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Lee J.H.,State University of New York at Stony Brook | McDonnell K.T.,Dowling College | Zelenyuk A.,Pacific Northwest National Laboratory | Imre D.,Imre Consulting | Mueller K.,State University of New York at Stony Brook
IEEE Transactions on Visualization and Computer Graphics | Year: 2014

Although the euclidean distance does well in measuring data distances within high-dimensional clusters, it does poorly when it comes to gauging intercluster distances. This significantly impacts the quality of global, low-dimensional space embedding procedures such as the popular multidimensional scaling (MDS) where one can often observe nonintuitive layouts. We were inspired by the perceptual processes evoked in the method of parallel coordinates which enables users to visually aggregate the data by the patterns the polylines exhibit across the dimension axes. We call the path of such a polyline its structure and suggest a metric that captures this structure directly in high-dimensional space. This allows us to better gauge the distances of spatially distant data constellations and so achieve data aggregations in MDS plots that are more cognizant of existing high-dimensional structure similarities. Our biscale framework distinguishes far-distances from near-distances. The coarser scale uses the structural similarity metric to separate data aggregates obtained by prior classification or clustering, while the finer scale employs the appropriate euclidean distance. © 2014 IEEE.

Earle M.E.,Environment Canada | Liu P.S.K.,Environment Canada | Strapp J.W.,Environment Canada | Zelenyuk A.,Pacific Northwest National Laboratory | And 4 more authors.
Journal of Geophysical Research: Atmospheres | Year: 2011

Aircraft measurements during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in April 2008 are used to investigate factors influencing the microphysics and radiative properties of springtime Arctic clouds. The analysis is focused on low-level, liquid-dominated clouds in two separate regimes with respect to cloud and aerosol properties: single-layer stratocumulus with below-cloud aerosol concentrations (Na) less than 250 cm-3 (clean cases); and layered stratocumulus with Na > 500 cm -3 below cloud base, associated with a biomass burning aerosol (polluted cases). For each regime, vertical profiles through cloud are used to determine cloud microphysical and radiative properties. The polluted cases were correlated with warmer, geometrically thicker clouds, with higher droplet number concentrations (Nd), liquid water paths (LWP), optical depths and albedo (A) relative to clean cases. The mean cloud droplet effective radii (reff), however, were similar (μ5.7 m) for both aerosol-cloud regimes. This discrepancy resulted mainly from the higher LWP of clouds in polluted cases, which can be explained by both meteorological (temperature, dynamics) and microphysical (precipitation inhibition) factors. Adiabatic parcel model simulations demonstrate that differences in droplet activation between the aerosol-cloud regimes may play a role, as the higher Na in polluted cases limits activation to larger and/or more hygroscopic particles. The observations and analysis presented here demonstrate the complex interactions among environmental conditions, aerosol, and the microphysics and radiative properties of Arctic clouds. Copyright 2011 by the American Geophysical Union.

Abramson E.,University of Washington | Imre D.,Imre Consulting | Beranek J.,Pacific Northwest National Laboratory | Wilson J.,Pacific Northwest National Laboratory | Zelenyuk A.,Pacific Northwest National Laboratory
Physical Chemistry Chemical Physics | Year: 2013

Formation, properties, transformations, and temporal evolution of secondary organic aerosol (SOA) particles depend strongly on SOA phase. Recent experimental evidence from both our group and several others indicates that, in contrast to common models' assumptions, SOA constituents do not form a low-viscosity, well-mixed solution, yielding instead a semisolid phase with high, but undetermined, viscosity. We find that when SOA particles are made in the presence of vapors of semi-volatile hydrophobic compounds, such molecules become trapped in the particles' interiors and their subsequent evaporation rates and thus their rates of diffusion through the SOA can be directly obtained. Using pyrene as the tracer molecule and SOA derived from α-pinene ozonolysis, we find that it takes ∼24 hours for half the pyrene to evaporate. Based on the observed pyrene evaporation kinetics we estimate a diffusivity of 2.5 × 10-21 m2 s -1 for pyrene in SOA. Similar measurements on SOA doped with fluoranthene and phenanthrene yield diffusivities comparable to that of pyrene. Assuming a Stokes-Einstein relation, an approximate viscosity of 108 Pa s can be calculated for this SOA. Such a high viscosity is characteristic of tars and is consistent with published measurements of SOA particle bounce, evaporation kinetics, and the stability of two reverse-layered morphologies. We show that a viscosity of 108 Pa s implies coalescence times of minutes, consistent with the findings that SOA particles formed by coagulation are spherical on the relevant experimental timescales. Measurements on aged SOA particles doped with pyrene yield an estimated diffusivity ∼3 times smaller, indicating that hardening occurs with time, which is consistent with the increase in SOA oligomer content, decrease in water uptake, and decrease in evaporation rates previously observed with aging.© 2013 the Owner Societies.

