromthose of aerosols and represents the largest component in our uncertainty in anthropogenic climate forcing.Ways to improve the retrieval accuracy include multiangle and multipolarimetric passive measurements of the optical signal and multispectral lidar polarimetric measurements. Indirect methods include proxies of trace gases, as retrieved by hyperspectral sensors. Perhaps the most promising emerging direction is retrieving the CCN properties by simultaneously retrieving convective cloud drop number concentrations and updraft speeds, which amounts to using clouds as natural CCN chambers. These satellite observations have to be constrained by in situ observations of aerosol-cloud-precipitation-climate (ACPC) interactions, which in turn constrain a hierarchy of model simulations of ACPC. Since the essence of a general circulation model is an accurate quantification of the energy and mass fluxes in all forms between the surface, atmosphere and outer space, a route to progress is proposed here in the form of a series of box flux closure experiments in the various climate regimes. A roadmap is provided for quantifying the ACPC interactions and thereby reducing the uncertainty in anthropogenic climate forcing

Soot-doped natural snow and its albedo — results from field experiments

Soot has a pronounced effect on the cryosphere and experiments are still needed to reduce the associated uncertainties. This work presents a series of experiments to address this issue, with soot being deposited onto a natural snow surface after which the albedo changes were monitored. The albedo reduction was the most pronounced for the snow with higher soot content, and it was observed immediately following soot deposition. Compared with a previous laboratory study the effects of soot on the snow were not as prominent in outdoor conditions. During snowmelt, about 50% of the originally deposited soot particles were observed to remain at the snow surface. More detailed experiments are however needed to better explain soot's effect on snow and to better quantify this effect. Our albedo versus soot parameterization agreed relatively well with previously published relationships.Peer reviewe

Comparison of particle number size distribution trends in ground measurements and climate models

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol-cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability

Comparison of particle number size distribution trends in ground measurements and climate models

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol-cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.Peer reviewe