Longitudinal spin Seebeck coefficient: heat flux vs. temperature difference method

The determination of the longitudinal spin Seebeck effect (LSSE) coefficient is currently plagued by a large uncertainty due to the poor reproducibility of the experimental conditions used in its measurement. In this work we present a detailed analysis of two different methods used for the determination of the LSSE coefficient. We have performed LSSE experiments in different laboratories, by using different setups and employing both the temperature difference method and the heat flux method. We found that the lack of reproducibility can be mainly attributed to the thermal contact resistance between the sample and the thermal baths which generate the temperature gradient. Due to the variation of the thermal resistance, we found that the scaling of the LSSE voltage to the heat flux through the sample rather than to the temperature difference across the sample greatly reduces the uncertainty. The characteristics of a single YIG/Pt LSSE device obtained with two different setups was $(1.143\pm0.007)\cdot 10^{-7}$ Vm/W and $(1.101\pm0.015)\cdot 10^{-7}$ Vm/W with the heat flux method and $(2.313\pm0.017)\cdot 10^{-7}$ V/K and $(4.956\pm0.005)\cdot 10^{-7}$ V/K with the temperature difference method. This shows that systematic errors can be considerably reduced with the heat flux method.Comment: PDFLaTeX, 10 pages, 6 figure

A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols

This document is the Accepted Manuscript version of the following article: S. Vratolis, et al, ‘A new method to retrieve the real part of the equivalent refractive index of atmospheric aerosols’, Journal of Aerosol Science, Vol. 117: 54-62, March 2018. Under embargo until 29 December 2019. The final, published version is available online at DOI: https://doi.org/10.1016/j.jaerosci.2017.12.013.In the context of the international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD, 15 May to 22 June 2014), dry aerosol size distributions were measured at Demokritos station (DEM) using a Scanning Mobility Particle Sizer (SMPS) in the size range from 10 to 550 nm (electrical mobility diameter), and an Optical Particle Counter (OPC model Grimm 107 operating at the laser wavelength of 660 nm) to acquire the particle size distribution in the size range of 250 nm to 2.5 μm optical diameter. This work describes a method that was developed to align size distributions in the overlapping range of the SMPS and the OPC, thus allowing us to retrieve the real part of the aerosol equivalent refractive index (ERI). The objective is to show that size distribution data acquired at in situ measurement stations can provide an insight to the physical and chemical properties of aerosol particles, leading to better understanding of aerosol impact on human health and earth radiative balance. The resulting ERI could be used in radiative transfer models to assess aerosol forcing direct effect, as well as an index of aerosol chemical composition. To validate the method, a series of calibration experiments were performed using compounds with known refractive index (RI). This led to a corrected version of the ERI values, (ERICOR). The ERICOR values were subsequently compared to model estimates of RI values, based on measured PM2.5 chemical composition, and to aerosol RI retrieved values by inverted lidar measurements on selected days.Peer reviewe

Size-resolved CCN distributions and activation kinetics of aged continental and marine aerosol

We present size-segregated measurements of cloud condensation nucleus (CCN) activity of aged aerosol sampled at Finokalia, Crete, during the Finokalia Aerosol Measurement Experiment of summer 2007 (FAME07). From analysis of the data, hygroscopicity and activation kinetics distributions are derived. The CCN are found to be highly hygroscopic, (expressed by a size- and time- averaged hygroscopicity parameter κ ∼ 0.22), with the majority of particles activating at ~0.5–0.6 % supersaturation. Air masses originating from Central-Eastern Europe tend to be associated with higher CCN concentrations and slightly lower hygroscopicity (κ ∼ 0.18) than for other airmass types. The particles were always well mixed, as reflected by the high activation ratios and narrow hygroscopicity distribution widths. Smaller particles (~40 nm) were found to be more hygroscopic (~0.1κ units higher) than the larger ones (~100 nm). The particles with diameters less than 80 nm exhibited a diurnal hygroscopicity cycle (with κ peaking at ~14 h local time), consistent with photochemical aging and volatilization of less hygroscopic material from the aerosol. Use of bulk chemical composition and the aerosol number distribution results in excellent CCN closure when applying Köhler theory in its simplest form. Using asymptotic and threshold droplet growth analysis, the "aged" organics present in the aerosol were found not to suppress or delay the water uptake kinetics of particles in this environment

Regional new particle formation as modulators of cloud condensation nuclei and cloud droplet number in the eastern Mediterranean

