The "glass transition'' as a topological defect driven transition in a distribution of crystals and a prediction of a universal viscosity collapse

Topological defects are typically quantified relative to ordered backgrounds. The importance of these defects to the understanding of physical phenomena including diverse equilibrium melting transitions from low temperature ordered to higher temperatures disordered systems (and vice versa) can hardly be overstated. Amorphous materials such as glasses seem to constitute a fundamental challenge to this paradigm. A long held dogma is that transitions into and out of an amorphous glassy state are distinctly different from typical equilibrium phase transitions and must call for radically different concepts. In this work, we critique this belief. We examine systems that may be viewed as simultaneous distribution of different ordinary equilibrium structures. In particular, we focus on the analogs of melting (or freezing) transitions in such distributed systems. The theory that we arrive at yields dynamical, structural, and thermodynamic behaviors of glasses and supercooled fluids that, for the properties tested thus far, are in qualitative and quantitative agreement with experiment. We arrive at a prediction for the viscosity and dielectric relaxations that is universally satisfied for all experimentally measured supercooled liquids and glasses over 15 decades.Comment: 21 pages, 2 figure

Dust-Bounded ULIRGs? Model Predictions for Infrared Spectroscopic Surveys

The observed faintness of infrared fine-structure line emission along with the warm far-infrared (FIR) colors of ultraluminous infrared galaxies (ULIRGs) is a long-standing problem. In this work, we calculate the line and continuum properties of a cloud exposed to an Active Galactic Nucleus (AGN) and starburst spectral energy distribution (SED). We use an integrated modeling approach, predicting the spectrum of ionized, atomic, and molecular environments in pressure equilibrium. We find that the effects of high ratios of impinging ionizing radiation density to particle density (i.e. high ionization parameters, or U) can reproduce many ULIRG observational characteristics. Physically, as U increases, the fraction of UV photons absorbed by dust increases, corresponding to fewer photons available to photoionize and heat the gas, producing what is known as a "dust-bounded" nebula. We show that high U effects can explain the "[C II] deficit", the ~1 dex drop in the [C II] 158 micron /FIR ratio seen in ULIRGs when compared to starburst or normal galaxies. Additionally, by increasing U through increasing the ionizing photon flux, warmer dust and thus higher IRAS F(60)/F(100) ratios result. High U effects also predict an increase in [O I]63 micron /[C II] 158 micron and a gradual decline in [O III] 88 micron /FIR, similar to the magnitude of the trends observed, and yield a reasonable fit to [Ne V]14 micron /FIR ratio AGN observations.Comment: 34 pages, 13 figures, accepted for publication in the Astrophysical Journa

Perspectives on Interstellar Dust Inside and Outside of the Heliosphere

Measurements by dust detectors on interplanetary spacecraft appear to indicate a substantial flux of interstellar particles with masses exceeding 10^{-12}gram. The reported abundance of these massive grains cannot be typical of interstellar gas: it is incompatible with both interstellar elemental abundances and the observed extinction properties of the interstellar dust population. We discuss the likelihood that the Solar System is by chance located near an unusual concentration of massive grains and conclude that this is unlikely, unless dynamical processes in the ISM are responsible for such concentrations. Radiation pressure might conceivably drive large grains into "magnetic valleys". If the influx direction of interstellar gas and dust is varying on a ~10 yr timescale, as suggested by some observations, this would have dramatic implications for the small-scale structure of the interstellar medium.Comment: 13 pages. To appear in Space Science Review

A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

International audienceAtmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces

Effects of relative humidity on aerosol light scattering in the Arctic

Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties – especially the aerosol light scattering – are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH>30–40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time for aerosol particles present in summer and fall in the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σ<sub>sp</sub>(λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions with an average RH<10% (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor <i>f</i>(RH, λ) is the key parameter to describe the RH effect on σ<sub>sp</sub>(λ) and is defined as the RH dependent σ<sub>sp</sub>(RH, λ) divided by the corresponding dry σ<sub>sp</sub>(RH<sub>dry</sub>, λ). During our campaign the average <i>f</i>(RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of <i>f</i>(RH, λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry measured in-situ scattering coefficients. The RH dependency of the recorded <i>f</i>(RH, λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor <i>g</i>(RH), defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found, on average, <i>g</i>(RH=85%) values to be 1.61±0.12 (mean±standard deviation). No clear seasonal shift of <i>f</i>(RH, λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of <i>f</i>(RH, λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we present a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location

