Jamming and condensation in one-dimensional driven flow.

PubMed

Soh, Hyungjoon; Ha, Meesoon; Jeong, Hawoong

2018-03-01

We revisit the slow-bond (SB) problem of the one-dimensional (1D) totally asymmetric simple exclusion process (TASEP) with modified hopping rates. In the original SB problem, it turns out that a local defect is always relevant to the system as jamming, so that phase separation occurs in the 1D TASEP. However, crossover scaling behaviors are also observed as finite-size effects. In order to check if the SB can be irrelevant to the system with particle interaction, we employ the condensation concept in the zero-range process. The hopping rate in the modified TASEP depends on the interaction parameter and the distance up to the nearest particle in the moving direction, besides the SB factor. In particular, we focus on the interplay of jamming and condensation in the current-density relation of 1D driven flow. Based on mean-field calculations, we present the fundamental diagram and the phase diagram of the modified SB problem, which are numerically checked. Finally, we discuss how the condensation of holes suppresses the jamming of particles and vice versa, where the partially condensed phase is the most interesting, compared to that in the original SB problem.

Two characteristic temperatures for a Bose-Einstein condensate of a finite number of particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Idziaszek, Z.; Institut fuer Theoretische Physik, Universitaet Hannover, D-30167 Hannover,; Rzazewski, K.

2003-09-01

We consider two characteristic temperatures for a Bose-Einstein condensate, which are related to certain properties of the condensate statistics. We calculate them for an ideal gas confined in power-law traps and show that they approach the critical temperature in the limit of large number of particles. The considered characteristic temperatures can be useful in the studies of Bose-Einstein condensates of a finite number of atoms indicating the point of a phase transition.

Can Bose condensation of alpha particles be observed in heavy ion collisions?

NASA Technical Reports Server (NTRS)

Tripathi, Ram K.; Townsend, Lawrence W.

1993-01-01

Using a fully self-consistent quantum statistical model, we demonstrate the possibility of Bose condensation of alpha particles with a concomitant phase transition in heavy ion collisions. Suggestions for the experimental observation of the signature of the onset of this phenomenon are made.

Biogenic Potassium Salt Particles as Seeds for Secondary Organic Aerosol in the Amazon

NASA Astrophysics Data System (ADS)

Pöhlker, Christopher; Wiedemann, Kenia T.; Sinha, Bärbel; Shiraiwa, Manabu; Gunthe, Sachin S.; Smith, Mackenzie; Su, Hang; Artaxo, Paulo; Chen, Qi; Cheng, Yafang; Elbert, Wolfgang; Gilles, Mary K.; Kilcoyne, Arthur L. D.; Moffet, Ryan C.; Weigand, Markus; Martin, Scot T.; Pöschl, Ulrich; Andreae, Meinrat O.

2012-08-01

The fine particles serving as cloud condensation nuclei in pristine Amazonian rainforest air consist mostly of secondary organic aerosol. Their origin is enigmatic, however, because new particle formation in the atmosphere is not observed. Here, we show that the growth of organic aerosol particles can be initiated by potassium-salt-rich particles emitted by biota in the rainforest. These particles act as seeds for the condensation of low- or semi-volatile organic compounds from the atmospheric gas phase or multiphase oxidation of isoprene and terpenes. Our findings suggest that the primary emission of biogenic salt particles directly influences the number concentration of cloud condensation nuclei and affects the microphysics of cloud formation and precipitation over the rainforest.

Spectral Properties of Gas-phase Condensed Fullerene-like Carbon Nanoparticles from Far-ultraviolet to Infrared Wavelengths

NASA Astrophysics Data System (ADS)

Jäger, C.; Mutschke, H.; Henning, Th.; Huisken, F.

2008-12-01

Carbon solids are ubiquitous material in interstellar space. However, the formation pathway of carbonaceous matter in astrophysical environments, as well as in terrestrial gas-phase condensation reactions, is not yet understood. Laser ablation of graphite in different quenching gas atmospheres, such as pure He, He/H2, and He/H2O at varying pressures, is used to synthesize very small, fullerene-like carbon nanoparticles. The particles are characterized by very small diameters between 1 and 4 nm and a disturbed onion-like structure. The soot particles extracted from the condensation zone obviously represent a very early stage of particle condensation. The spectral properties have been measured from the far-ultraviolet (FUV; λ = 120 nm) to the mid-infrared (MIR; λ = 15 μm). The seedlike soot particles show strong absorption bands in the 3.4 μm range. The profile and the intensity pattern of the 3.4 μm band of the diffuse interstellar medium can be well reproduced by the measured 3.4 μm profile of the condensed particles; however, all the carbon which is left to form solids is needed to fit the intensity of the interstellar bands. In contrast to the assumption that onion-like soot particles could be the carriers of the interstellar ultraviolet (UV) bump, our very small onion-like carbon nanoparticles do not show distinct UV bands due to (π-π*) transitions.

When is an INP not an INP?

NASA Astrophysics Data System (ADS)

Simpson, Emma; Connolly, Paul; McFiggans, Gordon

2016-04-01

Processes such as precipitation and radiation depend on the concentration and size of different hydrometeors within clouds therefore it is important to accurately predict them in weather and climate models. A large fraction of clouds present in our atmosphere are mixed phase; contain both liquid and ice particles. The number of drops and ice crystals present in mixed phase clouds strongly depends on the size distribution of aerosols. Cloud condensation nuclei (CCN), a subset of atmospheric aerosol particles, are required for liquid drops to form in the atmosphere. These particles are ubiquitous in the atmosphere. To nucleate ice particles in mixed phase clouds ice nucleating particles (INP) are required. These particles are rarer than CCN. Here we investigate the case where CCN and INPs are in direct competition with each other for water vapour within a cloud. Focusing on the immersion and condensation modes of freezing (where an INP must be immersed within a liquid drop before it can freeze) we show that the presence of CCN can suppress the formation of ice. CCN are more hydrophilic than IN and as such are better able to compete for water vapour than, typically insoluble, INPs. Therefore water is more likely to condense onto a CCN than INP, leaving the INP without enough condensed water on it to be able to freeze in the immersion or condensation mode. The magnitude of this suppression effect strongly depends on a currently unconstrained quantity. Here we refer to this quantity as the critical mass of condensed water required for freezing, Mwc. Mwc is the threshold amount of water that must be condensed onto a INP before it can freeze in the immersion or condensation mode. Using the detailed cloud parcel model, Aerosol-Cloud-Precipiation-Interaction Model (ACPIM), developed at the University of Manchester we show that if only a small amount of water is required for freezing there is little suppression effect and if a large amount of water is required there is a large suppression effect. In this poster possible ways to constrain Mwc are discussed as well as conditions where the suppression effect is likely to be greatest. Key Words: Clouds, aerosol, CCN, IN, modelling

Photoballistics of volcanic jet activity at Stromboli, Italy

NASA Technical Reports Server (NTRS)

Chouet, B.; Hamisevicz, N.; Mcgetchin, T. R.

1974-01-01

Two night eruptions of the volcano Stromboli were studied through 70-mm photography. Single-camera techniques were used. Particle sphericity, constant velocity in the frame, and radial symmetry were assumed. Properties of the particulate phase found through analysis include: particle size, velocity, total number of particles ejected, angular dispersion and distribution in the jet, time variation of particle size and apparent velocity distribution, averaged volume flux, and kinetic energy carried by the condensed phase. The frequency distributions of particle size and apparent velocities are found to be approximately log normal. The properties of the gas phase were inferred from the fact that it was the transporting medium for the condensed phase. Gas velocity and time variation, volume flux of gas, dynamic pressure, mass erupted, and density were estimated. A CO2-H2O mixture is possible for the observed eruptions. The flow was subsonic. Velocity variations may be explained by an organ pipe resonance. Particle collimation may be produced by a Magnus effect.

Phase separation of a Lennard-Jones fluid interacting with a long, condensed polymer chain: implications for the nuclear body formation near chromosomes.

PubMed

Oh, Inrok; Choi, Saehyun; Jung, YounJoon; Kim, Jun Soo

2015-08-28

Phase separation in a biological cell nucleus occurs in a heterogeneous environment filled with a high density of chromatins and thus it is inevitably influenced by interactions with chromatins. As a model system of nuclear body formation in a cell nucleus filled with chromatins, we simulate the phase separation of a low-density Lennard-Jones (LJ) fluid interacting with a long, condensed polymer chain. The influence of the density variation of LJ particles above and below the phase boundary and the role of attractive interactions between LJ particles and polymer segments are investigated at a fixed value of strong self-interaction between LJ particles. For a density of LJ particles above the phase boundary, phase separation occurs and a dense domain of LJ particles forms irrespective of interactions with the condensed polymer chain whereas its localization relative to the polymer chain is determined by the LJ-polymer attraction strength. Especially, in the case of moderately weak attractions, the domain forms separately from the polymer chain and subsequently associates with the polymer chain. When the density is below the phase boundary, however, the formation of a dense domain is possible only when the LJ-polymer attraction is strong enough, for which the domain grows in direct contact with the interacting polymer chain. In this work, different growth behaviors of LJ particles result from the differences in the density of LJ particles and in the LJ-polymer interaction, and this work suggests that the distinct formation of activity-dependent and activity-independent nuclear bodies (NBs) in a cell nucleus may originate from the differences in the concentrations of body-specific NB components and in their interaction with chromatins.

INTEGRATED AND REAL-TIME DIFFUSION DENUDER SAMPLE FOR PM2.5. (R825367)

EPA Science Inventory

Abstract

Particulate matter (PM) is a complex mixture of stable condensed phases, adsorbed or dissolved gases, and semi-volatile materials, i.e. compounds that transfer between the gas and condensed phases. Fine particles in both rural and urban environments contain su...

Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

NASA Astrophysics Data System (ADS)

Zuend, A.; Seinfeld, J.

2011-12-01

Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal mixtures substantially overestimates the SOA mass, especially at high relative humidity.

Constant-pressure nested sampling with atomistic dynamics

NASA Astrophysics Data System (ADS)

Baldock, Robert J. N.; Bernstein, Noam; Salerno, K. Michael; Pártay, Lívia B.; Csányi, Gábor

2017-10-01

The nested sampling algorithm has been shown to be a general method for calculating the pressure-temperature-composition phase diagrams of materials. While the previous implementation used single-particle Monte Carlo moves, these are inefficient for condensed systems with general interactions where single-particle moves cannot be evaluated faster than the energy of the whole system. Here we enhance the method by using all-particle moves: either Galilean Monte Carlo or the total enthalpy Hamiltonian Monte Carlo algorithm, introduced in this paper. We show that these algorithms enable the determination of phase transition temperatures with equivalent accuracy to the previous method at 1 /N of the cost for an N -particle system with general interactions, or at equal cost when single-particle moves can be done in 1 /N of the cost of a full N -particle energy evaluation. We demonstrate this speed-up for the freezing and condensation transitions of the Lennard-Jones system and show the utility of the algorithms by calculating the order-disorder phase transition of a binary Lennard-Jones model alloy, the eutectic of copper-gold, the density anomaly of water, and the condensation and solidification of bead-spring polymers. The nested sampling method with all three algorithms is implemented in the pymatnest software.

Self-cleaning of superhydrophobic surfaces by self-propelled jumping condensate

PubMed Central

Wisdom, Katrina M.; Qu, Xiaopeng; Liu, Fangjie; Watson, Gregory S.; Chen, Chuan-Hua

2013-01-01

The self-cleaning function of superhydrophobic surfaces is conventionally attributed to the removal of contaminating particles by impacting or rolling water droplets, which implies the action of external forces such as gravity. Here, we demonstrate a unique self-cleaning mechanism whereby the contaminated superhydrophobic surface is exposed to condensing water vapor, and the contaminants are autonomously removed by the self-propelled jumping motion of the resulting liquid condensate, which partially covers or fully encloses the contaminating particles. The jumping motion off the superhydrophobic surface is powered by the surface energy released upon coalescence of the condensed water phase around the contaminants. The jumping-condensate mechanism is shown to spontaneously clean superhydrophobic cicada wings, where the contaminating particles cannot be removed by gravity, wing vibration, or wind flow. Our findings offer insights for the development of self-cleaning materials. PMID:23630277

Cloud Condensation in Titan's Lower Stratosphere

NASA Technical Reports Server (NTRS)

Romani, Paul N.; Anderson, Carrie M.

2011-01-01

A 1-D condensation model is developed for the purpose of reproducing ice clouds in Titan's lower stratosphere observed by the Composite Infrared Spectrometer (CIRS) onboard Cassini. Hydrogen cyanide (HCN), cyanoacetylene (HC3N), and ethane (C2H6) vapors are treated as chemically inert gas species that flow from an upper boundary at 500 km to a condensation sink near Titan's tropopause (-45 km). Gas vertical profiles are determined from eddy mixing and a downward flux at the upper boundary. The condensation sink is based upon diffusive growth of the cloud particles and is proportional to the degree of supersaturation in the cloud formation regIOn. Observations of the vapor phase abundances above the condensation levels and the locations and properties of the ice clouds provide constraints on the free parameters in the model. Vapor phase abundances are determined from CIRS mid-IR observations, whereas cloud particle sizes, altitudes, and latitudinal distributions are derived from analyses of CIRS far-IR observations of Titan. Specific cloud constraints include: I) mean particle radii of2-3 J.lm inferred from the V6 506 cm- band of HC3N, 2) latitudinal abundance distributions of condensed nitriles, inferred from a composite emission feature that peaks at 160/cm , and 3) a possible hydrocarbon cloud layer at high latitudes, located near an altitude of 60 km, which peaks between 60 and 80 cm l . Nitrile abundances appear to diminish substantially at high northern latitudes over the time period 2005 to 2010 (northern mid winter to early spring). Use of multiple gas species provides a consistency check on the eddy mixing coefficient profile. The flux at the upper boundary is the net column chemical production from the upper atmosphere and provides a constraint on chemical pathways leading to the production of these compounds. Comparison of the differing lifetimes, vapor phase transport, vapor phase loss rate, and particle sedimentation, sheds light on temporal stability of the clouds.

Ferroelectricity by Bose-Einstein condensation in a quantum magnet.

PubMed

Kimura, S; Kakihata, K; Sawada, Y; Watanabe, K; Matsumoto, M; Hagiwara, M; Tanaka, H

2016-09-26

The Bose-Einstein condensation is a fascinating phenomenon, which results from quantum statistics for identical particles with an integer spin. Surprising properties, such as superfluidity, vortex quantization or Josephson effect, appear owing to the macroscopic quantum coherence, which spontaneously develops in Bose-Einstein condensates. Realization of Bose-Einstein condensation is not restricted in fluids like liquid helium, a superconducting phase of paired electrons in a metal and laser-cooled dilute alkali atoms. Bosonic quasi-particles like exciton-polariton and magnon in solids-state systems can also undergo Bose-Einstein condensation in certain conditions. Here, we report that the quantum coherence in Bose-Einstein condensate of the magnon quasi particles yields spontaneous electric polarization in the quantum magnet TlCuCl 3 , leading to remarkable magnetoelectric effect. Very soft ferroelectricity is realized as a consequence of the O(2) symmetry breaking by magnon Bose-Einstein condensation. The finding of this ferroelectricity will open a new window to explore multi-functionality of quantum magnets.

Composite particle theory of three-dimensional gapped fermionic phases: Fractional topological insulators and charge-loop excitation symmetry

NASA Astrophysics Data System (ADS)

Ye, Peng; Hughes, Taylor L.; Maciejko, Joseph; Fradkin, Eduardo

2016-09-01

Topological phases of matter are usually realized in deconfined phases of gauge theories. In this context, confined phases with strongly fluctuating gauge fields seem to be irrelevant to the physics of topological phases. For example, the low-energy theory of the two-dimensional (2D) toric code model (i.e., the deconfined phase of Z2 gauge theory) is a U(1 )×U(1 ) Chern-Simons theory in which gauge charges (i.e., e and m particles) are deconfined and the gauge fields are gapped, while the confined phase is topologically trivial. In this paper, we point out a route to constructing exotic three-dimensional (3D) gapped fermionic phases in a confining phase of a gauge theory. Starting from a parton construction with strongly fluctuating compact U(1 )×U(1 ) gauge fields, we construct gapped phases of interacting fermions by condensing two linearly independent bosonic composite particles consisting of partons and U(1 )×U(1 ) magnetic monopoles. This can be regarded as a 3D generalization of the 2D Bais-Slingerland condensation mechanism. Charge fractionalization results from a Debye-Hückel-type screening cloud formed by the condensed composite particles. Within our general framework, we explore two aspects of symmetry-enriched 3D Abelian topological phases. First, we construct a new fermionic state of matter with time-reversal symmetry and Θ ≠π , the fractional topological insulator. Second, we generalize the notion of anyonic symmetry of 2D Abelian topological phases to the charge-loop excitation symmetry (Charles ) of 3D Abelian topological phases. We show that line twist defects, which realize Charles transformations, exhibit non-Abelian fusion properties.

Numerical simulation of submicron particles formation by condensation at coals burning

NASA Astrophysics Data System (ADS)

Kortsenshteyn, N. M.; Petrov, L. V.

2017-11-01

The thermodynamic analysis of the composition of the combustion products of 15 types of coals was carried out with consideration for the formation of potassium and sodium aluminosilicates and solid and liquid slag removal. Based on the results of the analysis, the approximating temperature dependences of the concentrations of condensed components (potassium and sodium sulfates) were obtained for the cases of two-phase and single-phase equilibriums; conclusions on the comparative influence of solid and liquid slag removal on the probability of the formation of submicron particles on the combustion of coals were made. The found dependences was make it possible to perform a numerical simulation of the bulk condensation of potassium and sodium sulfate vapors upon the cooling of coal combustion products in a process flow. The number concentration and size distribution of the formed particles have been determined. Agreement with experimental data on the fraction composition of particles has been reached at a reasonable value of a free parameter of the model.

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

NASA Technical Reports Server (NTRS)

Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

2015-01-01

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

Deposition Nucleation or Pore Condensation and Freezing?

NASA Astrophysics Data System (ADS)

David, Robert O.; Mahrt, Fabian; Marcolli, Claudia; Fahrni, Jonas; Brühwiler, Dominik; Lohmann, Ulrike; Kanji, Zamin A.

2017-04-01

Ice nucleation plays an important role in moderating Earth's climate and precipitation formation. Over the last century of research, several mechanisms for the nucleation of ice have been identified. Of the known mechanisms for ice nucleation, only deposition nucleation occurs below water saturation. Deposition nucleation is defined as the formation of ice from supersaturated water vapor on an insoluble particle without the prior formation of liquid. However, recent work has found that the efficiency of so-called deposition nucleation shows a dependence on the homogeneous freezing temperature of water even though no liquid phase is presumed to be present. Additionally, the ability of certain particles to nucleate ice more efficiently after being pre-cooled (pre-activation) raises questions on the true mechanism when ice nucleation occurs below water saturation. In an attempt to explain the dependence of the efficiency of so-called deposition nucleation on the onset of homogeneous freezing of liquid water, pore condensation and freezing has been proposed. Pore condensation and freezing suggests that the liquid phase can exist under sub-saturated conditions with respect to liquid in narrow confinements or pores due to the inverse Kelvin effect. Once the liquid-phase condenses, it is capable of nucleating ice either homogeneously or heterogeneously. The role of pore condensation and freezing is assessed in the Zurich Ice Nucleation Chamber, a continuous flow diffusion chamber, using spherical nonporous and mesoporous silica particles. The mesoporous silica particles have a well-defined particle size range of 400 to 600nm with discreet pore sizes of 2.5, 2.8, 3.5 and 3.8nm. Experiments conducted between 218K and 238K show that so-called deposition nucleation only occurs below the homogenous freezing temperature of water and is highly dependent on the presence of pores and their size. The results strongly support pore condensation and freezing, questioning the role of deposition nucleation as an ice nucleation pathway.

Growth rates of fine aerosol particles at a site near Beijing in June 2013

NASA Astrophysics Data System (ADS)

Zhao, Chuanfeng; Li, Yanan; Zhang, Fang; Sun, Yele; Wang, Pucai

2018-02-01

Growth of fine aerosol particles is investigated during the Aerosol-CCN-Cloud Closure Experiment campaign in June 2013 at an urban site near Beijing. Analyses show a high frequency (˜ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h-1 with a mean value of ˜ 5.1 nm h-1. A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation, extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles. Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.

Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-04-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

PubMed Central

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

PubMed

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Shock Interaction of Metal Particles in Condensed Explosive Detonation

NASA Astrophysics Data System (ADS)

Ripley, Robert; Zhang, Fan; Lien, Fue-Sang

2005-07-01

For detonation propagation in a condensed explosive with metal particles, a macro-scale physical model describing the momentum transfer between the explosive and particles has yet to be completely established. Previous 1D and 2D meso-scale modeling studies indicated that significant momentum transfer from the explosive to the particles occurs as the leading shock front crosses the particles, thus influencing the initiation and detonation structure. In this work, 3D meso-scale modeling is conducted to further study the two-phase momentum transfer during the shock diffraction and subsequent detonation in liquid nitromethane containing packed metal particles. Detonation of the condensed explosive is computed using an Arrhenius reaction model and a hybrid EOS model that combines the Mie-Gruneisen equation for reactants and the JWL equation for products. The compressible particles are modeled using the Tait EOS, where the material strength is negligible. The effect of particle packing configuration and inter-particle spacing is shown by parametric studies. Finally, a physical description of the momentum transfer is discussed.

Development and evaluation of the aerosol dynamics and gas phase chemistry model ADCHEM

NASA Astrophysics Data System (ADS)

Roldin, P.; Swietlicki, E.; Schurgers, G.; Arneth, A.; Lehtinen, K. E. J.; Boy, M.; Kulmala, M.

2011-06-01

The aim of this work was to develop a model suited for detailed studies of aerosol dynamics, gas and particle phase chemistry within urban plumes, from local scale (1 × 1 km2) to regional scale. This article describes and evaluates the trajectory model for Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer (ADCHEM). The model treats both vertical and horizontal dispersion perpendicular to an air mass trajectory (2-space dimensions). The Lagrangian approach enables a more detailed representation of the aerosol dynamics, gas and particle phase chemistry and a finer spatial and temporal resolution compared to that of available regional 3D-CTMs. These features make it among others well suited for urban plume studies. The aerosol dynamics model includes Brownian coagulation, dry deposition, wet deposition, in-cloud processing, condensation, evaporation, primary particle emissions and homogeneous nucleation. The organic mass partitioning was either modeled with a 2-dimensional volatility basis set (2D-VBS) or with the traditional two-product model approach. In ADCHEM these models consider the diffusion limited and particle size dependent condensation and evaporation of 110 and 40 different organic compounds respectively. The gas phase chemistry model calculates the gas phase concentrations of 61 different species, using 130 different chemical reactions. Daily isoprene and monoterpene emissions from European forests were simulated separately with the vegetation model LPJ-GUESS, and included as input to ADCHEM. ADCHEM was used to simulate the ageing of the urban plumes from the city of Malmö in southern Sweden (280 000 inhabitants). Several sensitivity tests were performed concerning the number of size bins, size structure method, aerosol dynamic processes, vertical and horizontal mixing, coupled or uncoupled condensation and the secondary organic aerosol formation. The simulations show that the full-stationary size structure gives accurate results with little numerical diffusion when more than 50 size bins are used between 1.5 and 2500 nm, while the moving-center method is preferable when only a few size bins are selected. The particle number size distribution in the center of the urban plume from Malmö was mainly affected by dry deposition, coagulation and vertical dilution. The modeled PM2.5 mass was dominated by organic material, nitrate, sulfate and ammonium. If the condensation of HNO3 and NH3 was treated as a coupled process (pH independent) the model gave lower nitrate PM2.5 mass than if considering uncoupled condensation. Although the time of ageing from that SOA precursors are emitted until condensable products are formed is substantially different with the 2D-VBS and two product model, the models gave similar total organic mass concentrations.