A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN) are thought to originate from the condensational growth of new particle formation (NPF) from the gas phase. Here, 7 years of continuous aerosol and meteorological measurements (June 2008 to May 2015) at a remote background site of the eastern Mediterranean were recorded and analyzed to assess the impact of NPF (of 162 episodes identified) on CCN and cloud droplet number concentration (CDNC) formation in the region. A new metric is introduced to quantitatively determine the initiation and duration of the influence of NPF on the CCN spectrum. NPF days were found to increase CCN concentrations (from 0.10&thinsp;% to 1.00&thinsp;% supersaturation) between 29&thinsp;% and 77&thinsp;%. Enhanced CCN concentrations from NPF are mostly observed, as expected, under low preexisting particle concentrations and occur in the afternoon, relatively later in the winter and autumn than in the summer. Potential impacts of NPF on cloud formation were quantified by introducing the observed aerosol size distributions and chemical composition into an established cloud droplet parameterization. We find that the supersaturations that develop are very low (ranging between 0.03&thinsp;% and 0.27&thinsp;%) for typical boundary layer dynamics (σw ∼0.3&thinsp;m&thinsp;s−1) and NPF is found to enhance CDNC by a modest 13&thinsp;%. This considerable contrast between CCN and CDNC response is in part from the different supersaturation levels considered, but also because supersaturation drops from increasing CCN because of water vapor competition effects during the process of droplet formation. The low cloud supersaturation further delays the appearance of NPF impacts on CDNC to clouds formed in the late evening and nighttime – which has important implications for the extent and types of indirect effects induced by NPF events. An analysis based on CCN concentrations using prescribed supersaturation can provide very different, even misleading, conclusions and should therefore be avoided. The proposed approach here offers a simple, yet highly effective way for a more realistic impact assessment of NPF events on cloud formation.</p

Sources and processes that control the submicron organic aerosol composition in an urban Mediterranean environment (Athens): a high temporal-resolution chemical composition measurement study

Submicron aerosol chemical composition was studied during a year-long period (26 July 2016–31 July 2017) and two wintertime intensive campaigns (18 December 2013–21 February 2014 and 23 December 2015–17 February 2016), at a central site in Athens, Greece, using an Aerosol Chemical Speciation Monitor (ACSM). Concurrent measurements included a particle-into-liquid sampler (PILS-IC), a scanning mobility particle sizer (SMPS), an AE-33 Aethalometer, and ion chromatography analysis on 24 or 12&thinsp;h filter samples. The aim of the study was to characterize the seasonal variability of the main submicron aerosol constituents and decipher the sources of organic aerosol (OA). Organics were found to contribute almost half of the submicron mass, with 30&thinsp;min resolution concentrations during wintertime reaching up to 200&thinsp;µg&thinsp;m−3. During winter (all three campaigns combined), primary sources contributed about 33&thinsp;% of the organic fraction, and comprised biomass burning (10&thinsp;%), fossil fuel combustion (13&thinsp;%), and cooking (10&thinsp;%), while the remaining 67&thinsp;% was attributed to secondary aerosol. The semi-volatile component of the oxidized organic aerosol (SV-OOA; 22&thinsp;%) was found to be clearly linked to combustion sources, in particular biomass burning; part of the very oxidized, low-volatility component (LV-OOA; 44&thinsp;%) could also be attributed to the oxidation of emissions from these primary combustion sources. These results, based on the combined contribution of biomass burning organic aerosol (BBOA) and SV-OOA, indicate the importance of increased biomass burning in the urban environment of Athens as a result of the economic recession. During summer, when concentrations of fine aerosols are considerably lower, more than 80&thinsp;% of the organic fraction is attributed to secondary aerosol (SV-OOA 31&thinsp;% and LV-OOA 53&thinsp;%). In contrast to winter, SV-OOA appears to result from a well-mixed type of aerosol that is linked to fast photochemical processes and the oxidation of primary traffic and biogenic emissions. Finally, LV-OOA presents a more regional character in summer, owing to the oxidation of OA over the period of a few days.</p

Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

Aged organic aerosol (OA) was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008), which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS) was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM&lt;sub&gt;1&lt;/sub&gt;), and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM&lt;sub&gt;1&lt;/sub&gt; sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA) with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA) was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM&lt;sub&gt;1&lt;/sub&gt; such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4&amp;times;10&lt;sup&gt;11&lt;/sup&gt; molecules cm&lt;sup&gt;&amp;minus;3&lt;/sup&gt; s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source