Shrivastava M.,Pacific Northwest National Laboratory | Zelenyuk A.,Pacific Northwest National Laboratory | Imre D.,Imre Consulting | Easter R.,Pacific Northwest National Laboratory | And 3 more authors.
Journal of Geophysical Research: Atmospheres | Year: 2013

We investigate issues related to volatility and multi-generational gas-phase aging parameterizations affecting the formation and evolution of secondary organic aerosol (SOA) in models. We show that when assuming realistic values for the mass accommodation coefficient, experimentally observed SOA evaporation rates imply significantly lower "effective volatility" than those derived from SOA growth in smog chambers, pointing to the role of condensed phase processes and suggesting that models need to use different parameters to describe the formation and evolution of SOA. We develop a new, experimentally driven paradigm to represent SOA as a non-absorbing semi-solid with very low "effective volatility." We modify both a box model and a 3D chemical transport model, to include simplified parameterizations capturing the first-order effects of gas-phase fragmentation reactions and investigate the implications of treating SOA as a non-volatile, non-absorbing semi-solid (NVSOA). Box model simulations predict SOA loadings decrease with increasing fragmentation, and similar SOA loadings are calculated in the traditional, semi-volatile (SVSOA) approach and with the new paradigm (NVSOA) before evaporation reduces loadings of SVSOA. Box-model-calculated O:C ratios increase with aging in both the SVSOA and the NVSOA paradigms. Consistent with box model results, 3D model simulations demonstrate that predicted SOA loadings decrease with the addition of fragmentation reactions. The NVSOA paradigm predicts higher SOA loadings compared to the SVSOA paradigm over nearly the entire 3D modeling domain, with larger differences close to the surface and in regions where higher dilution favors SVSOA evaporation. Low effective volatility of SOA Gas phase fragmentation reaction Box and regional modeling ©2013. American Geophysical Union. All Rights Reserved.

Zelenyuk A.,Pacific Northwest National Laboratory | Imre D.,Imre Consulting | Earle M.,Environment Canada | Easter R.,Pacific Northwest National Laboratory | And 6 more authors.
Analytical Chemistry | Year: 2010

The aerosol indirect effect remains the most uncertain aspect of climate change modeling, calling for characterization of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of our single particle mass spectrometer (SPLAT II) operated in dual data acquisition mode to simultaneously measure particle number concentrations, density, asphericity, and individual particle size and quantitative composition, with temporal resolution better than 60 s, thus yielding all the required properties to definitively characterize the aerosol-cloud interaction in this exemplary case. We find that particles are composed of oxygenated organics, many mixed with sulfates, biomass burning particles, some with sulfates, and processed sea-salt. Cloud residuals are found to contain more sulfates than background particles, explaining their higher efficiency to serve as cloud condensation nuclei (CCN). Additionally, CCN sulfate content increased with time due to in-cloud droplet processing. A comparison between the size distributions of background, CCN, and interstitial particles shows that while nearly all CCN particles are larger than 100 nm, over 80% of interstitial particles are smaller than 100 nm. We conclude that for this cloud, particle size is the controlling factor on aerosol activation into cloud-droplets, with higher sulfate content playing a secondary role. © 2010 American Chemical Society.

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