Aerosol-chamber study of the α-pinene/O 3 reaction: influence of particle acidity on aerosol yields and products

NASA Astrophysics Data System (ADS)

Iinuma, Yoshiteru; Böge, Olaf; Gnauk, Thomas; Herrmann, Hartmut

α-Pinene ozonolysis was carried out in the presence of ammonium sulfate or sulfuric acid seed particles in a 9 m 3 Teflon chamber at the mixing ratios of 100 ppbv for α-pinene and about 70 ppbv for ozone. The evolution of size distribution was measured by means of a differential mobility particle sizer (DMPS). The resulting secondary organic aerosol (SOA) was sampled by a denuder/quartz fiber filter combination for the determination of the total organic carbon concentration (TOC) in the particle phase, using a thermographic method and by a denuder/PTFE filter combination for the analysis of individual chemical species in the particle phase using capillary electrophoresis-electrospray ionization-mass spectrometry (CE-ESI-MS). cis-Pinic acid ( m/ z 185) and another species tentatively identified at m/ z 171 and 199 were the major particle phase species for both seed particles although the product yields were different, indicating the influence of seed particle acidity. A thermographic method for the determination of TOC showed an increase of particle phase organics by 40% for the experiments with higher acidity. CE-ESI-MS analysis showed a large increase in the concentration of compounds with Mw>300 from the experiments with sulfuric acid seed particles. These results suggest that the seed particle acidity enhances the yield of SOA and plays an important role in the formation of larger molecules in the particle phase. Our results from direct particle phase chemical analysis suggest for the first time that condensation of smaller organics takes place by polymerization or aldol condensation following the formation of aldehydes, such as pinonaldehyde from the terpene ozonolysis.

The Exoplanet Cloud Atlas

NASA Astrophysics Data System (ADS)

Gao, Peter; Marley, Mark S.; Morley, Caroline; Fortney, Jonathan J.

2017-10-01

Clouds have been readily inferred from observations of exoplanet atmospheres, and there exists great variability in cloudiness between planets, such that no clear trend in exoplanet cloudiness has so far been discerned. Equilibrium condensation calculations suggest a myriad of species - salts, sulfides, silicates, and metals - could condense in exoplanet atmospheres, but how they behave as clouds is uncertain. The behavior of clouds - their formation, evolution, and equilibrium size distribution - is controlled by cloud microphysics, which includes processes such as nucleation, condensation, and evaporation. In this work, we explore the cloudy exoplanet phase space by using a cloud microphysics model to simulate a suite of cloud species ranging from cooler condensates such as KCl/ZnS, to hotter condensates like perovskite and corundum. We investigate how the cloudiness and cloud particle sizes of exoplanets change due to variations in temperature, metallicity, gravity, and cloud formation mechanisms, and how these changes may be reflected in current and future observations. In particular, we will evaluate where in phase space could cloud spectral features be observable using JWST MIRI at long wavelengths, which will be dependent on the cloud particle size distribution and cloud species.

Symmetry-enriched Bose-Einstein condensates in a spin-orbit-coupled bilayer system

NASA Astrophysics Data System (ADS)

Cheng, Jia-Ming; Zhou, Xiang-Fa; Zhou, Zheng-Wei; Guo, Guang-Can; Gong, Ming

2018-01-01

We consider the fate of Bose-Einstein condensation with time-reversal symmetry and inversion symmetry in a spin-orbit-coupled bilayer system. When these two symmetry operators commute, all the single-particle bands are exactly twofold degenerate in the momentum space. The scattering in the twofold-degenerate rings can relax the spin-momentum locking effect from spin-orbit-coupling interaction and thus can realize the spin-polarized plane-wave phase even when the interparticle interaction dominates. When these two operators anticommute, the lowest two bands may have the same minimal energy, but with totally different spin structures. As a result, the competition between different condensates in these two energetically degenerate rings can give rise to different stripe phases with atoms condensed at two or four collinear momenta. We find that the crossover between these two cases is accompanied by the excited band condensation when the interference energy can overcome the increased single-particle energy in the excited band. This effect is not based on strong interaction and thus can be realized even with moderate interaction strength.

Blockage-induced condensation controlled by a local reaction

NASA Astrophysics Data System (ADS)

Cirillo, Emilio N. M.; Colangeli, Matteo; Muntean, Adrian

2016-10-01

We consider the setup of stationary zero range models and discuss the onset of condensation induced by a local blockage on the lattice. We show that the introduction of a local feedback on the hopping rates allows us to control the particle fraction in the condensed phase. This phenomenon results in a current versus blockage parameter curve characterized by two nonanalyticity points.

Quantum fluids of light in acoustic lattices

NASA Astrophysics Data System (ADS)

Cerda-Méndez, E. A.; Krizhanovskii, D. N.; Skolnick, M. S.; Santos, P. V.

2018-01-01

In this topical review, we report on the recent advances on the manipulation of hybrid light-matter quasi-particles called exciton-polaritons and their quantum condensed phases by means of acoustic and static periodic potentials. Polaritons are a superposition of photons and excitons and form in optical microcavities with quantum wells embedded in it. They are low-mass bosons in the dilute limit and have strong inter-particle interactions inherited from the excitonic component. Their capability to form quantum-condensed phases at temperatures in the kelvin range and to behave like quantum fluids makes them very attractive for novel solid-state devices. Since their de Broglie wavelength is of the order of a few micrometers, polaritons can be manipulated using static or dynamic potentials with micrometer scales. We present here a summary of the techniques used to submit polaritons and their condensed phases to periodic potentials, with an emphasis in dynamic ones produced by surface acoustic waves. We discuss the interesting phenomena that occur under such a modulation, such as condensation in excited states of the Brillouin zone, fragmentation of a condensate, formation of self-localized wavepackets, and Dirac and massive polaritons in static hexagonal and kagome lattices, respectively. The different techniques explored open the way to implement polariton-based quantum simulators, nano-optomechanic resonators and polaritonic topological insulators.

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors.

PubMed

Hinton, J P; Thewalt, E; Alpichshev, Z; Mahmood, F; Koralek, J D; Chan, M K; Veit, M J; Dorow, C J; Barišić, N; Kemper, A F; Bonn, D A; Hardy, W N; Liang, Ruixing; Gedik, N; Greven, M; Lanzara, A; Orenstein, J

2016-04-13

In the underdoped copper-oxides, high-temperature superconductivity condenses from a nonconventional metallic "pseudogap" phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime. This CDW coexists and competes with superconductivity (SC) below the transition temperature Tc, suggesting that these two orders are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime, τqp, as a function of temperature and magnetic field in underdoped HgBa2CuO(4+δ) (Hg-1201) and YBa2Cu3O(6+x) (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that τqp(T) exhibits a local maximum in a small temperature window near Tc that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that Tc marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs.

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors

PubMed Central

Hinton, J. P.; Thewalt, E.; Alpichshev, Z.; Mahmood, F.; Koralek, J. D.; Chan, M. K.; Veit, M. J.; Dorow, C. J.; Barišić, N.; Kemper, A. F.; Bonn, D. A.; Hardy, W. N.; Liang, Ruixing; Gedik, N.; Greven, M.; Lanzara, A.; Orenstein, J.

2016-01-01

In the underdoped copper-oxides, high-temperature superconductivity condenses from a nonconventional metallic ”pseudogap” phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime. This CDW coexists and competes with superconductivity (SC) below the transition temperature Tc, suggesting that these two orders are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime, τqp, as a function of temperature and magnetic field in underdoped HgBa2CuO4+δ (Hg-1201) and YBa2Cu3O6+x (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that τqp(T ) exhibits a local maximum in a small temperature window near Tc that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that Tc marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs. PMID:27071712

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hodshire, Anna L.; Lawler, Michael J.; Zhao, Jun

New-particle formation (NPF) is a significant source of aerosol particles into the atmosphere. However, these particles are initially too small to have climatic importance and must grow, primarily through net uptake of low-volatility species, from diameters  ∼  1 to 30–100 nm in order to potentially impact climate. There are currently uncertainties in the physical and chemical processes associated with the growth of these freshly formed particles that lead to uncertainties in aerosol-climate modeling. Four main pathways for new-particle growth have been identified: condensation of sulfuric-acid vapor (and associated bases when available), condensation of organic vapors, uptake of organic acids through acid–base chemistrymore » in the particle phase, and accretion of organic molecules in the particle phase to create a lower-volatility compound that then contributes to the aerosol mass. The relative importance of each pathway is uncertain and is the focus of this work. The 2013 New Particle Formation Study (NPFS) measurement campaign took place at the DOE Southern Great Plains (SGP) facility in Lamont, Oklahoma, during spring 2013. Measured gas- and particle-phase compositions during these new-particle growth events suggest three distinct growth pathways: (1) growth by primarily organics, (2) growth by primarily sulfuric acid and ammonia, and (3) growth by primarily sulfuric acid and associated bases and organics. To supplement the measurements, we used the particle growth model MABNAG (Model for Acid–Base chemistry in NAnoparticle Growth) to gain further insight into the growth processes on these 3 days at SGP. MABNAG simulates growth from (1) sulfuric-acid condensation (and subsequent salt formation with ammonia or amines), (2) near-irreversible condensation from nonreactive extremely low-volatility organic compounds (ELVOCs), and (3) organic-acid condensation and subsequent salt formation with ammonia or amines. MABNAG is able to corroborate the observed differing growth pathways, while also predicting that ELVOCs contribute more to growth than organic salt formation. However, most MABNAG model simulations tend to underpredict the observed growth rates between 10 and 20 nm in diameter; this underprediction may come from neglecting the contributions to growth from semi-to-low-volatility species or accretion reactions. Our results suggest that in addition to sulfuric acid, ELVOCs are also very important for growth in this rural setting. We discuss the limitations of our study that arise from not accounting for semi- and low-volatility organics, as well as nitrogen-containing species beyond ammonia and amines in the model. Quantitatively understanding the overall budget, evolution, and thermodynamic properties of lower-volatility organics in the atmosphere will be essential for improving global aerosol models.« less

Anisotropic properties of phase separation in two-component dipolar Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Wang, Wei; Li, Jinbin

2018-03-01

Using Crank-Nicolson method, we calculate ground state wave functions of two-component dipolar Bose-Einstein condensates (BECs) and show that, due to dipole-dipole interaction (DDI), the condensate mixture displays anisotropic phase separation. The effects of DDI, inter-component s-wave scattering, strength of trap potential and particle numbers on the density profiles are investigated. Three types of two-component profiles are present, first cigar, along z-axis and concentric torus, second pancake (or blood cell), in xy-plane, and two non-uniform ellipsoid, separated by the pancake and third two dumbbell shapes.

Reactivity of liquid and semisolid secondary organic carbon with chloride and nitrate in atmospheric aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Bingbing; O'Brien, Rachel E.; Univ. of the Pacific, Stockton, CA

2015-05-14

Constituents of secondary organic carbon (SOC) in atmospheric aerosols are often mixed with inorganic components and compose a significant mass fraction of fine particulate matter in the atmosphere. Interactions between SOC and other condensed-phase species are not well understood. Here, we investigate the reactions of liquid-like and semi-solid SOC from ozonolysis of limonene (LSOC) and α-pinene (PSOC) with NaCl using a set of complementary micro-spectroscopic analyses. These reactions result in chloride depletion in the condensed phase, release of gaseous HCl, and formation of organic salts. The reactions attributed to acid displacement by SOC acidic components are driven by the highmore » volatility of HCl. Similar reactions can take place in SOC/NaNO₃ particles. The results show that an increase in SOC mass fraction in the internally mixed SOC/NaCl particles leads to higher chloride depletion. Glass transition temperatures and viscosity of PSOC were estimated for atmospherically relevant conditions. Data show that the reaction extent depends on SOC composition, particle phase state and viscosity, mixing state, temperature, relative humidity (RH), and reaction time. LSOC shows slightly higher potential to deplete chloride than PSOC. Higher particle viscosity at low temperatures and RH can hinder these acid displacement reactions. Formation of organic salts from these overlooked reactions can alter particle physiochemical properties and may affect their reactivity and ability to act as cloud condensation and ice nuclei. The release and potential recycling of HCl and HNO₃ from reacted aerosol particles may have important implications for atmospheric chemistry.« less

Reactivity of liquid and semisolid secondary organic carbon with chloride and nitrate in atmospheric aerosols.

PubMed

Wang, Bingbing; O'Brien, Rachel E; Kelly, Stephen T; Shilling, John E; Moffet, Ryan C; Gilles, Mary K; Laskin, Alexander

2015-05-14

Constituents of secondary organic carbon (SOC) in atmospheric aerosols are often mixed with inorganic components and compose a significant mass fraction of fine particulate matter in the atmosphere. Interactions between SOC and other condensed-phase species are not well understood. Here, we investigate the reactions of liquid-like and semisolid SOC from ozonolysis of limonene (LSOC) and α-pinene (PSOC) with NaCl using a set of complementary microspectroscopic analyses. These reactions result in chloride depletion in the condensed phase, release of gaseous HCl, and formation of organic salts. The reactions attributed to acid displacement by SOC acidic components are driven by the high volatility of HCl. Similar reactions can take place in SOC/NaNO3 particles. The results show that an increase in SOC mass fraction in the internally mixed SOC/NaCl particles leads to higher chloride depletion. Glass transition temperatures and viscosity of PSOC were estimated for atmospherically relevant conditions. Data show that the reaction extent depends on SOC composition, particle phase state and viscosity, mixing state, temperature, relative humidity (RH), and reaction time. LSOC shows slightly higher potential to deplete chloride than PSOC. Higher particle viscosity at low temperatures and RH can hinder these acid displacement reactions. Formation of organic salts from these overlooked reactions can alter particle physiochemical properties and may affect their reactivity and ability to act as cloud condensation and ice nuclei. The release and potential recycling of HCl and HNO3 from reacted aerosol particles may have important implications for atmospheric chemistry.

Organic cloud condensation nuclei: the effect of phase, surface tension, trace soluble species, and oxidative processing on particle activation.

NASA Astrophysics Data System (ADS)

Broekhuizen, K. E.; Thornberry, T.; Abbatt, J. P.

2003-12-01

The ability of organic aerosols to act as cloud condensation nuclei (CCN) will be discussed. A variety of laboratory experiments will be presented which address several key questions concerning organic particle activation. Does the particle phase impact activation? How does surface tension play a role and can a trace amount of a surface active species impact activation? Does a trace amount of a highly soluble species impact the activation of organic particles of moderate to low solubility? Can the activation properties of organic aerosols be enhanced through oxidative processing? To systematically address these issues, the CCN activity of various diacids such as oxalic, malonic, succinic, adipic and azelaic acid have been studied, as well as the addition of trace amounts of nonanoic acid and ammonium sulfate to examine the roles of surface active and soluble species, respectively. The first examination of the role of oxidative processing on CCN activity has involved investigating the effect of ozone oxidation on the activity of oleic acid particles.

Laboratory studies on tropospheric iodine chemistry: bridging the atomic, molecular and particle scale

NASA Astrophysics Data System (ADS)

Gomez Martin, J.; Saunders, R. W.; Blitz, M. A.; Mahajan, A. S.; Plane, J. M.

2008-12-01

High mixing ratios of the iodine oxides IO and OIO have been observed in the polar, mid-latitude and tropical marine boundary layer (MBL). The impact of the iodine chemistry on the oxidizing capacity of the MBL is well documented. Moreover, there is evidence showing that the bursts of new particles measured in coastal regions are produced by the biogenic emission of iodine containing precursors, followed by the photochemical production and condensation of iodine oxide vapours. Airborne measurements of particle growth rates show that these particles can reach significant sizes where they can contribute to the regional aerosol loading, thus suggesting a potential impact on climate on a regional or global scale. Within the frame of the INSPECT project (INorganic Secondary Particle Evolution, Chemistry and Transport) we wish to understand at a fundamental level the tendency for the iodine oxides formed from IO and OIO recombination to condense into particles. Elemental analysis of iodine oxide particles (IOP) made in the laboratory shows that they have the empirical formula I2O5. The major question is how this happens: through formation of I2O5 in the gas phase, followed by polymerization, or by condensation of various IxOy to form amorphous iodine oxides, which subsequently rearrange to I2O5. We are studying the gas phase photochemistry leading to nucleation of IOP, their growth kinetics, aspects of their heterogeneous chemistry, and their properties as ice condensation nuclei. In order to bridge the molecular and the particle scales, a wide variety of techniques are being used, including CRDS, ARAS, LIF, UV-VIS spectroscopy, PI-TOF-MS and mobility particle size scanning. The results obtained so far provide new and interesting insights to the problem. From the gas phase point of view, a unit iodine atom quantum yield from OIO photolysis has been now established across its strong visible spectral bands. This result implies a short lifetime of OIO and explains why in general it could not be observed during daytime in the field. This is also consistent with recently observed ozone depletion events possibly correlated to high concentrations of IO. On the other hand, atmospheric modelling shows that the rate of formation of condensable iodine vapours decreases when a high OIO photolysis rate is considered, although the modelled values are still consistent with the rates of particle formation observed in the MBL. On the particle scale, the role of water and sulphuric acid vapour uptake on the formation and growth of IOP has been studied by analysis of the observed changes to measured particle size distribution data. In the case of water, hygroscopic growth factors have been determined at different ambient relative humidities, while for H2SO4 the uptake coefficient onto IOP has been evaluated. The experimental data suggests the possibility of a ternary nucleation route involving iodine oxide-water-acid vapours. Currently, pulsed laser photolysis coupled to PI-TOF-MS is being used to study the transition regime between the gas and particle phase. With this technique it is possible to resolve small clusters up to 1200 amu with sufficient resolution to determine, e.g., whether I2O4 or I2O5 is the condensable unit of IOP.

Maintenance of order in a moving strong condensate

NASA Astrophysics Data System (ADS)

Whitehouse, Justin; Costa, André; Blythe, Richard A.; Evans, Martin R.

2014-11-01

We investigate the conditions under which a moving condensate may exist in a driven mass transport system. Our paradigm is a minimal mass transport model in which n - 1 particles move simultaneously from a site containing n > 1 particles to the neighbouring site in a preferred direction. In the spirit of a zero-range process the rate u(n) of this move depends only on the occupation of the departure site. We study a hopping rate u(n) = 1 + b/nα numerically and find a moving strong condensate phase for b > bc(α) for all α > 0. This phase is characterised by a condensate that moves through the system and comprises a fraction of the system's mass that tends to unity. The mass lost by the condensate as it moves is constantly replenished from the trailing tail of low occupancy sites that collectively comprise a vanishing fraction of the mass. We formulate an approximate analytical treatment of the model that allows a reasonable estimate of bc(α) to be obtained. We show numerically (for α = 1) that the transition is of mixed order, exhibiting a discontinuity in the order parameter as well as a diverging length scale as b\\searrow bc .

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors

DOE PAGES

Hinton, J. P.; Thewalt, E.; Alpichshev, Z.; ...

2016-04-13

In the underdoped copper-oxides, high-temperature superconductivity condenses from a nonconventional metallic ”pseudogap” phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime. This CDW coexists and competes with superconductivity (SC) below the transition temperature T c, suggesting that these two orders are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime,more » τ qp, as a function of temperature and magnetic field in underdoped HgBa 2CuO 4+δ (Hg-1201) and YBa 2Cu 3O 6+x (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that τ qp(T) exhibits a local maximum in a small temperature window near T c that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that T c marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Lastly, our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs.« less

Detection of molecular interactions

DOEpatents

Groves, John T [Berkeley, CA; Baksh, Michael M [Fremont, CA; Jaros, Michal [Brno, CH

2012-02-14

A method and assay are described for measuring the interaction between a ligand and an analyte. The assay can include a suspension of colloidal particles that are associated with a ligand of interest. The colloidal particles are maintained in the suspension at or near a phase transition state from a condensed phase to a dispersed phase. An analyte to be tested is then added to the suspension. If the analyte binds to the ligand, a phase change occurs to indicate that the binding was successful.

Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site

DOE PAGES

Hodshire, Anna L.; Lawler, Michael J.; Zhao, Jun; ...

2016-07-28

New-particle formation (NPF) is a significant source of aerosol particles into the atmosphere. However, these particles are initially too small to have climatic importance and must grow, primarily through net uptake of low-volatility species, from diameters  ∼  1 to 30–100 nm in order to potentially impact climate. There are currently uncertainties in the physical and chemical processes associated with the growth of these freshly formed particles that lead to uncertainties in aerosol-climate modeling. Four main pathways for new-particle growth have been identified: condensation of sulfuric-acid vapor (and associated bases when available), condensation of organic vapors, uptake of organic acids through acid–base chemistrymore » in the particle phase, and accretion of organic molecules in the particle phase to create a lower-volatility compound that then contributes to the aerosol mass. The relative importance of each pathway is uncertain and is the focus of this work. The 2013 New Particle Formation Study (NPFS) measurement campaign took place at the DOE Southern Great Plains (SGP) facility in Lamont, Oklahoma, during spring 2013. Measured gas- and particle-phase compositions during these new-particle growth events suggest three distinct growth pathways: (1) growth by primarily organics, (2) growth by primarily sulfuric acid and ammonia, and (3) growth by primarily sulfuric acid and associated bases and organics. To supplement the measurements, we used the particle growth model MABNAG (Model for Acid–Base chemistry in NAnoparticle Growth) to gain further insight into the growth processes on these 3 days at SGP. MABNAG simulates growth from (1) sulfuric-acid condensation (and subsequent salt formation with ammonia or amines), (2) near-irreversible condensation from nonreactive extremely low-volatility organic compounds (ELVOCs), and (3) organic-acid condensation and subsequent salt formation with ammonia or amines. MABNAG is able to corroborate the observed differing growth pathways, while also predicting that ELVOCs contribute more to growth than organic salt formation. However, most MABNAG model simulations tend to underpredict the observed growth rates between 10 and 20 nm in diameter; this underprediction may come from neglecting the contributions to growth from semi-to-low-volatility species or accretion reactions. Our results suggest that in addition to sulfuric acid, ELVOCs are also very important for growth in this rural setting. We discuss the limitations of our study that arise from not accounting for semi- and low-volatility organics, as well as nitrogen-containing species beyond ammonia and amines in the model. Quantitatively understanding the overall budget, evolution, and thermodynamic properties of lower-volatility organics in the atmosphere will be essential for improving global aerosol models.« less

Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs

2007-12-01

The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE-3, CLACE-3? and CLACE-4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed-phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in-cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to -25°C. The Wegener-Bergeron-Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.

Formation and Growth of New Organic Aerosol Particles over the Deepwater Horizon Oil Spill

NASA Astrophysics Data System (ADS)

Brock, C. A.; Murphy, D. M.; Bahreini, R.; Middlebrook, A. M.; De Gouw, J. A.

2011-12-01

Aerosol size distributions were measured in June 2010 downwind of the surface oil slick produced by the Deepwater Horizon oil spill in the Gulf of Mexico. Rapid condensation of partially oxidized hydrocarbons was responsible for formation of a plume of secondary organic aerosol downwind of the spill region. New particles were nucleated upwind of the freshest surface oil but downwind of oil that surfaced less than 100 hours previously. These new particles grew by condensation at rates of ~20 nm hr-1; preexisting accumulation mode particles grew by ~10 nm hr-1. The gas-phase concentration of a condensing species necessary to support the observed growth rate assuming irreversible adsorption with unit accommodation coefficient is estimated to be ~0.04-0.09 μg m-3 (~3-8 pptv). The ratio of growth rates for newly formed particles to accumulation mode particles was consistent within error limits with irreversible condensation. Because new particle formation did not occur in areas away from the <100 hr-old oil slick, these results indicate that the oxidation products of VOC species, probably C14-C16 compounds, were directly involved in the growth of the new particles. While a unique and extreme environment, the oil spill plume provides insight into similar processes that may occur in urban and industrial areas where petrochemical products are produced and consumed.

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

Titanium carbide and titania phases on Antarctic ice particles of probable extraterrrestrial origin

NASA Technical Reports Server (NTRS)

Zolensky, M. E.; Pun, A.; Thomas, K. L.

1989-01-01

Two unique titania-rich particles, found within ancient Antarctic ice have been discovered and characterized, and are believed to be of extraterrestrial origin. Both particles contain abundant submicron-sized crystals of Magneli phases (Ti(n)O(2n-1). In addition, one particle contains a core of TiC. Whereas the Magneli phases would have been stable in the early solar nebula, and so probably formed there, the TiC is more likely to have condensed in the cool, dusty, carbon-rich outer shell of a red giant star. It is suggested that both particles are interplanetary dust particles whose Magneli phases carry a record of the PO2-T conditions of the early solar nebula. It is further suggested that the TiC grain in particle 705 is remnant interstellar dust.