The Finokalia Aerosol Measurement Experiment – 2008 (FAME-08): an overview

A month (4 May to 8 June 2008) of ambient aerosol, air ion and gas phase sampling (Finokalia Aerosol Measurement Experiment 2008, FAME-08) was conducted at Finokalia, on the island of Crete, Greece. The purpose of the study was to characterize the physical and chemical properties of aged aerosol and to investigate new particle formation. Measurements included aerosol and air ion size distributions, size-resolved chemical composition, organic aerosol thermal volatility, water uptake and particle optical properties (light scattering and absorption). Statistical analysis of the aerosol mass concentration variations revealed the absence of diurnal patterns suggesting the lack of strong local sources. Sulfates accounted for approximately half of the particulate matter less than 1 micrometer in diameter (PM&lt;sub&gt;1&lt;/sub&gt;) and organics for 28%. The PM&lt;sub&gt;1&lt;/sub&gt; organic aerosol fraction was highly oxidized with 80% water soluble. The supermicrometer particles were dominated by crustal components (50%), sea salt (24%) and nitrates (16%). The organic carbon to elemental carbon (OC/EC) ratio correlated with ozone measurements but with a one-day lag. The average OC/EC ratio for the study period was equal to 5.4. For three days air masses from North Africa resulted in a 6-fold increase of particulate matter less than 10 micrometers in diameter (PM&lt;sub&gt;10&lt;/sub&gt;) and a decrease of the OC/EC ratio by a factor of 2. Back trajectory analysis, based on FLEXPART footprint plots, identified five source regions (Athens, Greece, Africa, other continental and marine), each of which influenced the PM&lt;sub&gt;1&lt;/sub&gt; aerosol composition and properties. Marine air masses had the lowest PM&lt;sub&gt;1&lt;/sub&gt; concentrations and air masses from the Balkans, Turkey and Eastern Europe the highest

Atmospheric new particle formation as a source of CCN in the eastern Mediterranean marine boundary layer

While cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is thought to be frequent throughout the continental boundary layers, few studies on this phenomenon in marine air exist. Here, based on simultaneous measurement of particle number size distributions, CCN properties and aerosol chemical composition, we present the first direct evidence on CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles to CCN sizes in this environment during the summertime. Sub-100 nm particles were found to be substantially less hygroscopic than larger particles during the period with active NPF and growth (the value of kappa was lower by 0.2-0.4 for 60 nm particles compared with 120 nm particles), probably due to enrichment of organic material in the sub-100 nm size range. The aerosol hygroscopicity tended to be at minimum just before the noon and at maximum in the afternoon, which was very likely due to the higher sulfate-to-organic ratios and higher degree of oxidation of the organic material during the afternoon. Simultaneous with the formation of new particles during daytime, particles formed during the previous day or even earlier were growing into the size range relevant to cloud droplet activation, and the particles formed in the atmosphere were possibly mixed with long-range-transported particles.Peer reviewe

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

This is the final version of the article. Available from American Geophysical Union via the DOI in this record.A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.The data presented in the paper will be available through the Bolin Centre database (http://bolin.su.se/data/). The EC H2020 European Research Council ERC (ERC-StGATMOGAIN-278277 and ERC-StG-QAPPA-335478) and integrated project 641816 CRESCENDO Svenska Forskningsrådet Formas (Swedish Research Council Formas) (2015-749), Knut och Alice Wallenbergs Stiftelse (Knut and Alice Wallenberg Foundation Wallenberg Fellowship AtmoRemove), Academy of Finland (grants 272041 and 259005), Natural Environment Research Council (NERC grants NE/M003531/1 and NE/J02175X/1), Norwegian Research Council (EVA grant 229771), Natural Sciences and Engineering Research Council of Canada (NSERC, grant RGPIN/04315-2014), National Science Foundation (NSF, grants ATM-1242258, AGS-1242932, and AGS-1360834), U.S. Environmental Protection Agency (EPA, STAR grant R835410), National Oceanic and Atmospheric Administration (NOAA, CPO award 538NA10OAR4310102), Electric Power Research Institute (EPRI, grant 10004734), U.S. Department of Energy (DOE, grants BER/ASR DE-SC0016559 and DE-SC0012792), Georgia Institute of Technology, and NordForsk (Nordic Centre of Excellence eSTICC) are gratefully acknowledged for funding. The climate model simulations were performed on resources provided by the Swedish National Infrastructure for Computing (SNIC) at the National Supercomputing Centre. Benjamin Murphy is acknowledged for useful discussions

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources. Plain Language Summary The interaction of airborne particulate matter ("aerosols") with water is of critical importance for processes governing climate, precipitation, and public health. It also modulates the delivery and bioavailability of nutrients to terrestrial and oceanic ecosystems. We present a microphysical explanation to the humidity-dependent water uptake behavior of organic aerosol, which challenges the highly simplified theoretical descriptions used in, e.g., present climate models. With the comprehensive analysis of laboratory data using molecular models, we explain the microphysical behavior of the aerosol over the range of humidity observed in the atmosphere, in a way that has never been done before. We also demonstrate the presence of these phenomena in the ambient atmosphere from data collected in the field. We further show, using two state-of-the-art climate models, that misrepresenting the water affinity of atmospheric organic aerosol can lead to significant biases in the estimates of the anthropogenic influence on climate.Peer reviewe