Effect of humidity on nitric acid uptake to mineral dust aerosol particles

International audienceThis study presents the first laboratory observation of HNO3 uptake by airborne mineral dust particles. The model aerosols were generated by dry dispersion of Arizona Test Dust (ATD), SiO2, and by nebulizing a saturated solution of calcium carbonate. The uptake of 13N-labeled gaseous nitric acid was observed in a flow reactor on the 0.2?2 s reaction time scale at room temperature and atmospheric pressure. The amount of nitric acid appearing in the aerosol phase at the end of the flow tube was found to be a linear function of the aerosol surface area. SiO2 particles did not show any significant uptake, while the CaCO3 aerosol was found to be more reactive than ATD. Due to the smaller uncertainty associated with the reactive surface area in the case of suspended particles as compared to bulk powder samples, we believe that we provide an improved estimate of the rate of uptake of HNO3 to mineral dust. The fact that the rate of uptake was smaller at a concentration of 1012 than at 1011 was indicative of a complex uptake mechanism. The uptake coefficient averaged over the first 2 s of reaction time at a concentration of 1012 molecules cm-3 was found to increase with increasing relative humidity, from 0.022±0.007 at 12% RH to 0.113±0.017 at 73% RH , which was attributed to an increasing degree of solvation of the more basic minerals. The extended processing of the dust by higher concentrations of HNO3 at 85% RH led to a water soluble coating on the particles and enhanced their hygroscopicity

Hygroscopicity of the submicrometer aerosol at the high-alpine site Jungfraujoch, 3580 m a.s.l., Switzerland

Data from measurements of hygroscopic growth of submicrometer aerosol with a hygroscopicity tandem differential mobility analyzer (HTDMA) during four campaigns at the high alpine research station Jungfraujoch, Switzerland, are presented. The campaigns took place during the years 2000, 2002, 2004 and 2005, each lasting approximately one month. Hygroscopic growth factors (<i>GF</i>, i.e. the relative change in particle diameter from dry diameter, <i>D</i><sub>0</sub>, to diameter measured at higher relative humidity, RH) are presented for three distinct air mass types, namely for: 1) free tropospheric winter conditions, 2) planetary boundary layer influenced air masses (during a summer period) and 3) Saharan dust events (SDE). The <i>GF</i> values at 85% RH (<i>D</i><sub>0</sub>=100 nm) were 1.40±0.11 and 1.29±0.08 for the first two situations while for SDE a bimodal <i>GF</i> distribution was often found. No phase changes were observed when the RH was varied between 10–90%, and the continuous water uptake could be well described with a single-parameter empirical model. The frequency distributions of the average hygroscopic growth factors and the width of the retrieved growth factor distributions (indicating whether the aerosol is internally or externally mixed) are presented, which can be used for modeling purposes. <br><br> Measurements of size resolved chemical composition were performed with an aerosol mass spectrometer in parallel to the <i>GF</i> measurements. This made it possible to estimate the apparent ensemble mean <i>GF</i> of the organics (<i>GF</i><sub>org</sub>) using inverse ZSR (Zdanovskii-Stokes-Robinson) modeling. <i>GF</i><sub>org</sub> was found to be ~1.20 at <i>a</i><sub>w</sub>=0.85, which is at the upper end of previous laboratory and field data though still in agreement with the highly aged and oxidized nature of the Jungfraujoch aerosol

Physical properties of Southern infrared dark clouds

It is commonly assumed that cold and dense Infrared Dark Clouds (IRDCs) likely represent the birth sites massive stars. Therefore, this class of objects gets increasing attention. To enlarge the sample of well-characterised IRDCs in the southern hemisphere, we have set up a program to study the gas and dust of southern IRDCs. The present paper aims at characterizing the continuuum properties of this sample of objects. We cross-correlated 1.2 mm continuum data from SIMBA@SEST with Spitzer/GLIMPSE images to establish the connection between emission sources at millimeter wavelengths and the IRDCs we see at 8 $\mu$m in absorption against the bright PAH background. Analysing the dust emission and extinction leads to a determination of masses and column densities, which are important quantities in characterizing the initial conditions of massive star formation. The total masses of the IRDCs were found to range from 150 to 1150 $\rm M_\odot$ (emission data) and from 300 to 1750 $\rm M_\odot$ (extinction data). We derived peak column densities between 0.9 and 4.6 $\times 10^{22}$ cm$^{-2}$ (emission data) and 2.1 and 5.4 $\times 10^{22}$ cm$^{-2}$ (extinction data). We demonstrate that the extinction method fails for very high extinction values (and column densities) beyond A$_{\rm V}$ values of roughly 75 mag according to the Weingartner & Draine (2001) extinction relation $R_{\rm V} = 5.5$ model B. The derived column densities, taking into account the spatial resolution effects, are beyond the column density threshold of 3.0 $\times 10^{23}$ cm$^{-2}$ required by theoretical considerations for massive star formation. We conclude that the values for column densities derived for the selected IRDC sample make these objects excellent candidates for objects in the earliest stages of massive star formation.Comment: Accepted for publication in Astronomy & Astrophysic

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=−88%) unless a secondary source of particles is included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental boundary layer (BL) are also biased low (NMB=−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