Organic Nitrogen in Atmospheric Drops and Particles: Concentrations, (Limited) Speciation, and Chemical Transformations

NASA Astrophysics Data System (ADS)

Anastasio, C.; Zhang, Q.

2003-12-01

While quite a bit is known of the concentrations, speciation, and chemistry of inorganic forms of nitrogen in the atmosphere, the same cannot be said for organic forms. Despite this, there is growing evidence that organic N (ON) is ubiquitous in the atmosphere, especially in atmospheric condensed phases such as fog/cloud drops and aerosol particles. Although the major compounds that make up organic N are generally unknown, as are the sources of these compounds, it is clear that there are significant fluxes of ON between the atmosphere and ecosystems. It also appears that organic N can have significant effects in both spheres. The goal of our recent work in this area has been to better describe the atmospheric component of the biogeochemistry of organic nitrogen. Based on particle, gas, and fogwater samples from Northern California we have made three major findings: 1) Organic N represents a significant component, approximately 20%, of the total atmospheric N loading in these samples. This is broadly consistent with studies from other locations. 2) Amino compounds, primarily as combined amino acids, account for approximately 20% of the measured ON in our condensed phase samples. Given the properties of amino acids, these compounds could significantly affect the chemical and physical properties of atmospheric particles. 3) Organic nitrogen in atmospheric particles and drops is transformed to inorganic forms - primarily ammonium, nitrate, and nitrogen oxides (NOx) - during exposure to sunlight and/or ozone. These chemical reactions likely increase the bioavailability of the condensed phase nitrogen pool and enhance its biological effects after deposition to ecosystems.

Optimization and characterization of condensation nucleation light scattering detection coupled with supercritical fluid chromatography

NASA Astrophysics Data System (ADS)

Yang, Shaoping

This dissertation is an investigation of two aspects of coupling condensation nucleation light scattering detection (CNLSD) with supercritical fluid chromatography (SFC). In the first part, it was demonstrated that CNLSD was compatible with packed column SFC using either pure CO2 or organic solvent modified CO2 as mobile phases. Factors which were expected to affect the interface between SFC and CNLSD were optimized for the detector to reach low detection limits. With SFC using pure CO2 as mobile phase, the detection limit of CNLSD with SFC was observed to be at low nanogram levels, which was at the same level of flame ionization detection (FID) coupled with SFC. For SFC using modified CO2 as mobile phase, detection limits at the picogram level were observed for CNLSD at optimal conditions, which were at least ten times lower than those reached by evaporative light scattering detection. In the second part, particle size distributions of aerosols produced from rapid expansion of supercritical solutions were measured with a scanning mobility particle sizer. The effect of the factors, which were investigated in the first part for their effects on signal intensities and signal to noise ratios (S/N), on particle size distributions (PSDs) of both analyte and background were investigated. Whenever possible, both particle sizes and particle number obtained from PSDs were used to explain the optimization results. In general, PSD data support the observations made in the first part. The detection limits of CNLSD obtained were much higher than predicted. PSDs did not provide direct explanation of this problem. The amount of analyte deposited in the transport tubing, evaporated to gas phase, and condensed to form particles was determined experimentally. Almost no analyte was found in the gas phase. Less than 3% was found in the particle forms. The vast majority of analyte was lost in the transport tubing, especially in the short distance after supercritical fluid expansion. A mechanism was proposed to explain the loss of analyte in the transport tubing.

Single-particle spectral functions in the normal phase of a strongly attractive Bose-Fermi mixture

NASA Astrophysics Data System (ADS)

Fratini, E.; Pieri, P.

2013-07-01

We calculate the single-particle spectral functions and quasiparticle dispersions for a Bose-Fermi mixture when the boson-fermion attraction is sufficiently strong to suppress completely the condensation of bosons at zero temperature. Within a T-matrix diagrammatic approach, we vary the boson-fermion attraction from the critical value where the boson condensate first disappears to the strongly attractive (molecular) regime and study the effect of both mass and density imbalance on the spectral weights and dispersions. An interesting spectrum of particle-hole excitations mixing two different Fermi surfaces is found. These unconventional excitations could be produced and explored experimentally with radio-frequency spectroscopy.

Preparation of amino acid nanoparticles at varying saturation conditions in an aerosol flow reactor

NASA Astrophysics Data System (ADS)

Raula, Janne; Lehtimäki, Matti; Karppinen, Maarit; Antopolsky, Maxim; Jiang, Hua; Rahikkala, Antti; Kauppinen, Esko I.

2012-07-01

Nanoparticle formation of five amino acids, glycine, l-proline, l-valine, l-phenylalanine, and l-leucine was studied. The aim was to explore factors determining nanoparticle formation and crystallinity. The amino acid nanoparticles have been prepared at different saturation conditions in the aerosol reactor. In a condensed state, the particles were formed by droplet drying. The raise in temperature induced the sublimation of amino acids from the aerosol particles. The amino acid vapor was condensed by physical vapor deposition in a rapid cooling process. The diffusion coefficients and nucleation rates of amino acids have been calculated to understand particle formation. Upon the vapor deposition, amino acids formed crystalline nanoparticles except in the case l-phenylalanine according to X-ray diffraction. The crystal polymorph of glycine in the nanoparticles depended on the applied reactor temperature. The preference of crystallographic orientation varied in both the particle formations from condensed and vapor phase. l-Valine, l-phenylalanine, and l-leucine formed leafy-looking particles. These results could be utilized in the fabrication of nano-sized asperities on drug particle surfaces to reduce forces between particles and accordingly increase particle dispersion in dry powder inhalers.

Ice Nucleation of Soot Particles in the Cirrus Regime: Is Pore Condensation and Freezing Relevant for Soot?

NASA Astrophysics Data System (ADS)

Kanji, Z. A.; Mahrt, F.; David, R.; Marcolli, C.; Lohmann, U.; Fahrni, J.; Brühwiler, D.

2017-12-01

Heterogeneous ice nucleation (HIN) onto soot particles from previous studies have produced inconsistent results of temperature and relative humidity conditions required for freezing depending on the source of soot particle investigated. The ability of soot to act as HIN depended on the type of soot and size of particle. Often homogenous freezing conditions or water saturation conditions were required to freeze soot particles, rendering HIN irrelevant. Using synthesised mesoporous silica particles, we show pore condensation and freezing works with experiments performed in the Zurich Ice Nucleation Chamber (ZINC). By testing a variety of soot particles in parallel in the Horizontal Ice Nucleation Chamber (HINC), we suggest that previously observed HIN on soot particles is not the responsible mechanism for ice formation. Laboratory generated CAST brown and black soot, commercially available soot and acid treated soot were investigated for their ice nucleation abilities in the mixed-phase and cirrus cloud temperature regimes. No heterogeneous ice nucleation activity is inferred at T > -38 °C (mixed-phase cloud regime), however depending on particle size and soot type, HIN was observed for T < -38 °C (cirrus could regime). Nevertheless, we question if this is caused by a heterogeneous phase change due the presence of a so called active site or due to pore-condensation of water as predicted by the inverse Kelvin effect followed by homogeneous nucleation of ice in the pores or cavities that are ubiquitous in soot particles between the primary spherules. The ability of some particles to freeze at lower relative humidity compared to others demonstrates why hydrophobicity plays a role in ice nucleation, i.e. controlling the conditions at which these cavities fill with water. Thus for more hydrophobic particles pore filling occurs at higher relative humidity, and therefore freezing of pore water and ice crystal growth. Future work focusses on testing the cloud processing ability of soot particles and water adsorption isotherms of the different soot samples to support the hydrophobicity inferences from the ice nucleation results.

Development and evaluation of the aerosol dynamic and gas phase chemistry model ADCHEM

NASA Astrophysics Data System (ADS)

Roldin, P.; Swietlicki, E.; Schurgers, G.; Arneth, A.; Lehtinen, K. E. J.; Boy, M.; Kulmala, M.

2010-08-01

The aim of this work was to develop a model ideally suited for detailed studies on aerosol dynamics, gas and particle phase chemistry within urban plumes, from local scale (1×1 km2) to regional or global scale. This article describes and evaluates the trajectory model for Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer (ADCHEM), which has been developed and used at Lund University since 2007. The model treats both vertical and horizontal dispersion perpendicular to an air mass trajectory (2-space dimensions), which is not treated in Lagrangian box-models (0-space dimensions). The Lagrangian approach enables a more detailed representation of the aerosol dynamics, gas and particle phase chemistry and a finer spatial and temporal resolution compared to that of available regional 3D-CTMs. These features make it among others ideally suited for urban plume studies. The aerosol dynamics model includes Brownian coagulation, dry deposition, wet deposition, in-cloud processing, condensation, evaporation, primary particle emissions and homogeneous nucleation. The gas phase chemistry model calculates the gas phase concentrations of 63 different species, using 119 different chemical reactions. Daily isoprene and monoterpene emissions from European forests were simulated separately with the vegetation model LPJ-GUESS, and included as input to ADCHEM. ADCHEM was used to simulate the ageing of the urban plumes from the city of Malmö in Southern Sweden (280 000 inhabitants). Several sensitivity tests were performed concerning the number of size bins, size structure method, coupled or uncoupled condensation, the volatility basis set (VBS) or traditional 2-product model for secondary organic aerosol formation, different aerosol dynamic processes and vertical and horizontal mixing. The simulations show that the full-stationary size structure gives accurate results with little numerical diffusion when more than 50 size bins are used between 1.5 and 2500 nm, while the moving-center method is preferable when only a few size bins are selected. The particle number size distribution in the center of the urban plume from Malmö is mainly affected by dry deposition, coagulation and condensation, and is relatively insensitive to moderate variations in the vertical and horizontal mixing, as long as the mixing height is relatively uniform. The modeled PM2.5 was dominated by organics, nitrate, sulfate and ammonium. If treating the condensation of HNO3 and NH3 as a coupled process (pH independent) the model gave lower nitrate PM2.5 values than if considering uncoupled condensation. However, both methods gave similar and significant temporal variation in the particulate nitrate content, primarily due to fluctuation in the relative humidity.

Vapor Wall Deposition in Chambers: Theoretical Considerations

NASA Astrophysics Data System (ADS)

McVay, R.; Cappa, C. D.; Seinfeld, J.

2014-12-01

In order to constrain the effects of vapor wall deposition on measured secondary organic aerosol (SOA) yields in laboratory chambers, Zhang et al. (2014) varied the seed aerosol surface area in toluene oxidation and observed a clear increase in the SOA yield with increasing seed surface area. Using a coupled vapor-particle dynamics model, we examine the extent to which this increase is the result of vapor wall deposition versus kinetic limitations arising from imperfect accommodation of organic species into the particle phase. We show that a seed surface area dependence of the SOA yield is present only when condensation of vapors onto particles is kinetically limited. The existence of kinetic limitation can be predicted by comparing the characteristic timescales of gas-phase reaction, vapor wall deposition, and gas-particle equilibration. The gas-particle equilibration timescale depends on the gas-particle accommodation coefficient αp. Regardless of the extent of kinetic limitation, vapor wall deposition depresses the SOA yield from that in its absence since vapor molecules that might otherwise condense on particles deposit on the walls. To accurately extrapolate chamber-derived yields to atmospheric conditions, both vapor wall deposition and kinetic limitations must be taken into account.

Gas uptake and chemical aging of semisolid organic aerosol particles

PubMed Central

Shiraiwa, Manabu; Ammann, Markus; Koop, Thomas; Pöschl, Ulrich

2011-01-01

Organic substances can adopt an amorphous solid or semisolid state, influencing the rate of heterogeneous reactions and multiphase processes in atmospheric aerosols. Here we demonstrate how molecular diffusion in the condensed phase affects the gas uptake and chemical transformation of semisolid organic particles. Flow tube experiments show that the ozone uptake and oxidative aging of amorphous protein is kinetically limited by bulk diffusion. The reactive gas uptake exhibits a pronounced increase with relative humidity, which can be explained by a decrease of viscosity and increase of diffusivity due to hygroscopic water uptake transforming the amorphous organic matrix from a glassy to a semisolid state (moisture-induced phase transition). The reaction rate depends on the condensed phase diffusion coefficients of both the oxidant and the organic reactant molecules, which can be described by a kinetic multilayer flux model but not by the traditional resistor model approach of multiphase chemistry. The chemical lifetime of reactive compounds in atmospheric particles can increase from seconds to days as the rate of diffusion in semisolid phases can decrease by multiple orders of magnitude in response to low temperature or low relative humidity. The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate. PMID:21690350

Characterization of On-Orbit U.S. Lab Condensate Vacuum Venting

NASA Astrophysics Data System (ADS)

Schmidl, W. D.; Alred, J. A.; Mikatarian, R.; Soares, C.; Miles, E.

2002-01-01

The venting of liquid streams into a vacuum has been studied extensively for many years. An experiment was performed aboard the International Space Station (ISS) to video tape the U.S. Lab's condensate venting event with cameras located on the Space Station Remote Manipulator System (SSRMS). Images of the vent plume were acquired close to both the port and starboard vent nozzles. The imaging started with a wider view and then zoomed in closer before the shutdown phase of the vent event occurred. The objective of this experiment was to extend our understanding of the properties of venting liquids into space. Data from the video images were analyzed to obtain the approximate cone angle encompassing the core of the vent plume. The condensate vent plume was characterized as having three phases, a startup phase, a nominal phase, and a shutdown phase. The startup phase consisted of the initial period when the vent first started and the liquid first entered the heated line. The nominal phase was the period when the majority of the liquid was vented. The shutdown phase occurs close to the end of the vent event. The shutdown phase was further divided into two parts, the shutdown initial phase, and a later shutdown sputtering phase. The shutdown initial phase occurs when gas becomes entrained in the condensate liquid being vented. The sputtering phase occurred after the vent valve was closed, and the liquid/ice in the line was removed by continuing to heat the line to bake it out. It was determined that the ice particles were ejected at higher angles, but lower velocities, during the startup and shutdown phases. The number and velocities of ice particles ejected outside of the core region, during the startup, initial shutdown and shutdown sputtering phases were determined. The core of liquid ejected during the startup and shutdown phases was contained within a half cone angle of less than 60 degrees. The startup phase took approximately 36 seconds, the shutdown initial phase took approximately 22 seconds, and the shutdown sputtering phase took approximately 32 seconds. Results from the experiment were correlated with the Boeing ISS vent plume model.

Bose-Einstein condensation of photons in a 'white-wall' photon box

NASA Astrophysics Data System (ADS)

Klärs, Jan; Schmitt, Julian; Vewinger, Frank; Weitz, Martin

2011-01-01

Bose-Einstein condensation, the macroscopic ground state occupation of a system of bosonic particles below a critical temperature, has been observed in cold atomic gases and solid-state physics quasiparticles. In contrast, photons do not show this phase transition usually, because in Planck's blackbody radiation the particle number is not conserved and at low temperature the photons disappear in the walls of the system. Here we report on the realization of a photon Bose-Einstein condensate in a dye-filled optical microcavity, which acts as a "white-wall" photon box. The cavity mirrors provide a trapping potential and a non-vanishing effective photon mass, making the system formally equivalent to a two-dimensional gas of trapped massive bosons. Thermalization of the photon gas is reached in a number conserving way by multiple scattering off the dye molecules. Signatures for a BEC upon increased photon density are: a spectral distribution that shows Bose-Einstein distributed photon energies with a macroscopically populated peak on top of a broad thermal wing, the observed threshold of the phase transition showing the predicted absolute value and scaling with resonator geometry, and condensation appearing at the trap centre even for a spatially displaced pump spot.

Controllable synthesis of iron oxide nanoparticles in porous NaCl matrix

NASA Astrophysics Data System (ADS)

Kurapov, Yury A.; E Litvin, Stanislav; Romanenko, Sergey M.; Didikin, Gennadii G.; Oranskaya, Elena I.

2017-03-01

The paper gives the results of studying the structure of porous condensates of Fe + NaCl composition, chemical and phase compositions and dimensions of nanoparticles produced from the vapor phase by EB-PVD. Iron nanoparticles at fast removal from the vacuum oxidize in air and possess significant sorption capacity relative to oxygen and moisture. At heating in air, reduction of porous condensate weight occurs right to the temperature of 650 °C, primarily, due to desorption of physically sorbed moisture. Final oxidation of Fe3O4 to Fe2O3 proceeds in the range of 380 °C-650 °C, due to the remaining fraction of physically adsorbed oxygen. At iron concentrations of up to 10-15 at%, condensate sorption capacity is markedly increased with increase of iron concentration, i.e. of the quantity of fine particles. Increase of condensation temperature is accompanied by increase of nanoparticle size, resulting in a considerable reduction of the total area of nanoparticle surface, and, hence of their sorption capacity. In addition to condensation temperature, the size and phase composition of nanoparticles can also be controlled by heat treatment of initial condensate, produced at low condensation temperatures. Magnetite nanoparticles can be transferred into stable colloid systems.

Correlations for Vapor Nucleating Critical Embryo Parameters

NASA Astrophysics Data System (ADS)

Magnusson, Lars-Erik; Koropchak, John A.; Anisimov, Michael P.; Poznjakovskiy, Valeriy M.; de la Mora, Juan Fernandez

2003-12-01

Condensation nucleation light scattering detection in principle works by converting the effluent of the chromatographic separation into an aerosol and then selectively evaporating the mobile phase, leaving less volatile analytes and nonvolatile impurities as dry aerosol particles. The dry particles produced are then exposed to an environment that is saturated with the vapors of an organic solvent (commonly n-butanol). The blend of aerosol particles and organic vapor is then cooled so that conditions of vapor supersaturation are achieved. In principle, the vapor then condenses onto the dry particles, growing each particle (ideally) from as small as a few nanometers in diameter into a droplet with a diameter up to about 10 μm. The grown droplets are then passed through a beam of light, and the light scattered by the droplets is detected and used as the detector response. This growth and detection step is generally carried out using commercial continuous-flow condensation nucleus counters. In the present research, the possibility of using other fluids than the commonly used n-butanol is investigated. The Kelvin equation and the Nucleation theorem [Anisimov et al. (1978)] are used to evaluate a range of fluids for efficacy of growing small particles by condensation nucleation. Using the available experimental data on vapor nucleation, the correlations of Kelvin diameters (the critical embryo sizes) and the bulk surface tension with dielectric constants of working liquids are found. A simple method for choosing the most efficient fluid, within a class of fluids, for growth of small particles is suggested.

Revealing the dark side of a bright exciton–polariton condensate

PubMed Central

Ménard, J. -M.; Poellmann, C.; Porer, M.; Leierseder, U.; Galopin, E.; Lemaître, A.; Amo, A.; Bloch, J.; Huber, R.

2014-01-01

Condensation of bosons causes spectacular phenomena such as superfluidity or superconductivity. Understanding the nature of the condensed particles is crucial for active control of such quantum phases. Fascinating possibilities emerge from condensates of light–matter-coupled excitations, such as exciton–polaritons, photons hybridized with hydrogen-like bound electron–hole pairs. So far, only the photon component has been resolved, while even the mere existence of excitons in the condensed regime has been challenged. Here we trace the matter component of polariton condensates by monitoring intra-excitonic terahertz transitions. We study how a reservoir of optically dark excitons forms and feeds the degenerate state. Unlike atomic gases, the atom-like transition in excitons is dramatically renormalized on macroscopic ground state population. Our results establish fundamental differences between polariton condensation and photon lasing and open possibilities for coherent control of condensates. PMID:25115964

Detuning-Controlled Internal Oscillations in an Exciton-Polariton Condensate

NASA Astrophysics Data System (ADS)

Voronova, N. S.; Elistratov, A. A.; Lozovik, Yu. E.

2015-10-01

We theoretically analyze exciton-photon oscillatory dynamics within a homogenous polariton gas in the presence of energy detuning between the cavity and quantum well modes. Whereas pure Rabi oscillations consist of the particle exchange between the photon and exciton states in the polariton system without any oscillations of the phases of the two subcondensates, we demonstrate that any nonzero detuning results in oscillations of the relative phase of the photon and exciton macroscopic wave functions. Different initial conditions reveal a variety of behaviors of the relative phase between the two condensates, and a crossover from Rabi-like to Josephson-like oscillations is predicted.

Computational techniques for flows with finite-rate condensation

NASA Technical Reports Server (NTRS)

Candler, Graham V.

1993-01-01

A computational method to simulate the inviscid two-dimensional flow of a two-phase fluid was developed. This computational technique treats the gas phase and each of a prescribed number of particle sizes as separate fluids which are allowed to interact with one another. Thus, each particle-size class is allowed to move through the fluid at its own velocity at each point in the flow field. Mass, momentum, and energy are exchanged between each particle class and the gas phase. It is assumed that the particles do not collide with one another, so that there is no inter-particle exchange of momentum and energy. However, the particles are allowed to grow, and therefore, they may change from one size class to another. Appropriate rates of mass, momentum, and energy exchange between the gas and particle phases and between the different particle classes were developed. A numerical method was developed for use with this equation set. Several test cases were computed and show qualitative agreement with previous calculations.

A Systematic Evaluation of the Extent of Photochemical Processing in Different Types of Secondary Organic Aerosols in the Aqueous Phase

NASA Astrophysics Data System (ADS)

Romonosky, D.; Lee, H.; Epstein, S. A.; Nizkorodov, S.; Laskin, J.; Laskin, A.

2013-12-01

A significant fraction of atmospheric organic compounds are predominantly found in condensed phases, such as organic phase in aerosol particles or aqueous phase in cloud droplets. The oxidation of VOCs followed by the condensation of products into particles was thought to be the main mechanism of organic aerosol (OA) formation. However, in the last several years, scientists have realized that a large fraction, if not the majority of organic particles, is produced through cloud and fog photochemical processes. Many of these organic compounds are photolabile, and can degrade through direct photolysis or indirect photooxidation processes on time scales that are comparable to the typical lifetimes of droplets (hours) and particles (days). We previously reported that compounds in secondary organic aerosol (SOA) from ozonolysis of d-limonene efficiently photodegrade in both organic (Walser et al., 2007) and aqueous phases (Bateman et al., 2011). Significant photolysis was also observed in an aqueous extract of SOA from high-NOx photooxidation of isoprene (Nguyen et al., 2012). More recent experiments studying the response to irradiation of complex aqueous mixtures (as opposed to solutions of isolated compounds) found surprising resilience to photodegradation in aqueous extracts of SOA prepared by photooxidation of alpha-pinene (Romonosky et al., unpublished). We present a systematic investigation of the extent of photochemical processing in different types of SOA from various biogenic and anthropogenic precursors. Chamber- or flowtube-generated SOA is collected on an inert substrate, extracted in a methanol/water solution (70:30), photolyzed in the aqueous solution, and the extent of change in the molecular level composition of the material is assessed with high-resolution mass spectrometry (HR-MS). The outcome of this study will be improved understanding of the role of condensed-phase photochemistry in chemical aging of aerosol particles and cloud droplets. Bateman et al. Photolytic processing of secondary organic aerosols dissolved in cloud droplets. Phys. Chem. Chem. Phys. 2011, 13, 12199. Nguyen et al. Direct aqueous photochemistry of isoprene high-NOx secondary organic aerosol. Phys. Chem. Chem. Phys. 2012, 14, 9702. Walser et al. Photochemical aging of secondary organic aerosol particles generated from the oxidation of d-limonene. J. Phys. Chem. A 2007, 111, 1907.

Theory of Fermi Liquid with Flat Bands

NASA Astrophysics Data System (ADS)

Khodel, V. A.

2018-04-01

A self-consistent theory of Fermi systems hosting flat bands is developed. Compared with an original model of fermion condensation, its key point consists in proper accounting for mixing between condensate and non-condensate degrees of freedom that leads to formation of a non-BCS gap Υ (p) in the single-particle spectrum. The results obtained explain: (1) the two-gap structure of spectra of single-particle excitations of electron systems of copper oxides, revealed in ARPES studies, (2) the role of violation of the topological stability of the Landau state in the arrangement of the T-x phase diagram of this family of high-T_c superconductors, (3) the topological nature of a metal-insulator transition, discovered in homogeneous two-dimensional low-density electron liquid of MOSFETs more than 20 years ago.

The track structure in condensed matter

NASA Astrophysics Data System (ADS)

Kaplan, I. G.

1995-11-01

The physical stage of track formation in a condensed phase is discussed. For interaction of charged particles with condensed molecular media its most important specific features are: (a) the continuous oscillator strength distribution with the broak peak in the energy range 21-22 eV attributed to the collective plasmon-type state; (b) the lowering of ionization potential compared to a gas phase. These specific features must be taken into account for simulation of track structures. The great difference in mass and charge for a electron and heavy ions cause a qualitative difference in their track structures. We analyse the structure of heavy ion tracks and prove the impossibility to use the LET as a universal characteristic for the radiation action of different ions.

Density functional description of size-dependent effects at nucleation on neutral and charged nanoparticles

NASA Astrophysics Data System (ADS)

Shchekin, Alexander K.; Lebedeva, Tatiana S.

2017-03-01

A numerical study of size-dependent effects in the thermodynamics of a small droplet formed around a solid nanoparticle has been performed within the square-gradient density functional theory. The Lennard-Jones fluid with the Carnahan-Starling model for the hard-sphere contribution to intermolecular interaction in liquid and vapor phases and interfaces has been used for description of the condensate. The intermolecular forces between the solid core and condensate molecules have been taken into account with the help of the Lennard-Jones part of the total molecular potential of the core. The influence of the electric charge of the particle has been considered under assumption of the central Coulomb potential in the medium with dielectric permittivity depending on local condensate density. The condensate density profiles and equimolecular radii for equilibrium droplets at different values of the condensate chemical potential have been computed in the cases of an uncharged solid core with the molecular potential, a charged core without molecular potential, and a core with joint action of the Coulomb and molecular potentials. The appearance of stable equilibrium droplets even in the absence of the electric charge has been commented. As a next step, the capillary, disjoining pressure, and electrostatic contributions to the condensate chemical potential have been considered and compared with the predictions of classical thermodynamics in a wide range of values of the droplet and the particle equimolecular radii. With the help of the found dependence of the condensate chemical potential in droplet on the droplet size, the activation barrier for nucleation on uncharged and charged particles has been computed as a function of the vapor supersaturation. Finally, the work of droplet formation and the work of wetting the particle have been found as functions of the droplet size.

Finite Density Condensation and Scattering Data: A Study in ϕ4 Lattice Field Theory

NASA Astrophysics Data System (ADS)

Gattringer, Christof; Giuliani, Mario; Orasch, Oliver

2018-06-01

We study the quantum field theory of a charged ϕ4 field in lattice regularization at finite density and low temperature in 2 and 4 dimensions with the goal of analyzing the connection of condensation phenomena to scattering data in a nonperturbative way. The sign problem of the theory at nonzero chemical potential μ is overcome by using a worldline representation for the Monte Carlo simulation. At low temperature we study the particle number as a function of μ and observe the steps for 1-, 2-, and 3-particle condensation. We determine the corresponding critical values μncrit , n =1 , 2, 3 and analyze their dependence on the spatial extent L of the lattice. Linear combinations of the μncrit give the interaction energies in the 2- and 3-particle sectors and their dependence on L is related to scattering data by Lüscher's formula and its generalizations to three particles. For two dimensions we determine the scattering phase shift and for four dimensions the scattering length. We cross-check our results with a determination of the mass and the 2- and 3-particle energies from conventional 2-, 4-, and 6-point correlators at zero chemical potential. The letter demonstrates that the physics of condensation at finite density and low temperature is closely related to scattering data of a quantum field theory.

Tracking Water Diffusion Fronts in a Highly Viscous Aerosol Particle

NASA Astrophysics Data System (ADS)

Bastelberger, Sandra; Krieger, Ulrich; Peter, Thomas

2016-04-01

Field measurements indicate that atmospheric secondary aerosol particles can be present in a highly viscous, glassy state [1]. In contrast to liquid state particles, the gas phase equilibration is kinetically limited and governed by condensed phase diffusion. In recent water diffusion experiments on highly viscous single aerosol particles levitated in an electrodynamic balance (EDB) we observed a characteristic shift behavior of the Mie whispering gallery modes (WGM) indicative of the changing radial structure of the particle, thus providing us with an experimental method to track the diffusion process inside the particle. When a highly viscous, homogeneous particle is exposed to an abrupt increase in relative humidity, the rapid gas phase diffusion and strong concentration dependence of the diffusion coefficient in the condensed phase lead to extremely steep water concentration gradients inside the particle, reminiscent of diffusion fronts. The resulting quasi step-like concentration profile motivates the introduction of a simple core-shell model describing the morphology of the non-equilibrium particle during humidification. The subsequent particle growth and reduction of the shell refractive index can be observed as red and blueshift behavior of the WGM, respectively. The shift pattern can be attributed to a core-shell radius ratio and particle radius derived from model calculations [2]. If supplemented with growth information obtained from the WGM redshift and thermodynamic equilibrium data, we can infer a comprehensive picture of the time evolution of the diffusion fronts in the framework of our core-shell model. The measured time dependent concentration profile is then compared with simulations solving the non-linear diffusion equation [3] [1] Virtanen, A., et al., Nature, 467, 824-827, 2010 [2] Kaiser, T., Schweiger, G., Computers in Physics, Vol. 7, No. 6, 682-686, Nov/Dec 1993 [3] Zobrist, B., Soonsin, V., Luo, B.P., Peter, T. et al., Phys. Chem. Chem. Phys., 13,3514-3526, 2011

Calculation of the Rate of Combustion of a Metallized Composite Solid Propellant with Allowance for the Size Distribution of Agglomerates

NASA Astrophysics Data System (ADS)

Poryazov, V. A.; Krainov, A. Yu.

2016-05-01

A physicomathematical model of combustion of a metallized composite solid propellant based on ammonium perchlorate has been presented. The model takes account of the thermal effect of decomposition of a condensed phase (c phase), convection, diffusion, the exothermal chemical reaction in a gas phase, the heating and combustion of aluminum particles in the gas flow, and the velocity lag of the particles behind the gas. The influence of the granulometric composition of aluminum particles escaping from the combustion surface on the linear rate of combustion has been investigated. It has been shown that information not only on the kinetics of chemical reactions in the gas phase, but also on the granulometric composition of aluminum particles escaping from the surface of the c phase into the gas, is of importance for determination of the linear rate of combustion.

Some experiments related to L-star instability in rocket motors

NASA Technical Reports Server (NTRS)

Kumar, R. N.; Mcnamara, R. P.

1973-01-01

The influence of condensed phase heterogeneity on the L-star instability of nonmetallized AP/PBAN propellants is explored using four propellants (with monomodal AP particle distributions having 50 per cent weight average points at 11, 39.5, 175, and 350 microns). An economical firing program is used. One-dimensional nature of the Helmholtz mode and the complex nature of the chuff mode are revealed through color movies. The stability boundary on the L-star pressure plot is found to be parabolic. Frequency correlations and many other features reveal the important role of condensed phase details in propellant combustion.

One-Pot Synthesis of GeAs Ultrafine Particles from Coal Fly Ash by Vacuum Dynamic Flash Reduction and Inert Gas Condensation.

PubMed

Zhang, Lingen; Xu, Zhenming

2017-06-16

Ge-monopnictides (GeAs) plays critical role in high-tech industry, especially in the field of advanced optical devices and infrared. As a secondary material, coal fly ash could be further recycled to retrieve germanium and prepare GeAs material with high added values. Hence, the aim of this paper is to propose a one-pot synthesis that uses vacuum flash reduction and inert-gas consolidation method to prepare GeAs ultrafine particles. Germanium in coal fly ash can be successfully recycled; simultaneously, GeAs ultrafine particles were prepared. Separation principle and feasibility of this process was discussed. Temperature, carrier gas flow rate and system pressure were the major factors on formation, morphology and distribution of particle size of GeAs ultrafine particles. A three steps synthetic mechanism was clarified, namely, thermal rupture of coal fly ash and release of GeO 2 and As 2 O 3 , the gas-solid phase reaction of GeO 2 , As 2 O 3 and coke to generate metallic Ge and As in vacuum flash reduction. Meantime, GeAs were produced in the gas phase reaction. Finally, GeAs ultrafine particles were obtained by carrier gas condensation. In short, this research developed a practical and environment-friendly one-pot synthesis to recycle germanium in coal fly ash and prepare GeAs ultrafine particles with high added values.

Rotational fluxons of Bose-Einstein condensates in coplanar double-ring traps

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brand, J.; Institute of Natural Sciences, Massey University; Haigh, T. J.

Rotational analogs to magnetic fluxons in conventional Josephson junctions are predicted to emerge in the ground state of rotating tunnel-coupled annular Bose-Einstein condensates (BECs). Such topological condensate-phase structures can be manipulated by external potentials. We determine conditions for observing macroscopic quantum tunneling of a fluxon. Rotational fluxons in double-ring BECs can be created, manipulated, and controlled by external potentials in different ways than is possible in the solid-state system, thus rendering them a promising candidate system for studying and utilizing quantum properties of collective many-particle degrees of freedom.

Analysis of nanoscale two-phase flow of argon using molecular dynamics

NASA Astrophysics Data System (ADS)

Verma, Abhishek Kumar; Kumar, Rakesh

2014-12-01

Two phase flows through micro and nanochannels have attracted a lot of attention because of their immense applicability to many advanced fields such as MEMS/NEMS, electronic cooling, bioengineering etc. In this work, a molecular dynamics simulation method is employed to study the condensation process of superheated argon vapor force driven flow through a nanochannel combining fluid flow and heat transfer. A simple and effective particle insertion method is proposed to model phase change of argon based on non-periodic boundary conditions in the simulation domain. Starting from a crystalline solid wall of channel, the condensation process evolves from a transient unsteady state where we study the influence of different wall temperatures and fluid wall interactions on interfacial and heat transport properties of two phase flows. Subsequently, we analyzed transient temperature, density and velocity fields across the channel and their dependency on varying wall temperature and fluid wall interaction, after a dynamic equilibrium is achieved in phase transition. Quasi-steady nonequilibrium temperature profile, heat flux and interfacial thermal resistance were analyzed. The results demonstrate that the molecular dynamics method, with the proposed particle insertion method, effectively solves unsteady nonequilibrium two phase flows at nanoscale resolutions whose interphase between liquid and vapor phase is typically of the order of a few molecular diameters.

Controlling particle properties in {{YBa}}_{2}{{Cu}}_{3}{{\\rm{O}}}_{7-\\delta } nanocomposites by combining PLD with an inert gas condensation system

NASA Astrophysics Data System (ADS)

Sparing, M.; Reich, E.; Hänisch, J.; Gottschall, T.; Hühne, R.; Fähler, S.; Rellinghaus, B.; Schultz, L.; Holzapfel, B.

2017-10-01

The critical current density {J}{{c}} in {{YBa}}2{{Cu}}3{{{O}}}7-δ thin films, which limits their application in external magnetic fields, can be enhanced by the introduction of artificial pinning centers such as non-superconducting nanoparticles inducing additional defects and local strain in the superconducting matrix. To understand the correlation between superconductivity, defect structures and particles, a controlled integration of particles with adjustable properties is essential. A powerful technique for the growth of isolated nanoparticles in the range of 10 nm is dc-magnetron sputtering in an inert gas flow. The inert gas condensation (IGC) of particles allows for an independent control of both the particle diameter distribution and the areal density. We report on the integration of such gas-phase-condensed {{HfO}}2 nanoparticles into pulsed laser deposited (PLD) {{YBa}}2{{Cu}}3{{{O}}}7-δ thin film multilayers with a combined PLD-IGC system. The particles and the structure of the multilayers are analyzed by transmission electron microscopy on cross-sectional FIB lamellae. As a result of the IGC particle implementation, randomly as well as biaxially oriented {{BaHfO}}3 precipitates are formed in the {{YBa}}2{{Cu}}3{{{O}}}7-δ thin films. With as few as three interlayers of nanoparticles, the pinning force density is enhanced in the low-field region.

Laboratory Studies of the Optical Properties and Condensation Processes of Cosmic Dust Grains

NASA Technical Reports Server (NTRS)

Abbas, M. M.; Craven, P. D.; Spann, J. F.; Tankosic, D.; LeClair, A.; West, E.; Sheldon, R.; Witherow, W. K.; Gallagher, D. L.; Adrian, M. L.

2002-01-01

A laboratory facility for conducting a variety of experiments on single isolated dust particles of astrophysical interest levitated in an electrodynamics balance has been developed at NASA/Marshall Space Flight Center. The objective of the research is to employ this experimental technique for studies of the physical and optical properties of individual cosmic dust grains of 0.1-100 micron size in controlled pressure/temperatures environments simulating astrophysical conditions. The physical and optical properties of the analogs of interstellar and interplanetary dust grains of known composition and size distribution will be investigated by this facility. In particular, we will carry out three classes of experiments to study the micro-physics of cosmic dust grains. (1) Charge characteristics of micron size single dust grains to determine the photoelectric efficiencies, yields, and equilibrium potentials when exposed to UV radiation. (2) Infrared optical properties of dust particles (extinction coefficients and scattering phase functions) in the 1-30 micron region using infrared diode lasers and measuring the scattered radiation. (3) Condensation experiments to investigate the condensation of volatile gases on colder nucleated particles in dense interstellar clouds and lower planetary atmospheres. The condensation experiments will involve levitated nucleus dust grains of known composition and initial mass (or m/q ratio), cooled to a temperature and pressure (or scaled pressure) simulating the astrophysical conditions, and injection of a volatile gas at a higher temperature from a controlled port. The increase in the mass due to condensation on the particle will be monitored as a function of the dust particle temperature and the partial pressure of the injected volatile gas. The measured data will permit determination of the sticking coefficients of volatile gases and growth rates of dust particles of astrophysical interest. Some preliminary results based on measurements of photoelectric emission and radiation pressure on single isolated 0.2 to 6.6 micron size silica particles exposed to UV radiation at 120-200 nm and green laser light at 532 nm are presented.

Analytical solutions for coagulation and condensation kinetics of composite particles

NASA Astrophysics Data System (ADS)

Piskunov, Vladimir N.

2013-04-01

The processes of composite particles formation consisting of a mixture of different materials are essential for many practical problems: for analysis of the consequences of accidental releases in atmosphere; for simulation of precipitation formation in clouds; for description of multi-phase processes in chemical reactors and industrial facilities. Computer codes developed for numerical simulation of these processes require optimization of computational methods and verification of numerical programs. Kinetic equations of composite particle formation are given in this work in a concise form (impurity integrated). Coagulation, condensation and external sources associated with nucleation are taken into account. Analytical solutions were obtained in a number of model cases. The general laws for fraction redistribution of impurities were defined. The results can be applied to develop numerical algorithms considerably reducing the simulation effort, as well as to verify the numerical programs for calculation of the formation kinetics of composite particles in the problems of practical importance.

Formation of double front detonations of a condensed-phase explosive with powdered aluminium

NASA Astrophysics Data System (ADS)

Kim, Wuhyun; Gwak, Min-cheol; Yoh, Jack J.

2018-03-01

The performance characteristics of aluminised high explosive are considered by varying the aluminium (Al) mass fraction in a hybrid non-ideal detonation model. Since the time scales of the characteristic induction and combustion of high explosives and Al particles differ, the process of energy release behind the leading detonation wave front occurs over an extended period of time. Two cardinal observations are reported: a decrease in detonation velocity with an increase in Al mass fraction and a double front detonation (DFD) feature when anaerobic Al reaction occurs behind the front. In order to simulate the performance characteristics due to the varying Al mass fraction, the tetrahexamine tetranitramine (HMX) is considered as a base high explosive when formulating the multiphase conservation laws of mass, momentum, and energy exchanges between particles and HMX product gases. While experimental studies have been reported on the effect of Al mass fraction on both gas-phase and solid-phase detonations, the numerical investigations have been limited to only gas-phase detonation for the varying Al particles in the mixture. In the current study, a two-phase model is utilised for understanding the volumetric effects of Al mass fraction in condensed phase detonations. A series of unconfined and confined rate sticks are considered for characterising the performance of aluminised HMX with a maximum Al mass fraction of 50%. The simulated results are compared with the experimental data for 5-25% mass fractions, and the higher mass fraction behaviours are consistent with the experimental observations.

Water interactions with condensed organic phases: a combined experimental and theoretical study of molecular-level processes

NASA Astrophysics Data System (ADS)

Johansson, Sofia M.; Kong, Xiangrui; Thomson, Erik S.; Papagiannakopoulos, Panos; Pettersson, Jan B. C.; Lovrić, Josip; Toubin, Céline

2016-04-01

Water uptake on aerosol particles modifies their chemistry and microphysics with important implications for air quality and climate. A large fraction of the atmospheric aerosol consists of organic aerosol particles or inorganic particles with condensed organic components. Here, we combine laboratory studies using the environmental molecular beam (EMB) method1 with molecular dynamics (MD) simulations to characterize water interactions with organic surfaces in detail. The over-arching aim is to characterize the mechanisms that govern water uptake, in order to guide the development of physics-based models to be used in atmospheric modelling. The EMB method enables molecular level studies of interactions between gases and volatile surfaces at near ambient pressure,1 and the technique may provide information about collision dynamics, surface and bulk accommodation, desorption and diffusion kinetics. Molecular dynamics simulations provide complementary information about the collision dynamics and initial interactions between gas molecules and the condensed phase. Here, we focus on water interactions with condensed alcohol phases that serve as highly simplified proxies for systems in the environment. Gas-surface collisions are in general found to be highly inelastic and result in efficient surface accommodation of water molecules. As a consequence, surface accommodation of water can be safely assumed to be close to unity under typical ambient conditions. Bulk accommodation is inefficient on solid alcohol and the condensed materials appear to produce hydrophobic surface structures, with limited opportunities for adsorbed water to form hydrogen bonds with surface molecules. Accommodation is significantly more efficient on the dynamic liquid alcohol surfaces. The results for n-butanol (BuOH) are particularly intriguing where substantial changes in water accommodation taking place over a 10 K interval below and above the BuOH melting point.2 The governing mechanisms for the observed water accommodation are discussed based on the combined EMB and MD results. The studies illustrate that the detailed surface properties of the condensed organic phase may substantially modify water uptake, with potential implications for the properties and action of aerosols and clouds in the Earth system. References: 1. X.R. Kong, E. S. Thomson, P. Papagiannakopoulos, S.M. Johansson, and J.B.C. Pettersson, Water Accommodation on Ice and Organic Surfaces: Insights from Environmental Molecular Beam Experiments. J. Phys. Chem. B 118 (2014) 13378-13386. 2. P. Papagiannakopoulos, X. Kong, E. S. Thomson, N. Marković, and J. B. C. Pettersson, Surface Transformations and Water Uptake on Liquid and Solid Butanol near the Melting Temperature. J. Phys. Chem. C 117 (2013) 6678-6685.

Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch

NASA Astrophysics Data System (ADS)

Cozic, J.; Verheggen, B.; Mertes, S.; Connolly, P.; Bower, K.; Petzold, A.; Baltensperger, U.; Weingartner, E.

2007-04-01

The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (droplets and ice particles) as well as interstitial (unactivated) aerosol particles; an interstitial inlet which collected only interstitial aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the condensed phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~5-10% in mixed-phase clouds with IMF>0.2. This can be explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.

Aging fingerprints in combustion particles

NASA Astrophysics Data System (ADS)

Zelenay, V.; Mooser, R.; Tritscher, T.; Křepelová, A.; Heringa, M. F.; Chirico, R.; Prévôt, A. S. H.; Weingartner, E.; Baltensperger, U.; Dommen, J.; Watts, B.; Raabe, J.; Huthwelker, T.; Ammann, M.

2011-05-01

Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing is still a subject of discussion. In this work, soot particles emitted from two different cars, a EURO 2 transporter, a EURO 3 passenger vehicle, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using x-ray absorption spectroscopy and scanning electron microscopy. Comparison of the spectra from the unprocessed and aged soot particles revealed changes in the carbon functional group content, such as that of carboxylic carbon, which can be ascribed to both the condensation of secondary organic compounds on the soot particles and oxidation of primary soot particles upon photochemical aging. Changes in the morphology and size of the single soot particles were also observed upon aging. Furthermore, we show that the soot particles take up water in humid environments and that their water uptake capacity increases with photochemical aging.

OH-initiated Aging of Biomass Burning Aerosol during FIREX

NASA Astrophysics Data System (ADS)

Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

2017-12-01

Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

Fast production of Bose-Einstein condensates of metastable helium

NASA Astrophysics Data System (ADS)

Bouton, Q.; Chang, R.; Hoendervanger, A. L.; Nogrette, F.; Aspect, A.; Westbrook, C. I.; Clément, D.

2015-06-01

We report on the Bose-Einstein condensation of metastable 4He atoms using a hybrid approach, consisting of a magnetic quadrupole and an optical dipole trap. In our setup we cross the phase transition with 2 ×106 atoms, and we obtain pure condensates of 5 ×105 atoms in the optical trap. This approach to cooling 4He provides enhanced cycle stability, large optical access to the atoms and results in the production of a condensate every 6 s—a factor 2 faster than the state of the art. This speed-up will significantly reduce the data acquisition time needed for the measurement of many particle correlations, made possible by the ability of metastable helium atoms to be detected individually.

Self-Consistency of the Theory of Elementary Stage Rates of Reversible Processes and the Equilibrium Distribution of Reaction Mixture Components

NASA Astrophysics Data System (ADS)

Tovbin, Yu. K.

2018-06-01

An analysis is presented of one of the key concepts of physical chemistry of condensed phases: the theory self-consistency in describing the rates of elementary stages of reversible processes and the equilibrium distribution of components in a reaction mixture. It posits that by equating the rates of forward and backward reactions, we must obtain the same equation for the equilibrium distribution of reaction mixture components, which follows directly from deducing the equation in equilibrium theory. Ideal reaction systems always have this property, since the theory is of a one-particle character. Problems arise in considering interparticle interactions responsible for the nonideal behavior of real systems. The Eyring and Temkin approaches to describing nonideal reaction systems are compared. Conditions for the self-consistency of the theory for mono- and bimolecular processes in different types of interparticle potentials, the degree of deviation from the equilibrium state, allowing for the internal motions of molecules in condensed phases, and the electronic polarization of the reagent environment are considered within the lattice gas model. The inapplicability of the concept of an activated complex coefficient for reaching self-consistency is demonstrated. It is also shown that one-particle approximations for considering intermolecular interactions do not provide a theory of self-consistency for condensed phases. We must at a minimum consider short-range order correlations.

Particles from a Diesel ship engine: Mixing state on the nano scale and cloud condensation abilities

NASA Astrophysics Data System (ADS)

Lieke, K. I.; Rosenørn, T.; Fuglsang, K.; Frederiksen, T.; Butcher, A. C.; King, S. M.; Bilde, M.

2012-04-01

Transport by ship plays an important role in global logistics. Current international policy initiatives by the International Maritime Organization (IMO) are taken to reduce emissions from ship propulsion systems (NO and SO, primarily). However, particulate emissions (e.g. soot) from ships are yet not regulated by legislations. To date, there is still a lack of knowledge regarding the global and local effects of the particulate matter emitted from ships at sea. Particles may influence the climate through their direct effects (scattering and absorption of long and shortwave radiation) and indirectly through formation of clouds. Many studies have been carried out estimating the mass and particle number from ship emissions (e.g. Petzold et al. 2008), many of them in test rig studies (e.g. Kasper et al. 2007). It is shown that particulate emissions vary with engine load and chemical composition of fuels. Only a few studies have been carried out to characterize the chemical composition and cloud-nucleating ability of the particulate matter (e.g. Corbett et al. 1997). In most cases, the cloud-nucleating ability of emission particles is estimated from number size distribution. We applied measurements to characterize particulate emissions from a MAN B&W Low Speed engine on test bed. A unique data set was obtained through the use of a scanning mobility particle sizing system (SMPS), combined with a cloud condensation nucleus (CCN) counter and a thermodenuder - all behind a dilution system. In addition, impactor samples were taken on nickel grids with carbon foil for use in an electron microscope (EM) to characterize the mineral phase and mixing state of the particles. The engine was operated at a series of different load conditions and an exhaust gas recirculation (EGR) system was applied. Measurements were carried out before and after the EGR system respectively. Our observations show significant changes in number size distribution and CCN activity with varying conditions. Results of transmission electron microscopy revealed salt condensates of nanometer size attached to soot particles. High resolution structural analysis of single particles shows that three different phases (graphitic soot, crystalline salt and amorphous condensed organic matter) may be present in the same particle volume. A closure between CCN activation curves, EM samples, and SMPS size distribution will be presented and used to identify climate active parts in single particles. ACKNOWLEDGEMENTS We thank the Danish Agency for Science, Technology and Innovation for support through the NaKIM project (www.nakim.dk).

Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

DOE PAGES

Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

2017-02-04

Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

Particulate matter in exhaled breath condensate: A promising indicator of environmental conditions

NASA Astrophysics Data System (ADS)

Pinheiro, Teresa; Alexandra Barreiros, M.; Alves, Luis C.; Felix, Pedro M.; Franco, Cristiana; Sousa, Joana; Almeida, S. M.

2011-10-01

Assessing the retention of aerosol particles in the human lung, one of the most important pathways of absorption, is a demanding issue. At present, there is no direct biomarker of exposure for the respiratory system. The collection of exhaled breath condensate (EBC) constitutes a new non-invasive method for sampling from the lung. However, the heterogeneity of the sample due to particulate matter suspended in the condensed phase may influence the quality of analytical results in occupational assessments. The main objective of the study was to confirm the presence of particulate matter in the condensate, to investigate how large the particles in suspension could be and to determine their elemental contents relative to those of EBC matrix. This paper reports on preliminary nuclear microprobe data of particulate matter in EBC. The sizes and the elemental contents of particles suspended in EBC of workers of a lead processing industry and in EBC of non-exposed individuals were inspected. Results demonstrated that EBC of workers contain large aerosol particles, isolated and in agglomerates, contrasting with non-exposed individuals. The particles contained high concentrations of Cl, Ca, Zn and Pb that are elements associated to the production process. These elements were also present in the EBC matrix although in much lower levels, suggesting that a fraction of the inhaled particulate matter was solubilised or their size-ranges were below the nuclear microprobe resolution. Therefore, the morphological characterization of individual particles achieved with nuclear microprobe techniques helped describing EBC constituents in detail, to comprehend their origin and enabled to delineate methodological procedures that can be recommended in occupational assessments. These aspects are critical to the validation of EBC as a biomarker of exposure to metals for the respiratory system.

Statistical properties and condensate fluctuation of attractive Bose gas with finite number of particles

NASA Astrophysics Data System (ADS)

Bera, Sangita; Lekala, Mantile Leslie; Chakrabarti, Barnali; Bhattacharyya, Satadal; Rampho, Gaotsiwe Joel

2017-09-01

'We study the condensate fluctuation and several statistics of weakly interacting attractive Bose gas of 7 Li atoms in harmonic trap. Using exact recursion relation we calculate canonical ensemble partition function and study the thermal evolution of the condensate. As 7 Li condensate is associated with collapse, the number of condensate atom is truly finite and it facilitates to study the condensate in mesoscopic region. Being highly correlated, we utilize the two-body correlated basis function to get the many-body effective potential which is further used to calculate the energy levels. Taking van der Waals interaction as interatomic interaction we calculate several quantities like condensate fraction N, root-mean-square fluctuation δn0 and different orders of central moments. We observe the effect of finite size on the calculation of condensate fluctuations and the effect of attractive interaction over the noninteracting limit. We observe the depletion of the condensate with increase in temperature. The calculated moments nicely exhibit the mesoscopic effect. The sharp fall in the root-mean-square fluctuation near the critical point signifies the possibility of phase transition.

Chiral organosilica particles and their use as inducers of conformational deracemization of liquid crystal phases

NASA Astrophysics Data System (ADS)

Cohen, Orit; Ferris, Andrew J.; Adkins, Raymond; Lemieux, Robert P.; Avnir, David; Gelman, Dmitri; Rosenblatt, Charles

2018-03-01

Chiral organosilica particles of size ∼200 nm were synthesized from an enantio-pure multi-armed chiral D-maltose organosilane precursor in the absence of co-condensation with an achiral monomer. Two distinct experiments were performed to demonstrate the particles' ability to induce conformational deracemization of a host liquid crystal. The first involves an electric field-induced tilt of the liquid crystal director in the deracemized smectic-A phase. The other involves domain wall curvature separating left- and right-handed liquid crystal helical pitch domains imposed by the cells' substrates. The results demonstrate unequivocally that enantio-pure organosilica nanoparticles can be synthesized and can induce chirality in a host.

Solubility and Phase Behavior of CL20 and RDX in Supercritical Carbon Dioxide

DTIC Science & Technology

2004-12-01

with Enhanced mass transfer (SAS-EMTM) are potential green processes for producing ultrafine particles . In these processes, the material to be...particulated will be dissolved (solubilized) into an environmentally benign solvent such as supercritical carbon dioxide and then condensed to ultrafine ... particles by reducing the pressure and temperature of the mixture. Theoretical and/or predictive models are required for process simulation and to

Experimental investigation of aerosol composition and growth rates

NASA Astrophysics Data System (ADS)

Wimmer, Daniela; Winkler, Paul; Kulmala, Markku; Petäjä, Tuukka

2017-04-01

Atmospheric aerosol particles have relevant influence on human lives. Human health is affected, as by breathing in the aerosol particles, they deposit in the lungs causing various health problems. Also they interfere indirectly and directly with sunlight, which affects the climate on Earth. Primary aerosol particles originate for example from anthropogenic sources, such as Diesel cars or natural sources such as dessert dust. Secondary aerosol particles are formed via condensation of low volatile gas phase compounds. First, small clusters consisting of a few gas molecules only are formed, which can then grow to bigger aerosol particles. These then form seeds for cloud droplets. The chemical composition of the cloud particles determines whether the cloud absorbs or scatters sunlight more. Intensive experimental and theoretical work has been put into understanding the details of the initial processes leading to the natural formation of these secondary aerosol particles. According to modelling studies, aerosol particles formed via the nucleation process are responsible for about 50% of the global cloud condensation nuclei concentration. With currently used methods, the chemical composition of small molecular clusters (up to 2nm in diameter) can be resolved. Also standard methods to determine aerosol particle composition at sizes >10 nm are available. Within this project, the aerosol particle composition in the 2-4 nm size range will be investigated experimentally. The setup will consist of a combination of an electrical method that allows determine the electrical mobility of the particles which then can be converted to a diameter. By letting the charged particles travel through a changing electrical field, they travel at different speeds according to their mobility. That allows to particles with certain mobilities, which then can be converted to a diameter. After the size selection, the particles are counted by means of optical detection. Condensation particle counters (CPCs) grow the particles internally, after which they are detected optically. By changing the condensing liquid, depending on the aerosol particle composition, they are activated differently. By combining the electrical size selection with CPCs with different liquids, information about particle composition can be determined. The project includes laboratory studies and field measurements in different locations (one rural site and two urban sites). I wish to acknowledge the Austrian Science Fund (FWF; Grant No J3951 - N36).

Composition, morphology, and growth of clusters in a gas of particles with random interactions

NASA Astrophysics Data System (ADS)

Azizi, Itay; Rabin, Yitzhak

2018-03-01

We use Langevin dynamics simulations to study the growth kinetics and the steady-state properties of condensed clusters in a dilute two-dimensional system of particles that are all different (APD) in the sense that each particle is characterized by a randomly chosen interaction parameter. The growth exponents, the transition temperatures, and the steady-state properties of the clusters and of the surrounding gas phase are obtained and compared with those of one-component systems. We investigate the fractionation phenomenon, i.e., how particles of different identities are distributed between the coexisting mother (gas) and daughter (clusters) phases. We study the local organization of particles inside clusters, according to their identity—neighbourhood identity ordering (NIO)—and compare the results with those of previous studies of NIO in dense APD systems.

The equations of motion for moist atmospheric air

NASA Astrophysics Data System (ADS)

Makarieva, Anastassia M.; Gorshkov, Victor G.; Nefiodov, Andrei V.; Sheil, Douglas; Nobre, Antonio Donato; Bunyard, Peter; Nobre, Paulo; Li, Bai-Lian

2017-07-01

How phase transitions affect the motion of moist atmospheric air remains controversial. In the early 2000s two distinct differential equations of motion were proposed. Besides their contrasting formulations for the acceleration of condensate, the equations differ concerning the presence/absence of a term equal to the rate of phase transitions multiplied by the difference in velocity between condensate and air. This term was interpreted in the literature as the "reactive motion" associated with condensation. The reasoning behind this reactive motion was that when water vapor condenses and droplets begin to fall the remaining gas must move upward to conserve momentum. Here we show that the two contrasting formulations imply distinct assumptions about how gaseous air and condensate particles interact. We show that these assumptions cannot be simultaneously applicable to condensation and evaporation. Reactive motion leading to an upward acceleration of air during condensation does not exist. The reactive motion term can be justified for evaporation only; it describes the downward acceleration of air. We emphasize the difference between the equations of motion (i.e., equations constraining velocity) and those constraining momentum (i.e., equations of motion and continuity combined). We show that owing to the imprecise nature of the continuity equations, consideration of total momentum can be misleading and that this led to the reactive motion controversy. Finally, we provide a revised and generally applicable equation for the motion of moist air.

Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer

NASA Astrophysics Data System (ADS)

Murray, B. J.; Haddrell, A. E.; Peppe, S.; Davies, J. F.; Reid, J. P.; O'Sullivan, D.; Price, H. C.; Kumar, R.; Saunders, R. W.; Plane, J. M. C.; Umo, N. S.; Wilson, T. W.

2012-09-01

Iodine oxide particles are known to nucleate in the marine boundary layer where gas phase molecular iodine and organoiodine species are produced by macroalgae. These ultra-fine particles may then grow through the condensation of other materials to sizes where they may serve as cloud condensation nuclei. There has been some debate over the chemical identity of the initially nucleated particles. In laboratory simulations, hygroscopic measurements have been used to infer that they are composed of insoluble I2O4, while elemental analysis of laboratory generated particles suggests soluble I2O5 or its hydrated form iodic acid, HIO3 (I2O5·H2O). In this paper we explore the response of super-micron sized aqueous iodic acid solution droplets to varying humidity using both Raman microscopy and single particle electrodynamic traps. These measurements reveal that the propensity of an iodic acid solution droplet to crystallise is negligible on drying to ~0% relative humidity (RH). On applying mechanical pressure to these droplets they shatter in a manner consistent with an ultra-viscous liquid or a brittle glass. Water retention in amorphous material at low RH is important for understanding the hygroscopic growth of aerosol particles and uptake of other condensable material. Subsequent water uptake between 10 and 20% RH causes their viscosity to reduce sufficiently that the cracked droplets flow and merge. The persistence of iodic acid solution in an amorphous state, rather than a crystalline state, suggests they will more readily accommodate other condensable material and are therefore more likely to grow to sizes where they may serve as cloud condensation nuclei. On increasing the humidity to ~90% the mass of the droplets only increases by ~20% with a corresponding increase in radius of only 6%, which is remarkably small for a highly soluble material. We suggest that the small growth factor of aqueous iodic acid solution droplets is consistent with the small aerosol growth factors observed in previous experiments.

Magnetofermionic condensate in two dimensions

PubMed Central

Kulik, L. V.; Zhuravlev, A. S.; Dickmann, S.; Gorbunov, A. V.; Timofeev, V. B.; Kukushkin, I. V.; Schmult, S.

2016-01-01

Coherent condensate states of particles obeying either Bose or Fermi statistics are in the focus of interest in modern physics. Here we report on condensation of collective excitations with Bose statistics, cyclotron magnetoexcitons, in a high-mobility two-dimensional electron system in a magnetic field. At low temperatures, the dense non-equilibrium ensemble of long-lived triplet magnetoexcitons exhibits both a drastic reduction in the viscosity and a steep enhancement in the response to the external electromagnetic field. The observed effects are related to formation of a super-absorbing state interacting coherently with the electromagnetic field. Simultaneously, the electrons below the Fermi level form a super-emitting state. The effects are explicable from the viewpoint of a coherent condensate phase in a non-equilibrium system of two-dimensional fermions with a fully quantized energy spectrum. The condensation occurs in the space of vectors of magnetic translations, a property providing a completely new landscape for future physical investigations. PMID:27848969

Communications: Complete description of re-entrant phase behavior in a charge variable colloidal model system.

PubMed

Wette, Patrick; Klassen, Ina; Holland-Moritz, Dirk; Herlach, Dieter M; Schöpe, Hans Joachim; Lorenz, Nina; Reiber, Holger; Palberg, Thomas; Roth, Stephan V

2010-04-07

In titration experiments with NaOH, we have determined the full phase diagram of charged colloidal spheres in dependence on the particle density n, the particle effective charge Z(eff) and the concentration of screening electrolyte c using microscopy, light and ultrasmall angle x-ray scattering (USAXS). For sufficiently large n, the system crystallizes upon increasing Z(eff) at constant c and melts upon increasing c at only slightly altered Z(eff). In contrast to earlier work, equilibrium phase boundaries are consistent with a universal melting line prediction from computer simulation, if the elasticity effective charge is used. This charge accounts for both counterion condensation and many-body effects.

A kinetic model for heterogeneous condensation of vapor on an insoluble spherical particle.

PubMed

Luo, Xisheng; Fan, Yu; Qin, Fenghua; Gui, Huaqiao; Liu, Jianguo

2014-01-14

A kinetic model is developed to describe the heterogeneous condensation of vapor on an insoluble spherical particle. This new model considers two mechanisms of cluster growth: direct addition of water molecules from the vapor and surface diffusion of adsorbed water molecules on the particle. The effect of line tension is also included in the model. For the first time, the exact expression of evaporation coefficient is derived for heterogeneous condensation of vapor on an insoluble spherical particle by using the detailed balance. The obtained expression of evaporation coefficient is proved to be also correct in the homogeneous condensation and the heterogeneous condensation on a planar solid surface. The contributions of the two mechanisms to heterogeneous condensation including the effect of line tension are evaluated and analysed. It is found that the cluster growth via surface diffusion of adsorbed water molecules on the particle is more important than the direct addition from the vapor. As an example of our model applications, the growth rate of the cap shaped droplet on the insoluble spherical particle is derived. Our evaluation shows that the growth rate of droplet in heterogeneous condensation is larger than that in homogeneous condensation. These results indicate that an explicit kinetic model is benefit to the study of heterogeneous condensation on an insoluble spherical particle.

BES-HEP Connections: Common Problems in Condensed Matter and High Energy Physics, Round Table Discussion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fradkin, Eduardo; Maldacena, Juan; Chatterjee, Lali

2015-02-02

On February 2, 2015 the Offices of High Energy Physics (HEP) and Basic Energy Sciences (BES) convened a Round Table discussion among a group of physicists on ‘Common Problems in Condensed Matter and High Energy Physics’. This was motivated by the realization that both fields deal with quantum many body problems, share many of the same challenges, use quantum field theoretical approaches and have productively interacted in the past. The meeting brought together physicists with intersecting interests to explore recent developments and identify possible areas of collaboration.... Several topics were identified as offering great opportunity for discovery and advancement inmore » both condensed matter physics and particle physics research. These included topological phases of matter, the use of entanglement as a tool to study nontrivial quantum systems in condensed matter and gravity, the gauge-gravity duality, non-Fermi liquids, the interplay of transport and anomalies, and strongly interacting disordered systems. Many of the condensed matter problems are realizable in laboratory experiments, where new methods beyond the usual quasi-particle approximation are needed to explain the observed exotic and anomalous results. Tools and techniques such as lattice gauge theories, numerical simulations of many-body systems, and tensor networks are seen as valuable to both communities and will likely benefit from collaborative development.« less

Chiral liquid phase of simple quantum magnets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhentao; Feiguin, Adrian E.; Zhu, Wei

2017-11-07

We study a T=0 quantum phase transition between a quantum paramagnetic state and a magnetically ordered state for a spin S=1 XXZ Heisenberg antiferromagnet on a two-dimensional triangular lattice. The transition is induced by an easy-plane single-ion anisotropy D. At the mean-field level, the system undergoes a direct transition at a critical D=D c between a paramagnetic state at D>D c and an ordered state with broken U(1) symmetry at Dc. We show that beyond mean field the phase diagram is very different and includes an intermediate, partially ordered chiral liquid phase. Specifically, we find that inside the paramagnetic phasemore » the Ising (J z) component of the Heisenberg exchange binds magnons into a two-particle bound state with zero total momentum and spin. This bound state condenses at D>D c, before single-particle excitations become unstable, and gives rise to a chiral liquid phase, which spontaneously breaks spatial inversion symmetry, but leaves the spin-rotational U(1) and time-reversal symmetries intact. This chiral liquid phase is characterized by a finite vector chirality without long-range dipolar magnetic order. In our analytical treatment, the chiral phase appears for arbitrarily small J z because the magnon-magnon attraction becomes singular near the single-magnon condensation transition. This phase exists in a finite range of D and transforms into the magnetically ordered state at some Dc. In conclusion, we corroborate our analytic treatment with numerical density matrix renormalization group calculations.« less

Metal Sulfide Cluster Complexes and their Biogeochemical Importance in the Environment

NASA Astrophysics Data System (ADS)

Luther, George W.; Rickard, David T.

2005-10-01

Aqueous clusters of FeS, ZnS and CuS constitute a major fraction of the dissolved metal load in anoxic oceanic, sedimentary, freshwater and deep ocean vent environments. Their ubiquity explains how metals are transported in anoxic environmental systems. Thermodynamic and kinetic considerations show that they have high stability in oxic aqueous environments, and are also a significant fraction of the total metal load in oxic river waters. Molecular modeling indicates that the clusters are very similar to the basic structural elements of the first condensed phase forming from aqueous solutions in the Fe-S, Zn-S and Cu-S systems. The structure of the first condensed phase is determined by the structure of the cluster in solution. This provides an alternative explanation of Ostwald's Rule, where the most soluble, metastable phases form before the stable phases. For example, in the case of FeS, we showed that the first condensed phase is nanoparticulate, metastable mackinawite with a particle size of 2 nm consisting of about 150 FeS subunits, representing the end of a continuum between aqueous FeS clusters and condensed material. These metal sulfide clusters and nanoparticles are significant in biogeochemistry. Metal sulfide clusters reduce sulfide and metal toxicity and help drive ecology. FeS cluster formation drives vent ecology and AgS cluster formation detoxifies Ag in Daphnia magna neonates. We also note a new reaction between FeS and DNA and discuss the potential role of FeS clusters in denaturing DNA.

Temperature dependence of the coherence in polariton condensates

NASA Astrophysics Data System (ADS)

Rozas, E.; Martín, M. D.; Tejedor, C.; Viña, L.; Deligeorgis, G.; Hatzopoulos, Z.; Savvidis, P. G.

2018-02-01

We present a time-resolved experimental study of the temperature effect on the coherence of traveling polariton condensates. The simultaneous detection of their emission both in real and reciprocal space allows us to fully monitor the condensates' dynamics. We obtain fringes in reciprocal space as a result of the interference between polariton wave packets (WPs) traveling with the same speed. The periodicity of these fringes is inversely proportional to the spatial distance between the interfering WPs. In a similar fashion, we obtain interference fringes in real space when WPs traveling in opposite directions meet. The visibility of both real- and reciprocal-space interference fringes rapidly decreases with increasing temperature and vanishes. A theoretical description of the phase transition, considering the coexistence of condensed and noncondensed particles, for an out-of-equilibrium condensate such as ours is still missing, yet a comparison with theories developed for atomic condensates allows us to infer a critical temperature for the BEC-like transition when the visibility goes to zero.

Machine learning phases of matter

NASA Astrophysics Data System (ADS)

Carrasquilla, Juan; Melko, Roger G.

2017-02-01

Condensed-matter physics is the study of the collective behaviour of infinitely complex assemblies of electrons, nuclei, magnetic moments, atoms or qubits. This complexity is reflected in the size of the state space, which grows exponentially with the number of particles, reminiscent of the `curse of dimensionality' commonly encountered in machine learning. Despite this curse, the machine learning community has developed techniques with remarkable abilities to recognize, classify, and characterize complex sets of data. Here, we show that modern machine learning architectures, such as fully connected and convolutional neural networks, can identify phases and phase transitions in a variety of condensed-matter Hamiltonians. Readily programmable through modern software libraries, neural networks can be trained to detect multiple types of order parameter, as well as highly non-trivial states with no conventional order, directly from raw state configurations sampled with Monte Carlo.

Cluster model studies of anion and molecular specificities via electrospray ionization photoelectron spectroscopy

DOE PAGES

Wang, Xue -Bin

2017-01-06

Ion specificity, a widely observed macroscopic phenomenon in condensed phases and at interfaces, is essentially a fundamental chemical physical issue. We have been investigating such effects using cluster models in an “atom-by-atom” and “molecule-by-molecule” fashion not possible with condensed-phase methods. We use electrospray ionization (ESI) to generate molecular and ionic clusters to simulate key molecular entities involved in local binding regions, and characterize them employing negative ion photoelectron spectroscopy (NIPES). Inter- and intramolecular interactions and binding configurations are directly obtained as functions of cluster size and composition, providing insightful molecular-level description and characterization over the local active sites that playmore » crucial roles in determining solution chemistry and condensed phase phenomena. Finally, the topics covered in this article are relevant to a wide scope of research fields ranging from ion specific effects in electrolyte solutions, ion selectivity/recognition in normal functioning of life, to molecular specificity in aerosol particle formation, as well as in rational material design and synthesis.« less

Vortex and half-vortex dynamics in a nonlinear spinor quantum fluid

PubMed Central

Dominici, Lorenzo; Dagvadorj, Galbadrakh; Fellows, Jonathan M.; Ballarini, Dario; De Giorgi, Milena; Marchetti, Francesca M.; Piccirillo, Bruno; Marrucci, Lorenzo; Bramati, Alberto; Gigli, Giuseppe; Szymańska, Marzena H.; Sanvitto, Daniele

2015-01-01

Vortices are archetypal objects that recur in the universe across the scale of complexity, from subatomic particles to galaxies and black holes. Their appearance is connected with spontaneous symmetry breaking and phase transitions. In Bose-Einstein condensates and superfluids, vortices are both point-like and quantized quasiparticles. We use a two-dimensional (2D) fluid of polaritons, bosonic particles constituted by hybrid photonic and electronic oscillations, to study quantum vortex dynamics. Polaritons benefit from easiness of wave function phase detection, a spinor nature sustaining half-integer vorticity, strong nonlinearity, and tuning of the background disorder. We can directly generate by resonant pulsed excitations a polariton condensate carrying either a full or half-integer vortex as initial condition and follow their coherent evolution using ultrafast imaging on the picosecond scale. The observations highlight a rich phenomenology, such as the spiraling of the half-vortex and the joint path of the twin charges of a full vortex, until the moment of their splitting. Furthermore, we observe the ordered branching into newly generated secondary couples, associated with the breaking of radial and azimuthal symmetries. This allows us to devise the interplay of nonlinearity and sample disorder in shaping the fluid and driving the vortex dynamics. In addition, our observations suggest that phase singularities may be seen as fundamental particles whose quantized events span from pair creation and recombination to 2D+t topological vortex strings. PMID:26665174

Vortex and half-vortex dynamics in a nonlinear spinor quantum fluid.

PubMed

Dominici, Lorenzo; Dagvadorj, Galbadrakh; Fellows, Jonathan M; Ballarini, Dario; De Giorgi, Milena; Marchetti, Francesca M; Piccirillo, Bruno; Marrucci, Lorenzo; Bramati, Alberto; Gigli, Giuseppe; Szymańska, Marzena H; Sanvitto, Daniele

2015-12-01

Vortices are archetypal objects that recur in the universe across the scale of complexity, from subatomic particles to galaxies and black holes. Their appearance is connected with spontaneous symmetry breaking and phase transitions. In Bose-Einstein condensates and superfluids, vortices are both point-like and quantized quasiparticles. We use a two-dimensional (2D) fluid of polaritons, bosonic particles constituted by hybrid photonic and electronic oscillations, to study quantum vortex dynamics. Polaritons benefit from easiness of wave function phase detection, a spinor nature sustaining half-integer vorticity, strong nonlinearity, and tuning of the background disorder. We can directly generate by resonant pulsed excitations a polariton condensate carrying either a full or half-integer vortex as initial condition and follow their coherent evolution using ultrafast imaging on the picosecond scale. The observations highlight a rich phenomenology, such as the spiraling of the half-vortex and the joint path of the twin charges of a full vortex, until the moment of their splitting. Furthermore, we observe the ordered branching into newly generated secondary couples, associated with the breaking of radial and azimuthal symmetries. This allows us to devise the interplay of nonlinearity and sample disorder in shaping the fluid and driving the vortex dynamics. In addition, our observations suggest that phase singularities may be seen as fundamental particles whose quantized events span from pair creation and recombination to 2D+t topological vortex strings.

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

NASA Astrophysics Data System (ADS)

Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lützenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq

2016-04-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, the model predicts that condensational growth contributes to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes predicts the change in particle number concentrations between roadside and urban background within 10 % of that predicted by the fully size-resolved MAFOR model.

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

DOE PAGES

Lienhard, D. M.; Huisman, A. J.; Krieger, U. K.; ...

2015-01-01

New measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH 4HSO 4, raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous icemore » nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.« less

New particle formation leads to cloud dimming

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sullivan, Ryan C.; Crippa, Paola; Matsui, Hitoshi

New particle formation (NPF), nucleation of condensable vapors to the solid or liquid phase, is a significant source of atmospheric aerosol particle number concentrations. With sufficient growth, these nucleated particles may be a significant source of cloud condensation nuclei (CCN), thus altering cloud albedo, structure, and lifetimes, and insolation reaching the Earth's surface. Herein we present one of the first numerical experiments to quantify the impact of NPF on cloud radiative properties that is conducted at a convection permitting resolution and that explicitly simulates cloud droplet number concentrations. Consistent with observations, these simulations suggest that in spring over the Midwesternmore » U.S.A., NPF occurs frequently and on regional scales. However, the simulations suggest that NPF is not associated with enhancement of regional cloud albedos as would be expected from an increase of CCN. These simulations indicate that NPF reduces ambient sulfuric acid concentrations sufficiently to inhibit growth of preexisting particles to CCN sizes. This reduction in CCN-sized particles reduces cloud albedo, resulting in a domain average positive top of atmosphere cloud radiative forcing of 10 W m-2 and up to ~ 50 W m-2 in individual grid cells relative to a simulation in which NPF is excluded.« less

Repulsive four-body interactions of α particles and quasistable nuclear α -particle condensates in heavy self-conjugate nuclei

NASA Astrophysics Data System (ADS)

Bai, Dong; Ren, Zhongzhou

2018-05-01

We study the effects of repulsive four-body interactions of α particles on nuclear α -particle condensates in heavy self-conjugate nuclei using a semianalytic approach, and find that the repulsive four-body interactions could decrease the critical number of α particles, beyond which quasistable α -particle condensate states can no longer exist, even if these four-body interactions make only tiny contributions to the total energy of the Hoyle-like state of 16O. Explicitly, we study eight benchmark parameter sets, and find that the critical number Ncr decreases by |Δ Ncr|˜1 -4 from Ncr˜11 with vanishing four-body interactions. We also discuss the effects of four-body interactions on energies and radii of α -particle condensates. Our study can be useful for future experiments to study α -particle condensates in heavy self-conjugate nuclei. Also, the experimental determination of Ncr will eventually help establish a better understanding on the α -particle interactions, especially the four-body interactions.

A fiery birth of aluminosilica analogs of refractory dust in the upper stratosphere

NASA Astrophysics Data System (ADS)

Rietmeijer, F. J. M.; Ferrari, M.; Della Corte, V.; Rotundi, A.; Palumbo, P.; De Angelis, S.; Galluzzi, V.

2017-11-01

Following a successful dust collection flight in the upper stratosphere our DUSTER (Dust in the Upper Stratosphere Tracking Experiment and Retrieval) made a safe remote landing at its assigned location on Baffin Island during early June 2009. When the balloon payload that included DUSTER was retrieved it was found part of the payload had experienced a lithium-sparked fire while the payload was being dragged across the landing site. In this process the housing of DUSTER had developed a pin-sized hole that allowed smoke of the fire to enter the collector. Numerous smoke particles were found covering both the DUSTER collection and blank collector surfaces an indication that our experiment to collect upper stratospheric dust had failed! Both collector surfaces were covered by numerous carbon smoke and amorphous, aluminosilica nanoparticles. The compositions of vast majority of these aluminosilica nanoparticles, Al2O3 = 49 wt% and SiO2 = 51 wt%, was both surprising and unique because it was an exact match of the Deep Metastable Eutectic (DME) nanoparticles found in vapor phase condensation experiments. These vapor phase condensation experiments were conducted to explore the formation of extraterrestrial dust particles. We are not claiming an extraterrestrial origin for these particles from this DUSTER experiment. We submit that given the appropriate conditions of high temperature alumina and silica vapors and rapid quenching in a contained natural environment, DME aluminosilica nanoparticles will likely condense. This serendipitous result can be used to explore nanoparticle formation inside incandescent clouds associated with bolides and fireballs.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lienhard, D. M.; Huisman, A. J.; Krieger, U. K.

New measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH 4HSO 4, raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous icemore » nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.« less

Instability of Bose-Einstein condensation into the one-particle ground state on quantum graphs under repulsive perturbations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bolte, Jens, E-mail: jens.bolte@rhul.ac.uk; Kerner, Joachim, E-mail: joachim.kerner@fernuni-hagen.de

In this paper we investigate Bose-Einstein condensation into the one-particle ground state in interacting quantum many-particle systems on graphs. We extend previous results obtained for particles on an interval and show that even arbitrarily small repulsive two-particle interactions destroy the condensate in the one-particle ground state present in the non-interacting Bose gas. Our results also cover singular two-particle interactions, such as the well-known Lieb-Liniger model, in the thermodynamic limit.

Tunable Spin-orbit Coupling and Quantum Phase Transition in a Trapped Bose-Einstein Condensate

PubMed Central

Zhang, Yongping; Chen, Gang; Zhang, Chuanwei

2013-01-01

Spin-orbit coupling (SOC), the intrinsic interaction between a particle spin and its motion, is responsible for various important phenomena, ranging from atomic fine structure to topological condensed matter physics. The recent experimental breakthrough on the realization of SOC for ultra-cold atoms provides a completely new platform for exploring spin-orbit coupled superfluid physics. However, the SOC strength in the experiment is not tunable. In this report, we propose a scheme for tuning the SOC strength through a fast and coherent modulation of the laser intensities. We show that the many-body interaction between atoms, together with the tunable SOC, can drive a quantum phase transition (QPT) from spin-balanced to spin-polarized ground states in a harmonic trapped Bose-Einstein condensate (BEC), which resembles the long-sought Dicke QPT. We characterize the QPT using the periods of collective oscillations of the BEC, which show pronounced peaks and damping around the quantum critical point. PMID:23727689

In situ measurements of oxide particles in boron-containing diffusion flames

DOE Office of Scientific and Technical Information (OSTI.GOV)

Turns, S.R.; Funari, M.J.; Khan, A.

1989-02-01

Particulate matter in axisymmetric laminar diffusion flames produced by burning mixtures of either CO and trimethylborate (TMB) or CH/sub 4/ and TMB with air were investigated using laser light-scattering techniques. Boron oxide particle sizes and number densities were determined at various heights in the flames using polarization ratio and relative intensity measurements, respectively. In the CO/TMB flames, two distinct particle-laden regions were found. The first region was located on the rich side of the luminous flame zone and initially appeared as a narrow annulus, which grew in width downstream until the particles filled the core. A second thin annular zonemore » appeared on the air side of the flame zone, starting approximately at the height of the luminous green flame tip and continuing to grow downstream. Particle sizes did not vary significantly with location in the flames, with diameters of approximately 0.09 and 0.15 ..mu..m in the 95% CO/5% TMB and 90% CO/10% TMB flames, respectively. Corresponding peak number densities were approximately 1.5 X 10/sup 10/ and 6 X 10/sup 9/ cm/sup -3/. The CH/sub 4//TMB flames were considerably different than the CO/TMB flames. The presence of significant quantities of water vapor presumably contributed to the formation of HBO/sub 2/(g) in favor of condensed-phase B/sub 2/O/sub 3/. At locations where oxide particles did form, they were closer to the flame centerline than the soot-containing regions. Computations of equilibrium yields of condensed-phase oxide were in qualitative agreement with the experimental results.« less

Quartetting in Nuclear Matter and α Particle Condensation in Nuclear Systems

NASA Astrophysics Data System (ADS)

Röpke, G.; Schuck, P.; Horiuchi, H.; Tohsaki, A.; Funaki, Y.; Yamada, T.

2008-02-01

Alternatively to pairing, four-particle correlations may become of importance for the formation of quantum condensates in nuclear matter. With increasing density, four-particle correlations are suppressed because of Pauli blocking. Signatures of α-like clusters are expected to occur in low-density nuclear systems. The famous Hoyle state (02+ at 7.654 MeV in 12C) is identified as being an almost ideal condensate of three α-particles, hold together only by the Coulomb barrier. It, therefore, has a 8Be-α structure of low density. Transition probability and inelastic form factor together with position and other physical quantities are correctly reproduced without any adjustable parameter from our two parameter wave function of α-particle condensate type. The possibility of the existence of α-particle condensed states in heavier nα nuclei is also discussed.

Deterministic entanglement generation from driving through quantum phase transitions.

PubMed

Luo, Xin-Yu; Zou, Yi-Quan; Wu, Ling-Na; Liu, Qi; Han, Ming-Fei; Tey, Meng Khoon; You, Li

2017-02-10

Many-body entanglement is often created through the system evolution, aided by nonlinear interactions between the constituting particles. These very dynamics, however, can also lead to fluctuations and degradation of the entanglement if the interactions cannot be controlled. Here, we demonstrate near-deterministic generation of an entangled twin-Fock condensate of ~11,000 atoms by driving a arubidium-87 Bose-Einstein condensate undergoing spin mixing through two consecutive quantum phase transitions (QPTs). We directly observe number squeezing of 10.7 ± 0.6 decibels and normalized collective spin length of 0.99 ± 0.01. Together, these observations allow us to infer an entanglement-enhanced phase sensitivity of ~6 decibels beyond the standard quantum limit and an entanglement breadth of ~910 atoms. Our work highlights the power of generating large-scale useful entanglement by taking advantage of the different entanglement landscapes separated by QPTs. Copyright © 2017, American Association for the Advancement of Science.

Enthalpy versus entropy: What drives hard-particle ordering in condensed phases?

DOE PAGES

Anthamatten, Mitchell; Ou, Jane J.; Weinfeld, Jeffrey A.; ...

2016-07-27

In support of mesoscopic-scale materials processing, spontaneous hard-particle ordering has been actively pursued for over a half-century. The generally accepted view that entropy alone can drive hard particle ordering is evaluated. Furthermore, a thermodynamic analysis of hard particle ordering was conducted and shown to agree with existing computations and experiments. Conclusions are that (i) hard particle ordering transitions between states in equilibrium are forbidden at constant volume but are allowed at constant pressure; (ii) spontaneous ordering transitions at constant pressure are driven by enthalpy, and (iii) ordering under constant volume necessarily involves a non-equilibrium initial state which has yet tomore » be rigorously defined.« less

The expanding materials multiverse

NASA Astrophysics Data System (ADS)

Powell, Ben J.

2018-06-01

High-energy physicists are limited to studying a single vacuum and its excitations, the particles of the standard model. For condensed-matter physicists, every new phase of matter brings a new “‘vacuum.” Remarkably, the low-energy excitations of these new vacua can be very different from the individual electrons, protons, and neutrons that constitute the material. The materials multiverse contains universes where the particle-like excitations carry only a fraction of the elementary electronic charge (1), are magnetic monopoles (2), or are their own antiparticles (3). None of these properties have ever been observed in the particles found in free space. Often, emergent gauge fields accompany these “fractionalized” particles (2, 4, 5), just as electromagnetic gauge fields accompany charged particles. On page 1101 of this issue, Hassan et al. (6) provide a glimpse of the emergent behaviors of a putative new phase of matter, the dipole liquid. What particles live in this universe, and what new physics is found in this and neighboring parts of the multiverse?

Spin-Orbit-Coupled Interferometry with Ring-Trapped Bose-Einstein Condensates

NASA Astrophysics Data System (ADS)

Helm, J. L.; Billam, T. P.; Rakonjac, A.; Cornish, S. L.; Gardiner, S. A.

2018-02-01

We propose a method of atom interferometry using a spinor Bose-Einstein condensate with a time-varying magnetic field acting as a coherent beam splitter. Our protocol creates long-lived superpositional counterflow states, which are of fundamental interest and can be made sensitive to both the Sagnac effect and magnetic fields on the sub-μ G scale. We split a ring-trapped condensate, initially in the mf=0 hyperfine state, into superpositions of internal mf=±1 states and condensate superflow, which are spin-orbit coupled. After interrogation, the relative phase accumulation can be inferred from a population transfer to the mf=±1 states. The counterflow generation protocol is adiabatically deterministic and does not rely on coupling to additional optical fields or mechanical stirring techniques. Our protocol can maximize the classical Fisher information for any rotation, magnetic field, or interrogation time and so has the maximum sensitivity available to uncorrelated particles. Precision can increase with the interrogation time and so is limited only by the lifetime of the condensate.

Sensing spontaneous collapse and decoherence with interfering Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Schrinski, Björn; Hornberger, Klaus; Nimmrichter, Stefan

2017-12-01

We study how matter-wave interferometry with Bose-Einstein condensates is affected by hypothetical collapse models and by environmental decoherence processes. Motivated by recent atom fountain experiments with macroscopic arm separations, we focus on the observable signatures of first-order and higher-order coherence for different two-mode superposition states, and on their scaling with particle number. This can be used not only to assess the impact of environmental decoherence on many-body coherence, but also to quantify the extent to which macrorealistic collapse models are ruled out by such experiments. We find that interference fringes of phase-coherently split condensates are most strongly affected by decoherence, whereas the quantum signatures of independent interfering condensates are more immune against macrorealistic collapse. A many-body enhanced decoherence effect beyond the level of a single atom can be probed if higher-order correlations are resolved in the interferogram.

Experimental studies of aerosol- cloud droplet interactions at the puy de Dome observatory (France)

NASA Astrophysics Data System (ADS)

Laj, P.; Dupuy, R.; Sellegri, K.; Pichon, J.; Fournol, J.; Cortes, L.; Preunkert, S.; Legrand, M.

2001-05-01

The interactions between aerosol particles, gases and cloud droplets were studied at the puy de Dome cloud station (France, 1465 a.s.l.) during winter 2000. The partitioning of gas and aerosol species between interstitial and condensed phases is achieved using a series of instrumentation including a newly developed dual counter-flow virtual impactor (CVI)/ Round jet impactor (RJI) system. The RJI/CVI system, coupled with measurement of cloud microphysical properties, provided direct observation of number and mass partitioning of aerosols under different air mass conditions. Preliminary results from this field experiment allowed for the characterization of size segregated chemical composition of CCNs and of interstitial aerosols by means of gravimetric analysis and ion chromatography. It appears that CCNs are clearly enriched in soluble species as respect to interstitial aerosols. We found evidences of limited growth of Ca2+ - rich coarse particles (>1 μm) that did not form droplets larger than the 5 μm CVI cut-off. The number partitioning of aerosol particles between interstitial and condensed phases clearly depends upon cloud microphysics and aerosol properties and therefore undergoes different behaviour according to air mass origin. However, results cannot be fully explained by diffusion growth alone, in particular for high cloud LWC.

Antarctic polar stratospheric aerosols: The roles of nitrates, chlorides and sulfates

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Snetsinger, K. G.; Goodman, J. K.; Ferry, G. V.; Oberbeck, V. R.; Verma, S.; Fong, W.

1988-01-01

Nitric and hydrochloric acids have been postulated to condense in the winter polar stratosphere to become an important component of polar stratospheric clouds. One implication is that the removal of NO(y) from the gas phase by this mechanism allows high Cl(x) concentrations to react with O3, because the formation of ClNO3 is inhibited. Contributions of NO3 and Cl to the stratospheric aerosol were determined during the 1987 Airborne Antarctic Ozone Experiment by testing for the presence of nitrates and chlorides in the condensed phase. Aerosol particles were collected on four 500 micron diameter gold wires, each pretreated differently to give results that were specific to certain physical and chemical aerosol properties. One wire was carbon-coated for concentration and size analyses by scanning electron microscopy; X-ray energy dispersive analyses permitted the detection of S and Cl in individual particles. Three more wires were coated with Nitron, barium chloride and silver nitrate, respectively, to detect nitrate, sulfate and chloride in aerosol particles. All three ions, viz., sulfates, nitrates and chlorides were detected in the Antarctic stratospheric aerosol. In terms of number concentrations, the aerosol was dominated by sulfates, followed by chlorides and nitrates. An inverse linear regression can be established between nitrate concentrations and ozone mixing ratio, and between temperature and nitrates.

Weak lasing in one-dimensional polariton superlattices.

PubMed

Zhang, Long; Xie, Wei; Wang, Jian; Poddubny, Alexander; Lu, Jian; Wang, Yinglei; Gu, Jie; Liu, Wenhui; Xu, Dan; Shen, Xuechu; Rubo, Yuri G; Altshuler, Boris L; Kavokin, Alexey V; Chen, Zhanghai

2015-03-31

Bosons with finite lifetime exhibit condensation and lasing when their influx exceeds the lasing threshold determined by the dissipative losses. In general, different one-particle states decay differently, and the bosons are usually assumed to condense in the state with the longest lifetime. Interaction between the bosons partially neglected by such an assumption can smear the lasing threshold into a threshold domain--a stable lasing many-body state exists within certain intervals of the bosonic influxes. This recently described weak lasing regime is formed by the spontaneously symmetry breaking and phase-locking self-organization of bosonic modes, which results in an essentially many-body state with a stable balance between gains and losses. Here we report, to our knowledge, the first observation of the weak lasing phase in a one-dimensional condensate of exciton-polaritons subject to a periodic potential. Real and reciprocal space photoluminescence images demonstrate that the spatial period of the condensate is twice as large as the period of the underlying periodic potential. These experiments are realized at room temperature in a ZnO microwire deposited on a silicon grating. The period doubling takes place at a critical pumping power, whereas at a lower power polariton emission images have the same periodicity as the grating.

Inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy

NASA Astrophysics Data System (ADS)

Krieger, Ulrich; Lienhard, Daniel; Bastelberger, Sandra; Steimer, Sarah

2014-05-01

Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a "white light" LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary organic aerosol particles, Nature 467, 824-827. [2] B. Zobrist et al. (2011): Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys. 13, 3514-3526. [3] D. L. Bones, J. P. Reid, D. M. Lienhard, and U. K. Krieger (2012): Comparing the mechanism of water condensation and evaporation in glassy aerosol, PNAS 109, 11613-11618. [4] O. Peña and U. Pal (2009): Scattering of electromagnetic radiation by a multilayered sphere, Comput. Phys. Commun. 180, 2348-2354.

Interstellar abundances - Gas and dust

NASA Technical Reports Server (NTRS)

Field, G. B.

1974-01-01

Data on abundances of interstellar atoms, ions and molecules in front of zeta Oph are assembled and analyzed. The gas-phase abundances of at least 11 heavy elements are significantly lower, relative to hydrogen, than in the solar system. The abundance deficiencies of certain elements correlate with the temperatures derived theoretically for particle condensation in stellar atmospheres or nebulae, suggesting that these elements have condensed into dust grains near stars. There is evidence that other elements have accreted onto such grains after their arrival in interstellar space. The extinction spectrum of zeta Oph can be explained qualitatively and, to a degree, quantitatively by dust grains composed of silicates, graphite, silicon carbide, and iron, with mantles composed of complex molecules of H, C, N, and O. This composition is consistent with the observed gas-phase deficiencies.

Nanoparticle growth by particle-phase chemistry

NASA Astrophysics Data System (ADS)

Apsokardu, Michael J.; Johnston, Murray V.

2018-02-01

The ability of particle-phase chemistry to alter the molecular composition and enhance the growth rate of nanoparticles in the 2-100 nm diameter range is investigated through the use of a kinetic growth model. The molecular components included are sulfuric acid, ammonia, water, a non-volatile organic compound, and a semi-volatile organic compound. Molecular composition and growth rate are compared for particles that grow by partitioning alone vs. those that grow by a combination of partitioning and an accretion reaction in the particle phase between two organic molecules. Particle-phase chemistry causes a change in molecular composition that is particle diameter dependent, and when the reaction involves semi-volatile molecules, the particles grow faster than by partitioning alone. These effects are most pronounced for particles larger than about 20 nm in diameter. The modeling results provide a fundamental basis for understanding recent experimental measurements of the molecular composition of secondary organic aerosol showing that accretion reaction product formation increases linearly with increasing aerosol volume-to-surface-area. They also allow initial estimates of the reaction rate constants for these systems. For secondary aerosol produced by either OH oxidation of the cyclic dimethylsiloxane (D5) or ozonolysis of β-pinene, oligomerization rate constants on the order of 10-3 to 10-1 M-1 s-1 are needed to explain the experimental results. These values are consistent with previously measured rate constants for reactions of hydroperoxides and/or peroxyacids in the condensed phase.

Observational Constraints on Modeling Growth and Evaporation Kinetics of Isoprene SOA

NASA Astrophysics Data System (ADS)

Zaveri, R. A.; Shilling, J. E.; Zelenyuk, A.; Liu, J.; Wilson, J. M.; Laskin, A.; Wang, B.; Fast, J. D.; Easter, R. C.; Wang, J.; Kuang, C.; Thornton, J. A.; Setyan, A.; Zhang, Q.; Onasch, T. B.; Worsnop, D. R.

2014-12-01

Isoprene is thought to be a major contributor to the global secondary organic aerosol (SOA) budget, and therefore has the potential to exert a significant influence on earth's climate via aerosol direct and indirect radiative effects. Both aerosol optical and cloud condensation nuclei properties are quite sensitive to aerosol number size distribution, as opposed to the total aerosol mass concentration. Recent studies suggest that SOA particles can be highly viscous, which can affect the kinetics of SOA partitioning and size distribution evolution when the condensing organic vapors are semi-volatile. In this study, we examine the growth kinetics of SOA formed from isoprene photooxidation in the presence of pre-existing Aitken and accumulation mode aerosols in: (a) the ambient atmosphere during the CARES field campaign, and (b) the environmental chamber at PNNL. Each growth episode is analyzed and interpreted with the updated MOSAIC aerosol box model, which performs kinetic gas-particle partitioning of SOA and takes into account diffusion and chemical reaction within the particle phase. The model is initialized with the observed aerosol size distribution and composition at the beginning of the experiment, and the total amount of SOA formed in the model at any given time is constrained by the observed total amount of SOA formed. The variable model parameters include the number of condensing organic species, their gas-phase formation rates, their effective volatilities, and their bulk diffusivities in the Aitken and accumulation modes. The objective of the constrained modeling exercise is then to determine which model configuration is able to best reproduce the observed size distribution evolution, thus providing valuable insights into the possible mechanism of SOA formation. We also examine the evaporation kinetics of size-selected particles formed in the environmental chamber to provide additional constraints on the effective volatility and bulk diffusivity of the organic species. Our results suggest that SOA formed from isoprene photooxidation is semi-volatile, and the resulting size distribution evolution is highly sensitive to the phase state (bulk diffusivity) of the pre-existing aerosol. Implications of these findings on further SOA model development and evaluation strategy will be discussed.

An Analysis of Neptune's Stratospheric Haze Using High-Phase-Angle Voyager Images

NASA Technical Reports Server (NTRS)

Moses, Julianne I.; Rages, Kathy; Pollack, James B.

1995-01-01

We have inverted high-phase-angle Voyager images of Neptune to determine the atmospheric extinction coefficient as a function of altitude and the scattering phase function at a reference altitude. Comparisons between theoretical model and observations help separate the contributions from molecular Rayleigh and aerosol scattering and help determine the variation of the aerosol size, concentration, and scattering properties with altitude. Further comparisons between models and data allow us to place constraints on the location and composition of the hazes, the concentration and downward flux of certain condensible hydrocarbon gases, the eddy diffusion coefficient in the lower stratosphere, and the thermal profile in parts of Neptune's stratosphere. We find that a distinct stratospheric haze layer exists near 12(sub -1, sup +1) mbar in Neptune's lower stratosphere, most probably due to condensed ethane. The derived stratospheric haze production rate of 1.0(sub -0.3, sup +0.2) x 10(exp -15) g cm(exp -2) sec(exp -1) is substantially lower than photochemical model predictions. Evidence for hazes at higher altitudes also exists. Unlike the situation on Uranus, large particles (0.08-0.11 microns) may be present at high altitudes on Neptune (e.g., near 0.5 mbar), well above the region in which we expect the major hydrocarbon species to condense. Near 28 mbar, the mean particle size is about 0.13(sub -0.02, sup +0.02) microns with a concentration of 5(sub -3, sup +3) particles cm(exp -3). The cumulative haze extinction optical depth above 15 mbar in the clear filter is approx. 3 x 10(exp -3), and much of this extinction is due to scattering rather than absorption; thus, if our limb-scan sites are typical, the hazes cannot account for the stratospheric temperature inversion on Neptune and may not contribute significantly to atmospheric heating. We compare the imaging results with the results from other observations, including those of the Voyager Photopolarimeter Subsystem, and discuss differences between Neptune and Uranus.

Condensation Kinetics of Water on Amorphous Aerosol Particles.

PubMed

Rothfuss, Nicholas E; Marsh, Aleksandra; Rovelli, Grazia; Petters, Markus D; Reid, Jonathan P

2018-06-25

Responding to changes in the surrounding environment, aerosol particles can grow by water condensation changing rapidly in composition and changing dramatically in viscosity. The timescale for growth is important to establish for particles undergoing hydration processes in the atmosphere or during inhalation. Using an electrodynamic balance, we report direct measurements at -7.5, 0, and 20 °C of timescales for hygroscopic condensational growth on a range of model hygroscopic aerosol systems. These extend from viscous aerosol particles containing a single saccharide solute (sucrose, glucose, raffinose, or trehalose) and a starting viscosity equivalent to a glass of ∼10 12 Pa·s, to nonviscous (∼10 -2 Pa·s) tetraethylene glycol particles. The condensation timescales observed in this work indicate that water condensation occurs rapidly at all temperatures examined (<10 s) and for particles of all initial viscosities spanning 10 -2 to 10 12 Pa·s. Only a marginal delay (<1 order of magnitude) is observed for particles starting as a glass.

The Messy Aerosol Submodel MADE3 (v2.0b): Description and a Box Model Test

NASA Technical Reports Server (NTRS)

Kaiser, J. C.; Hendricks, J.; Righi, M.; Riemer, N.; Zaveri, R. A.; Metzger, S.; Aquila, Valentina

2014-01-01

We introduce MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, 3rd generation), an aerosol dynamics submodel for application within the MESSy framework (Modular Earth Submodel System). MADE3 builds on the predecessor aerosol submodels MADE and MADE-in. Its main new features are the explicit representation of coarse particle interactions both with other particles and with condensable gases, and the inclusion of hydrochloric acid (HCl)chloride (Cl) partitioning between the gas and condensed phases. The aerosol size distribution is represented in the new submodel as a superposition of nine lognormal modes: one for fully soluble particles, one for insoluble particles, and one for mixed particles in each of three size ranges (Aitken, accumulation, and coarse mode size ranges). In order to assess the performance of MADE3 we compare it to its predecessor MADE and to the much more detailed particle-resolved aerosol model PartMC-MOSAIC in a box model simulation of an idealized marine boundary layer test case. MADE3 and MADE results are very similar, except in the coarse mode, where the aerosol is dominated by sea spray particles. Cl is reduced in MADE3 with respect to MADE due to the HClCl partitioning that leads to Cl removal from the sea spray aerosol in our test case. Additionally, aerosol nitrate concentration is higher in MADE3 due to the condensation of nitric acid on coarse particles. MADE3 and PartMC- MOSAIC show substantial differences in the fine particle size distributions (sizes about 2 micrometers) that could be relevant when simulating climate effects on a global scale. Nevertheless, the agreement between MADE3 and PartMC-MOSAIC is very good when it comes to coarse particle size distribution, and also in terms of aerosol composition. Considering these results and the well-established ability of MADE in reproducing observed aerosol loadings and composition, MADE3 seems suitable for application within a global model.

Microstructure and Thermal History of Metal Particles in CH Chondrites

NASA Technical Reports Server (NTRS)

Goldstein, J. I.; Jones, R. H.; Kotula, P. G.; Michael, J. R.

2005-01-01

Fe-Ni metal particles with smooth Ni, Co, and Cr zoning patterns, 8-13 wt.% Ni in the center of the particle to 3-5 wt% Ni at the rim, have been identified in several CR-clan (CH, Bencubbinlike, and CR) chondrites. These zoning patterns are broadly consistent with an origin by gas-solid condensation in the solar nebula at temperatures between approximately 1500 to 1300 K and fast cooling rates, 2 to 25 K/day. Apparently, this condensate metal was not melted during chondrule formation or affected significantly in the solid-state by alteration during parent body processing. Consideration of diffusional redistribution of Ni, Co, Cr and siderophile elements have further constrained the calculated condensation temperatures and cooling rates of the zoned condensates. These condensate metals have irregular shapes and vary in size from 50 to 350 m as revealed in some detail by optical and SEM techniques. In addition to zoned condensate particles, other types of metal particles have been observed. These include zoned condensates with exsolution-precipitates, unzoned homogeneous metal with no exsolution precipitates, unzoned metal exhibiting exsolution precipitates and high Ni metal grains.

Aerosol mobility imaging for rapid size distribution measurements

DOEpatents

Wang, Jian; Hering, Susanne Vera; Spielman, Steven Russel; Kuang, Chongai

2016-07-19

A parallel plate dimensional electrical mobility separator and laminar flow water condensation provide rapid, mobility-based particle sizing at concentrations typical of the remote atmosphere. Particles are separated spatially within the electrical mobility separator, enlarged through water condensation, and imaged onto a CCD array. The mobility separation distributes particles in accordance with their size. The condensation enlarges size-separated particles by water condensation while they are still within the gap of the mobility drift tube. Once enlarged the particles are illuminated by a laser. At a pre-selected frequency, typically 10 Hz, the position of all of the individual particles illuminated by the laser are captured by CCD camera. This instantly records the particle number concentration at each position. Because the position is directly related to the particle size (or mobility), the particle size spectra is derived from the images recorded by the CCD.

The Impact of Condensed-Phase Viscosity on Multiphase Oxidation Kinetics Involving O3, NO3, and OH

NASA Astrophysics Data System (ADS)

Li, J.; Forrester, S. M.; Knopf, D. A.

2017-12-01

Organic aerosol (OA) particles are ubiquitous in the atmosphere and have a significant influence on air quality, human health, cloud formation processes and global climate. By now it is well-recognized that organic particulate species can be amorphous in nature, existing in liquid, semi-solid and solid (glassy) phase states. The phase state is modulated by particle composition and environmental conditions such as relative humidity and temperature. These modifications can influence particle viscosity and molecular diffusion and, therefore, impact the reactive uptake of gas-phase oxidants and radicals by the organic substrate. In this study, we determined the reactive uptake coefficients (γ) of O3 by canola oil, NO3 by levoglucosan (LEV) and a LEV/xylitol mixture, and OH by glucose/sulfuric acid mixtures and glucose/1,2,6-hexanetriol mixtures under dry conditions and for temperatures ranging from 293 K to 213 K. Uptake coefficients have been measured employing a chemical ionization mass spectrometer coupled to a temperature-controlled rotating-wall flow reactor. Glass transition temperatures (Tg) of applied substrates were estimated by the Gordon-Taylor equation. Phase states were qualitatively probed via poking experiment using a temperature-controlled cooling stage. Shattering of the substrates indicated the formation of a glassy state. Results show a significant impact of condensed phase state on reactive uptake kinetics whereby γ changed most profoundly around estimated Tg. For example, γ decreases from 6.5×10-4 to 1.9 ×10-5 for O3 uptake by canola oil and from 8.3×10-4 to 3.1×10-4 for NO3 uptake by the LEV/xylitol mixture, respectively. The decrease in γ will be discussed with regard to phase state, desorption lifetime, and Arrhenius temperature dependence of reaction rates. First results of OH uptakes at low temperatures are presented, together with a discussion of the relevant atmospheric implications.

A thermodynamics model for morphology prediction of aluminum nano crystals fabricated by the inert gas condensation method

NASA Astrophysics Data System (ADS)

Wen, Yu; Xia, Dehong

2018-03-01

The purpose of this study is to provide scientific guidance for the morphological control of nanoparticle synthesis using the gas phase method. A universal thermodynamics model is developed to predict the morphology of nanoparticles fabricated using the inert gas condensation method. By using this model, the morphologies of aluminum nanocrystals are predicted under various preparation conditions. There are two types of energy that jointly determine the formation of nanoparticle morphology—Gibbs free energy for nanoparticles and energy variation during the process. The results show that energy variation dominates morphology formation when the cooling rate is less than 2 × 1011 K s-1 in the aluminum nanocrystal production process. At the beginning of the nanoparticle growth, the most stable morphology is predicted to be spherical, but the energetically preferred morphology becomes cubic as the particle grows. The turning point in the particle size at which spherical morphology is no longer the most stable morphology is exhibited as a function of pressure in a condensation chamber for different cooling rates. In this paper, we focus on the need for morphology prediction based on preparation conditions. It is concluded that nanoparticles with various morphologies could be obtained by adjusting the cooling rate and pressure in the condensation chamber.

Dust in brown dwarfs. III. Formation and structure of quasi-static cloud layers

NASA Astrophysics Data System (ADS)

Woitke, P.; Helling, Ch.

2004-01-01

In this paper, first solutions of the dust moment equations developed in (Woitke & Helling \\cite{wh2003a}) for the description of dust formation and precipitation in brown dwarf and giant gas planet atmospheres are presented. We consider the special case of a static brown dwarf atmosphere, where dust particles continuously nucleate from the gas phase, grow by the accretion of molecules, settle gravitationally and re-evaporate thermally. Mixing by convective overshoot is assumed to replenish the atmosphere with condensable elements, which is necessary to counterbalance the loss of condensable elements by dust formation and gravitational settling (no dust without mixing). Applying a kinetic description of the relevant microphysical and chemical processes for TiO2-grains, the model makes predictions about the large-scale stratification of dust in the atmosphere, the depletion of molecules from the gas phase, the supersaturation of the gas in the atmosphere as well as the mean size and the mass fraction of dust grains as function of depth. Our results suggest that the presence of relevant amounts of dust is restricted to a layer, where the upper boundary (cloud deck) is related to the requirement of a minimum mixing activity (mixing time-scale τmix ≈ 10 6 s) and the lower boundary (cloud base) is determined by the thermodynamical stability of the grains. The nucleation occurs around the cloud deck where the gas is cool, strongly depleted, but nevertheless highly supersaturated (S ≫ 1). These particles settle gravitationally and populate the warmer layers below, where the in situ formation (nucleation) is ineffective or even not possible. During their descent, the particles grow and reach mean radii of ≈30 \\mum ... 400 \\mum at the cloud base, but the majority of the particles in the cloud layer remains much smaller. Finally, the dust grains sink into layers which are sufficiently hot to cause their thermal evaporation. Hence, an effective transport mechanism for condensable elements exists in brown dwarfs, which depletes the gas above and enriches the gas below the cloud base of a considered solid/liquid material. The dust-to-gas mass fraction in the cloud layer results to be approximately given by the mass fraction of condensable elements in the gas being mixed up. Only for artificially reduced mixing we find a self-regulation mechanism that approximately installs phase equilibrium (S ≈ 1) in a limited region around the cloud base.

The volumetric fraction of inorganic particles and the flexural strength of composites for posterior teeth.

PubMed

Adabo, Gelson Luis; dos Santos Cruz, Carlos Alberto; Fonseca, Renata Garcia; Vaz, Luís Geraldo

2003-07-01

To evaluate the content of inorganic particles and the flexural strength of new condensable composites for posterior teeth in comparison to hybrid conventional composites. The determination of the content of inorganic particles was performed by mass weighing of a polymerized composite before and after the elimination of the organic phase. The volumetric particle content was determined by a practical method based on Archimedes' principle, which calculates the volume of the composite and their particles by differential mass measured in the air and in water. The flexural strength of three points was evaluated according to the norm ISO 4049:1988. The results showed the following filler content: Alert, 67.26%; Z-100, 65.27%; Filtek P 60, 62.34%; Ariston pHc, 64.07%; Tetric Ceram, 57.22%; Definite, 54.42%; Solitaire, 47.76%. In the flexural strength test, the materials presented the following decreasing order of resistance: Filtek P 60 (170.02 MPa)>Z-100 (151.34 MPa)>Tetric Ceram (126.14 MPa)=Alert (124.89 MPa)>Ariston pHc (102.00 MPa)=Definite (93.63 MPa)>Solitaire (56.71 MPa). New condensable composites for posterior teeth present a concentration of inorganic particles similar to those of hybrid composites but do not necessarily present higher flexural strength.

Minimizing Concentration Effects in Water-Based, Laminar-Flow Condensation Particle Counters

PubMed Central

Lewis, Gregory S.; Hering, Susanne V.

2013-01-01

Concentration effects in water condensation systems, such as used in the water-based condensation particle counter, are explored through numeric modeling and direct measurements. Modeling shows that the condensation heat release and vapor depletion associated with particle activation and growth lowers the peak supersaturation. At higher number concentrations, the diameter of the droplets formed is smaller, and the threshold particle size for activation is higher. This occurs in both cylindrical and parallel plate geometries. For water-based systems we find that condensational heat release is more important than is vapor depletion. We also find that concentration effects can be minimized through use of smaller tube diameters, or more closely spaced parallel plates. Experimental measurements of droplet diameter confirm modeling results. PMID:24436507

Synthesis of TiO2 Nanoparticles from Ilmenite Through the Mechanism of Vapor-Phase Reaction Process by Thermal Plasma Technology

NASA Astrophysics Data System (ADS)

Samal, Sneha

2017-11-01

Synthesis of nanoparticles of TiO2 was carried out by non-transferred arc thermal plasma reactor using ilmenite as the precursor material. The powder ilmenite was vaporized at high temperature in plasma flame and converted to a gaseous state of ions in the metastable phase. On cooling, chamber condensation process takes place on recombination of ions for the formation of nanoparticles. The top-to-bottom approach induces the disintegration of complex ilmenite phases into simpler compounds of iron oxide and titanium dioxide phases. The vapor-phase reaction mechanism was carried out in thermal plasma zone for the synthesis of nanoparticles from ilmenite compound in a plasma reactor. The easy separation of iron particles from TiO2 was taken place in the plasma chamber with deposition of light TiO2 particles at the top of the cooling chamber and iron particles at the bottom. The dissociation and combination process of mechanism and synthesis are studied briefly in this article. The product TiO2 nanoparticle shows the purity with a major phase of rutile content. TiO2 nanoparticles produced in vapor-phase reaction process shows more photo-induced capacity.

Uniform discotic wax particles via electrospray emulsification.

PubMed

Mejia, Andres F; He, Peng; Luo, Dawei; Marquez, Manuel; Cheng, Zhengdong

2009-06-01

We present a novel colloidal discotic system: the formation and self-assembling of wax microdisks with a narrow size distribution. Uniform wax emulsions are first fabricated by electrospraying of melt alpha-eicosene. The size of the emulsions can be flexibly tailored by varying the flow rate of the discontinuous phase, its electric conductivity, and the applied voltage. The process of entrainment of wax droplets, vital for obtaining uniform emulsions, is facilitated by the reduction of air-water surface tension and the density of the continuous phase. Then uniform wax discotic particles are produced via phase transition, during which the formation of a layered structure of the rotator phase of wax converts the droplets, one by one, into oblate particles. The time span for the conversion from spherical emulsions to disk particles is linearly dependent on the size of droplets in the emulsion, indicating the growth of a rotator phase from surface to the center is the limiting step in the shape transition. Using polarized light microscopy, the self-assembling of wax disks is observed by increasing disk concentration and inducing depletion attraction among disks, where several phases, such as isotropic, condensed, columnar stacking, and self-assembly of columnar rods are present sequentially during solvent evaporation of a suspension drop.

Laboratory Studies of the Optical Properties and Condensation Processes of Cosmic Dust Particles

NASA Technical Reports Server (NTRS)

Abbas, Mian M.; Craven, Paul D.; Spann, James F.; Tankosic, Dragana; Six, N. Frank (Technical Monitor)

2002-01-01

A laboratory facility for levitating single isolated dust particles in an electrodynamics balance has been developing at NASA/Marshall Space Flight Center for conducting a variety of experimental, of astrophysical interest. The objective of this research is to employ this innovative experimental technique for studies of the physical and optical properties of the analogs of cosmic grains of 0.2-10 micron size in a chamber with controlled pressure/temperatures simulating astrophysical environments. In particular, we will carry out three classes of experiments to investigate the microphysics of the analogs of interstellar and interplanetary dust grains. (1) Charge characteristics of micron size single dust grains to determine the photoelectric efficiencies, yields, and equilibrium potentials when exposed to UV radiation. These measurements will provide the much-needed photoelectric emission data relating to individual particles as opposed to that for the bulk materials available so far. (2) Infrared optical properties of dust particles obtained by irradiating the particles with radiation from tunable infrared diode lasers and measuring the scattered radiation. Specifically, the complex refractive indices, the extinction coefficients, the scattering phase functions, and the polarization properties of single dust grains of interest in interstellar environments, in the 1-25 micron spectral region will be determined. (3) Condensation experiments to investigate the deposition of volatile gases on colder nucleated particles in dense interstellar clouds and lower planetary atmospheres. The increase in the mass or m/q ratio due to condensation on the particle will be monitored as a function of the dust particle temperature and the partial pressure of the injected volatile gas. The measured data wild permit determination of the sticking efficiencies of volatile gases of astrophysical interest. Preliminary results based on photoelectric emission experiments on 0.2-6.6 micron size silica particles exposed to UV radiation in the 120-200 nm spectral region will be presented.

Fundamental Research Applied To Enable Hardware Performance in Microgravity

NASA Technical Reports Server (NTRS)

Sheredy, William A.

2005-01-01

NASA sponsors microgravity research to generate knowledge in physical sciences. In some cases, that knowledge must be applied to enable future research. This article describes one such example. The Dust and Aerosol measurement Feasibility Test (DAFT) is a risk-mitigation experiment developed at the NASA Glenn Research Center by NASA and ZIN Technologies, Inc., in support of the Smoke Aerosol Measurement Experiment (SAME). SAME is an investigation that is being designed for operation in the Microgravity Science Glovebox aboard the International Space Station (ISS). The purpose of DAFT is to evaluate the performance of P-Trak (TSI Incorporated, Shoreview, MN)--a commercially available condensation nuclei counter and a key SAME diagnostic- -in long-duration microgravity because of concerns about its ability to operate properly in that environment. If its microgravity performance is proven, this device will advance the state of the art in particle measurement capabilities for space vehicles and facilities, such as aboard the ISS. The P-Trak, a hand-held instrument, can count individual particles as small as 20 nm in diameter in an aerosol stream. Particles are drawn into the device by a built-in suction pump. Upon entering the instrument, these particles pass through a saturator tube where they mix with an alcohol vapor (see the following figure). This mixture then flows through a cooled condenser tube where some of the alcohol condenses onto the sample particles, and the droplets grow in a controlled fashion until they are large enough to be counted. These larger droplets pass through an internal nozzle and past a focused laser beam, producing flashes of light that are sensed by a photodetector and then counted to determine particle number concentration. The operation of the instrument depends on the proper internal flow and recycling of isopropyl alcohol in both the vapor and liquid phases.

Anderson localization and Mott insulator phase in the time domain

PubMed Central

Sacha, Krzysztof

2015-01-01

Particles in space periodic potentials constitute standard models for investigation of crystalline phenomena in solid state physics. Time periodicity of periodically driven systems is a close analogue of space periodicity of solid state crystals. There is an intriguing question if solid state phenomena can be observed in the time domain. Here we show that wave-packets localized on resonant classical trajectories of periodically driven systems are ideal elements to realize Anderson localization or Mott insulator phase in the time domain. Uniform superpositions of the wave-packets form stationary states of a periodically driven particle. However, an additional perturbation that fluctuates in time results in disorder in time and Anderson localization effects emerge. Switching to many-particle systems we observe that depending on how strong particle interactions are, stationary states can be Bose-Einstein condensates or single Fock states where definite numbers of particles occupy the periodically evolving wave-packets. Our study shows that non-trivial crystal-like phenomena can be observed in the time domain. PMID:26074169

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1987-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

NASA Technical Reports Server (NTRS)

Gokoglu, S. A.

1986-01-01

The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

Measurements of the hygroscopic and deliquescence properties of organic compounds of different solubilities in water and their relationship with cloud condensation nuclei activities.

PubMed

Chan, Man Nin; Kreidenweis, Sonia M; Chan, Chak K

2008-05-15

The initial phase (solid or aqueous droplet) of aerosol particles prior to activation is among the critical factors in determining their cloud condensation nuclei (CCN) activity. Single-particle levitation in an electrodynamic balance (EDB)was used to measure the phase transitions and hygroscopic properties of aerosol particles of 11 organic compounds with different solubilities (10(-1) to 102 g solute/100 g water). We use these data and other literature data to relate the CCN activity and hygroscopicity of organic compounds with different solubilities. The EDB data show that glyoxylic acid, 4-methylphthalic acid, monosaccharides (fructose and mannose), and disaccharides (maltose and lactose) did not crystallize and existed as metastable droplets at low relative humidity (RH). Hygroscopic data from this work and in the literature support earlier studies showing that the CCN activities of compounds with solubilities down to the order of 10(-1) g solute/100 g water can be predicted by standard Köhler theory with the assumption of complete dissolution of the solute at activation. We also demonstrate the use of evaporation data (or efflorescence data), which provides information on the water contents of metastable solutions below the compound deliquescence RH that can be extrapolated to higher dilutions, to predict the CCN activity of organic particles, particularly for sparingly soluble organic compounds that do not deliquesce at RH achievable in the EDB and in the hygroscopic tandem differential mobility analyzer.

Density-induced suppression of the {alpha}-particle condensate in nuclear matter and the structure of {alpha}-cluster states in nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Funaki, Y.; Horiuchi, H.; International Institute for Advanced Studies, Kizugawa 619-0225

2008-06-15

At low densities, with decreasing temperatures, in symmetric nuclear matter {alpha} particles are formed, which eventually give raise to a quantum condensate with four-nucleon {alpha}-like correlations (quartetting). Starting with a model of {alpha} matter, where undistorted {alpha} particles interact via an effective interaction such as the Ali-Bodmer potential, the suppression of the condensate fraction at zero temperature with increasing density is considered. Using a Jastrow-Feenberg approach, it is found that the condensate fraction vanishes near saturation density. Additionally, the modification of the internal state of the {alpha} particle due to medium effects will further reduce the condensate. In finite systems,more » an enhancement of the S-state wave function of the center-of-mass orbital of {alpha}-particle motion is considered as the correspondence to the condensate. Wave functions have been constructed for self-conjugate 4n nuclei that describe the condensate state but are fully antisymmetrized on the nucleonic level. These condensate-like cluster wave functions have been successfully applied to describe properties of low-density states near the n{alpha} threshold. Comparison with orthogonality condition model calculations in {sup 12}C and {sup 16}O shows strong enhancement of the occupation of the S-state center-of-mass orbital of the {alpha} particles. This enhancement is decreasing if the baryon density increases, similar to the density-induced suppression of the condensate fraction in {alpha} matter. The ground states of {sup 12}C and {sup 16}O show no enhancement at all, thus a quartetting condensate cannot be formed at saturation densities.« less

Explosive desorption of icy grain mantles in dense clouds

NASA Technical Reports Server (NTRS)

Schutte, W. A.; Greenberg, J. M.

1991-01-01

The cycling of the condensible material in dense clouds between the gas phase and the icy grain mantles is investigated. In the model studied, desorption of the ice occurs due to grain mantle explosions when photochemically stored energy is released after transient heating by a cosmic ray particle. It is shown that, depending on the grain size distribution in dense clouds, explosive desorption can maintain up to about eight percent of the carbon in the form of CO in the gas phase at typical cloud densities.

Aerosol Particle Interfacial Thermodynamics and Phase Partitioning Measurements Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Dutcher, Cari; Metcalf, Andrew

2015-03-01

Secondary organic aerosol particles are nearly ubiquitous in the atmosphere and yet there remain large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. Interfacial properties affect the ambient aerosol morphology, or internal structure of the particle, which in turn can affect the way a particle interacts with an environment of condensable clusters and organic vapors. To improve our ability to accurately predict ambient aerosol morphology, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Unfortunately, many techniques employed to measure interfacial properties do so in bulk solutions or in the presence of a ternary (e.g. solid) phase. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface or interfacial tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred.

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation.

PubMed

Charnawskas, Joseph C; Alpert, Peter A; Lambe, Andrew T; Berkemeier, Thomas; O'Brien, Rachel E; Massoli, Paola; Onasch, Timothy B; Shiraiwa, Manabu; Moffet, Ryan C; Gilles, Mary K; Davidovits, Paul; Worsnop, Douglas R; Knopf, Daniel A

2017-08-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles' organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g ) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.

Radial inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy (Invited)

NASA Astrophysics Data System (ADS)

Krieger, U. K.; Steimer, S.; Lienhard, D.; Bastelberger, S.

2013-12-01

Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous MBTCA (3-methyl-1,2,3-Butanetricarboxylic acid) and shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a 'white light ' LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. Potential implications for gas to particle partitioning and heterogeneous chemistry are discussed. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary organic aerosol particles, Nature 467, 824-827. [2] B. Zobrist et al. (2011): Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys. 13, 3514-3526. [3] D. L. Bones, J. P. Reid, D. M. Lienhard, and U. K. Krieger (2012): Comparing the mechanism of water condensation and evaporation in glassy aerosol, PNAS 109, 11613-11618. [4] O. Peña and U. Pal (2009): Scattering of electromagnetic radiation by a multilayered sphere, Comput. Phys. Commun. 180, 2348-2354.

Conversion of fogwater and aerosol organic nitrogen to ammonium, nitrate, and NOx during exposure to simulated sunlight and ozone.

PubMed

Zhang, Qi; Anastasio, Cort

2003-08-15

Although organic nitrogen (ON) compounds are apparently ubiquitous in the troposphere, very little is known about their fate and transformations. As one step in addressing this issue, we have studied the transformations of bulk (uncharacterized) organic nitrogen in fogwaters and aerosol aqueous extracts during exposure to simulated sunlight and O3. Our results show that over the course of several hours of exposure a significant portion of condensed-phase organic nitrogen is transformed into ammonium, nitrite, nitrate, and NOx. For nitrite, there was both photochemical formation and destruction, resulting in a slow net loss. Ammonium and nitrate were formed at initial rates on the order of a few micromolar per hour in the bulk fogwaters, corresponding to formation rates of approximately 10 and 40 ng m(-3) h(-1), respectively, in ambient fog. The average initial formation rate (expressed as ng (m of air)(-3) h(-1)) of NH4+ in the aqueous extracts of fine particles (PM2.5) was approximately one-half of the corresponding fogwater value. Initial formation rates of NOx (i.e., NO + NO2) were equivalent to approximately 2-11 pptv h(-1) in the three fogwaters tested. Although the formation rates of ammonium and nitrate were relatively small as compared to their initial concentrations in fogwaters (approximately 200-2000 microM) and aerosol particles (approximately 400-1500 ng m(-3)), this photochemical mineralization and "renoxification" from condensed-phase organic N is a previously uncharacterized source of inorganic N in the atmosphere. This conversion also represents a new component in the biogeochemical cycle of nitrogen that might have significant influences on atmospheric composition, condensed-phase properties, and the ecological impacts of N deposition.

The Fireball integrated code package

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dobranich, D.; Powers, D.A.; Harper, F.T.

1997-07-01

Many deep-space satellites contain a plutonium heat source. An explosion, during launch, of a rocket carrying such a satellite offers the potential for the release of some of the plutonium. The fireball following such an explosion exposes any released plutonium to a high-temperature chemically-reactive environment. Vaporization, condensation, and agglomeration processes can alter the distribution of plutonium-bearing particles. The Fireball code package simulates the integrated response of the physical and chemical processes occurring in a fireball and the effect these processes have on the plutonium-bearing particle distribution. This integrated treatment of multiple phenomena represents a significant improvement in the state ofmore » the art for fireball simulations. Preliminary simulations of launch-second scenarios indicate: (1) most plutonium vaporization occurs within the first second of the fireball; (2) large non-aerosol-sized particles contribute very little to plutonium vapor production; (3) vaporization and both homogeneous and heterogeneous condensation occur simultaneously; (4) homogeneous condensation transports plutonium down to the smallest-particle sizes; (5) heterogeneous condensation precludes homogeneous condensation if sufficient condensation sites are available; and (6) agglomeration produces larger-sized particles but slows rapidly as the fireball grows.« less

Cloud Condensation Nuclei Particle Counter (CCN) Instrument Handbook

DOE Office of Scientific and Technical Information (OSTI.GOV)

Uin, Janek

2016-04-01

The Cloud Condensation Nuclei Counter—CCN (Figure 1) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility instrument for measuring the concentration of aerosol particles that can act as cloud condensation nuclei [1, 2]. The CCN draws the sample aerosol through a column with thermodynamically unstable supersaturated water vapor that can condense onto aerosol particles. Particles that are activated, i.e., grown larger in this process, are counted (and sized) by an Optical Particle Counter (OPC). Thus, activated ambient aerosol particle number concentration as a function of supersaturation is measured. Models CCN-100 and CCN-200 differ only inmore » the number of humidifier columns and related subsystems: CCN-100 has one column and CCN-200 has two columns along with dual flow systems and electronics.« less

Condensed phase conversion and growth of nanorods and other materials instead of from vapor

DOEpatents

Geohegan, David B.; Seals, Roland D.; Puretzky, Alex A.; Fan, Xudong

2010-10-19

Compositions, systems and methods are described for condensed phase conversion and growth of nanorods and other materials. A method includes providing a condensed phase matrix material; and activating the condensed phase matrix material to produce a plurality of nanorods by condensed phase conversion and growth from the condensed phase matrix material instead of from vapor. The compositions are very strong. The compositions and methods provide advantages because they allow (1) formation rates of nanostructures necessary for reasonable production rates, and (2) the near net shaped production of component structures.

Metrologically useful states of spin-1 Bose condensates with macroscopic magnetization

NASA Astrophysics Data System (ADS)

Kajtoch, Dariusz; Pawłowski, Krzysztof; Witkowska, Emilia

2018-02-01

We study theoretically the usefulness of spin-1 Bose condensates with macroscopic magnetization in a homogeneous magnetic field for quantum metrology. We demonstrate Heisenberg scaling of the quantum Fisher information for states in thermal equilibrium. The scaling applies to both antiferromagnetic and ferromagnetic interactions. The effect preserves as long as fluctuations of magnetization are sufficiently small. Scaling of the quantum Fisher information with the total particle number is derived within the mean-field approach in the zero-temperature limit and exactly in the high-magnetic-field limit for any temperature. The precision gain is intuitively explained owing to subtle features of the quasidistribution function in the phase space.

Evaluation of Selected Chemical Processes for Production of Low-cost Silicon, Phase 3. [using a fluidized bed reactor

NASA Technical Reports Server (NTRS)

Blocher, J. M., Jr.; Browning, M. F.

1979-01-01

The construction and operation of an experimental process system development unit (EPSDU) for the production of granular semiconductor grade silicon by the zinc vapor reduction of silicon tetrachloride in a fluidized bed of seed particles is presented. The construction of the process development unit (PDU) is reported. The PDU consists of four critical units of the EPSDU: the fluidized bed reactor, the reactor by product condenser, the zinc vaporizer, and the electrolytic cell. An experimental wetted wall condenser and its operation are described. Procedures are established for safe handling of SiCl4 leaks and spills from the EPSDU and PDU.

Induction of chromatin damage and distribution of isochromatid breaks in human fibroblast cells exposed to heavy ions

NASA Technical Reports Server (NTRS)

Kawata, Tetsuya; Ito, Hisao; Motoori, Ken; Ueda, Takuya; Shigematsu, Naoyuki; Furusawa, Yoshiya; Durante, Marco; George, Kerry; Wu, Honglu; Cucinotta, Francis A.

2002-01-01

The frequency of chromatid breaks and the distribution of isochromatid breaks were measured in G2-phase normal human fibroblasts prematurely condensed a short time after exposure to low- or high-LET radiations. The average number of isochromatid breaks from a single particle traversal increased with increasing LET values, while the average number of chromatid-type breaks appeared to reach a plateau. The distribution of isochromatid breaks after high-LET iron particles exposure was overdispersed compared to gamma-rays, indicating that a single iron particle traversal through a cell nucleus can produce multiple isochromatid breaks.

Induction of chromatin damage and distribution of isochromatid breaks in human fibroblast cells exposed to heavy ions.

PubMed

Kawata, Tetsuya; Ito, Hisao; Motoori, Ken; Ueda, Takuya; Shigematsu, Naoyuki; Furusawa, Yoshiya; Durante, Marco; George, Kerry; Wu, Honglu; Cucinotta, Francis A

2002-12-01

The frequency of chromatid breaks and the distribution of isochromatid breaks were measured in G2-phase normal human fibroblasts prematurely condensed a short time after exposure to low- or high-LET radiations. The average number of isochromatid breaks from a single particle traversal increased with increasing LET values, while the average number of chromatid-type breaks appeared to reach a plateau. The distribution of isochromatid breaks after high-LET iron particles exposure was overdispersed compared to gamma-rays, indicating that a single iron particle traversal through a cell nucleus can produce multiple isochromatid breaks.

Particle Size of CO2 Condensates in Mars Atmosphere Revealed by Climate Sounder and Laser Ranging Observations

NASA Astrophysics Data System (ADS)

Hu, Renyu

Current-generation Mars Climate Sounder (MCS) onboard the Mars Reconnaissance Orbiter (MRO) offers extensive coverage of the latitudinal and seasonal distribution of CO_2 condensation in Mars’s atmosphere. The atmospheric temperature profiles measured by MCS reveal that the thickness of CO_2 condensation layer reaches a maximum of 10-15 km (north) or ˜20 km (south) during the middle of winter. There is a shrinking of the CO_2 condensation layer from L_S ˜270(°) to ˜300(°) in 2007, probably related to a planet-encircling dust storm. We integrate the condensation area and the condensation occurrence rate synthesized from the MCS observations to estimate cumulative masses of CO2 condensates deposited onto the northern and southern seasonal polar caps. The mass loading of CO_2 condensate particles, when condensation occurs, can be independently inferred from the detections of reflective clouds by the Mars Orbiter Laser Altimetry (MOLA) onboard the Mars Global Surveyor (MGS). Therefore, we approximate the precipitation flux by the particle settling flux, which is estimated using the impulse responses of MOLA filter channels. With our approach, the total atmospheric condensation mass can be estimated from these observational data sets, with average particle size as the only free parameter. By comparison with the seasonal polar cap masses inferred from the time-varying gravity of Mars, our estimates indicate that the average condensate particle radius is 8 - 22 mum in the northern hemisphere and 4 - 13 mum in the southern hemisphere. This multi-instrument data analysis provides new constraints on modeling the microphysics of CO_2 clouds on Mars.

Weak lasing in one-dimensional polariton superlattices

PubMed Central

Zhang, Long; Xie, Wei; Wang, Jian; Poddubny, Alexander; Lu, Jian; Wang, Yinglei; Gu, Jie; Liu, Wenhui; Xu, Dan; Shen, Xuechu; Rubo, Yuri G.; Altshuler, Boris L.; Kavokin, Alexey V.; Chen, Zhanghai

2015-01-01

Bosons with finite lifetime exhibit condensation and lasing when their influx exceeds the lasing threshold determined by the dissipative losses. In general, different one-particle states decay differently, and the bosons are usually assumed to condense in the state with the longest lifetime. Interaction between the bosons partially neglected by such an assumption can smear the lasing threshold into a threshold domain—a stable lasing many-body state exists within certain intervals of the bosonic influxes. This recently described weak lasing regime is formed by the spontaneously symmetry breaking and phase-locking self-organization of bosonic modes, which results in an essentially many-body state with a stable balance between gains and losses. Here we report, to our knowledge, the first observation of the weak lasing phase in a one-dimensional condensate of exciton–polaritons subject to a periodic potential. Real and reciprocal space photoluminescence images demonstrate that the spatial period of the condensate is twice as large as the period of the underlying periodic potential. These experiments are realized at room temperature in a ZnO microwire deposited on a silicon grating. The period doubling takes place at a critical pumping power, whereas at a lower power polariton emission images have the same periodicity as the grating. PMID:25787253

Reaction Mechanisms and Particle Interaction in Burning Two-Phase Systems

NASA Technical Reports Server (NTRS)

Dreizin, Edward L.; Shoshin, Yuriy L.; Murdyy, Ruslan S.; Hoffmann, Vern K.

2001-01-01

The main objective of this research is to understand the mechanisms by which particle interactions affect ignition and combustion in the two-phase systems. Combustion of metal aerosols representing the two-phase systems is carried out in the microgravity environment enabling one to avoid the buoyant flows that mask the particle motion due to the particle-particle interaction effects. In addition, relatively large, e.g., 100 micron diameter particles can be used, that remain aerosolized (i.e., do not fall down as they would at normal gravity) so that their behavior ahead, behind, and within the propagating flame can be resolved optically. An experimental apparatus exploiting this approach has been designed for the 2.2-s drop tower microgravity experiments. A typical experiment includes fluidizing metal particles under microgravity in an acoustic field, turning off the acoustic exciter, and igniting the created aerosol at a constant pressure using a hot wire igniter. The flame propagation and details of the individual particle combustion and particle interactions are studied using high-speed movie and video cameras coupled with microscope lenses to resolve individual particles. Recorded flame images are digitized and various image processing techniques including flame position tracking, color separation, and pixel by pixel image comparisons are employed to understand the processes occurring in the burning aerosols. Condensed combustion products are collected after each experiment for the phase, composition, and morphology analyses. New experiments described in this paper address combustion of Ti and Al particle clouds in air and combustion of Mg particle clouds in CO2. In addition, microgravity combustion experiments have been conducted with the particles of the newly produced Al-Mg mechanical alloys aerosolized in air.

Bose-Einstein condensate in an optical lattice with Raman-assisted two-dimensional spin-orbit coupling

NASA Astrophysics Data System (ADS)

Pan, Jian-Song; Zhang, Wei; Yi, Wei; Guo, Guang-Can

2016-10-01

In a recent experiment (Z. Wu, L. Zhang, W. Sun, X.-T. Xu, B.-Z. Wang, S.-C. Ji, Y. Deng, S. Chen, X.-J. Liu, and J.-W. Pan, arXiv:1511.08170 [cond-mat.quant-gas]), a Raman-assisted two-dimensional spin-orbit coupling has been realized for a Bose-Einstein condensate in an optical lattice potential. In light of this exciting progress, we study in detail key properties of the system. As the Raman lasers inevitably couple atoms to high-lying bands, the behaviors of the system in both the single- and many-particle sectors are significantly affected. In particular, the high-band effects enhance the plane-wave phase and lead to the emergence of "roton" gaps at low Zeeman fields. Furthermore, we identify high-band-induced topological phase boundaries in both the single-particle and the quasiparticle spectra. We then derive an effective two-band model, which captures the high-band physics in the experimentally relevant regime. Our results not only offer valuable insights into the two-dimensional lattice spin-orbit coupling, but also provide a systematic formalism to model high-band effects in lattice systems with Raman-assisted spin-orbit couplings.

Preliminary investigation of a water-based method for fast integrating mobility spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Spielman, Steven R.; Hering, Susanne V.; Kuang, Chongai

A water-based condensational growth channel was developed for imaging mobility-separated particles within a parallel plate separation channel of the Fast Integrated Mobility Spectrometer (FIMS). Reported are initial tests of that system, in which the alcohol condenser of the FIMS was replaced by a water-based condensational growth channel. Tests with monodispersed sodium chloride aerosol verify that the water-condensational growth maintained the laminar flow, while providing sufficient growth for particle imaging. Particle positions mapped onto particle mobility, in accordance with theoretical expectations. Particles ranging in size from 12 nm to 100 nm were counted with the same efficiency as with a butanol-based ultrafine particlemore » counter, once inlet and line losses were taken into account.« less

Preliminary investigation of a water-based method for fast integrating mobility spectrometry

DOE PAGES

Spielman, Steven R.; Hering, Susanne V.; Kuang, Chongai; ...

2017-06-06

A water-based condensational growth channel was developed for imaging mobility-separated particles within a parallel plate separation channel of the Fast Integrated Mobility Spectrometer (FIMS). Reported are initial tests of that system, in which the alcohol condenser of the FIMS was replaced by a water-based condensational growth channel. Tests with monodispersed sodium chloride aerosol verify that the water-condensational growth maintained the laminar flow, while providing sufficient growth for particle imaging. Particle positions mapped onto particle mobility, in accordance with theoretical expectations. Particles ranging in size from 12 nm to 100 nm were counted with the same efficiency as with a butanol-based ultrafine particlemore » counter, once inlet and line losses were taken into account.« less

Design Rule for Colloidal Crystals of DNA-Functionalized Particles

NASA Astrophysics Data System (ADS)

Martinez-Veracoechea, Francisco J.; Mladek, Bianca M.; Tkachenko, Alexei V.; Frenkel, Daan

2011-07-01

We report a Monte Carlo simulation study of the phase behavior of colloids coated with long, flexible DNA chains. We find that an important change occurs in the phase diagram when the number of DNAs per colloid is decreased below a critical value. In this case, the triple point disappears and the condensed phase that coexists with the vapor is always liquid. Our simulations thus explain why, in the dilute solutions typically used in experiments, colloids coated with a small number of DNA strands cannot crystallize. We understand this behavior in terms of the discrete nature of DNA binding.

Bose-Einstein condensation in an ultra-hot gas of pumped magnons.

PubMed

Serga, Alexander A; Tiberkevich, Vasil S; Sandweg, Christian W; Vasyuchka, Vitaliy I; Bozhko, Dmytro A; Chumak, Andrii V; Neumann, Timo; Obry, Björn; Melkov, Gennadii A; Slavin, Andrei N; Hillebrands, Burkard

2014-03-11

Bose-Einstein condensation of quasi-particles such as excitons, polaritons, magnons and photons is a fascinating quantum mechanical phenomenon. Unlike the Bose-Einstein condensation of real particles (like atoms), these processes do not require low temperatures, since the high densities of low-energy quasi-particles needed for the condensate to form can be produced via external pumping. Here we demonstrate that such a pumping can create remarkably high effective temperatures in a narrow spectral region of the lowest energy states in a magnon gas, resulting in strikingly unexpected transitional dynamics of Bose-Einstein magnon condensate: the density of the condensate increases immediately after the external magnon flow is switched off and initially decreases if it is switched on again. This behaviour finds explanation in a nonlinear 'evaporative supercooling' mechanism that couples the low-energy magnons overheated by pumping with all the other thermal magnons, removing the excess heat, and allowing Bose-Einstein condensate formation.

Dimethylsulfide/cloud condensation nuclei/climate system - Relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles

NASA Technical Reports Server (NTRS)

Quinn, P. K.; Covert, D. S.; Bates, T. S.; Kapustin, V. N.; Ramsey-Bell, D. C.; Mcinnes, L. M.

1993-01-01

The mass and number relationships occurring within the atmospheric dimethylsulfide/cloud condensation nuclei (CCN)/climate system, using simultaneous measurements of particulate phase mass size distributions of nss SO4(2-), methanesulfonic acid (MSA), and NH4(+); number size distributions of particles having diameters between 0.02 and 9.6 microns; CCN concentrations at a supersaturation of 0.3 percent; relative humidity; and temperature, obtained for the northeastern Pacific Ocean in April and May 1991. Based on these measurements, particulate nss SO4(2-), MSA, and NH4(+) mass appeared to be correlated with both particle effective surface area and number in the accumulation mode size range (0.16 to 0.5 micron). No correlations were found in the size range below 0.16 micron. A correlation was also found between nss SO4(2-) mass and the CCN number concentration, such that a doubling of the SO4(2-) mass corresponded to a 40 percent increase in the CCN number concentration. However, no correlation was found between MSA mass and CCN concentration.

Production and condensation of organic gases in the atmosphere of Titan

NASA Technical Reports Server (NTRS)

Sagan, C.; Thompson, W. R.

1982-01-01

The rates and altitudes for the dissociation of atmospheric constituents on Titan are calculated for solar ultraviolet radiation, the solar wind, Saturn magnetospheric particles, the Saturn co-rotating plasma, and cosmic rays. Laboratory experiments show that a variety of simple gas phase organic molecules and more complex organic solids called tholins are produced by such irradiations of simulated Titanian atmospheres. Except for ultraviolet wavelengths longward of the methane photodissociation continuum, most dissociation events occur between about 3100 and 3600 km altitude, corresponding well to the region of EUV opacity detected by Voyager. For a wide variety of simple to moderately complex organic gases in the Titanian atmosphere, condensation occurs below the top of the main cloud deck at about 2825 km. It is proposed that such condensates, beginning with CH4 at about 2615 km, comprise the principal mass of the Titan clouds. There is a distinct tendency for the atmosphere of Titan to act as a fractional distillation device, molecules of greater complexity condensing out at higher altitudes.

Determination of the Cd-bearing phases in municipal solid waste and biomass single fly ash particles using SR-microXRF spectroscopy.

PubMed

Camerani, Maria Caterina; Somogyi, Andrea; Vekemans, Bart; Ansell, Stuart; Simionovici, Alexandre S; Steenari, Britt-Marie; Panas, Itai

2007-09-01

By using an excitation energy of 27.0 keV, synchrotron radiation-induced micro-X-ray fluorescence (SR-microXRF) is employed to extract information regarding the composition and distribution of Cd-bearing phases in municipal solid waste (MSW) and biomass fly ashes. Significance of observation is based on statistics of totally more than 100 individual MSW and biomass fly ash particles from a fluidized bed combustion (FBC) plant. Cd concentrations in the parts-per-million range are determined. In general, although previous leaching studies have indicated Cd to be predominant in the smaller-size ash particles, in the present study Cd is more evenly distributed throughout all the particle sizes. For MSW fly ashes, results indicate the presence of Cd mainly as CdBr2 hot-spots, whereas for biomass fly ashes, which exhibit lower CdX2 concentration, a thin Cd layer on/in the particles is reported. For both ashes, Ca-containing matrixes are found to be the main Cd-bearing phases. Support for this observation is found from independent first-principles periodic density functional theory calculations. The observations are condensed into a schematic mechanism for Cd adsorption on the fly ash particles.

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibitmore » a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.« less

Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew T.; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfatemore » mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveT gand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.« less

DUSTER: collection of meteoric CaO and carbon smoke particles in the upper stratosphere .

NASA Astrophysics Data System (ADS)

Della Corte, V.; Rietmeijer, F. J. M.; Rotundi, A.; Ferrari, M.; Palumbo, P.

Nanometer- to micrometer-size particles present in the upper stratosphere are a mixture of terrestrial and extra-terrestrial origins. They can be extraterrestrial particles condensed after meteor ablation. Meteoric dust in bolides is occasionally deposited into the lower stratosphere around 20 km altitude. Nanometer CaO and pure carbon smoke particles were collected at 38 km altitude in the upper stratosphere in the Arctic during June 2008 using DUSTER (Dust in the Upper Stratosphere Tracking Experiment and Retrieval), a balloon-borne instrument for the non-destructive collection of solid particles between 200 nm to 40 microns. We report the collection of micron sized CaCO_3 (calcite) grains. Their morphologies show evidence of melting and condensation after vaporization suggest at temperatures of approximately 3500 K. The formation environment of the collected grains was probably a dense dust cloud formed by the disintegration of a carbonaceous meteoroid during deceleration in the Earth� atmosphere. For the first time, DUSTER collected meteor ablation products that were presumably associated with the disintegration of a bolide crossing the Earth's atmosphere. The collected mostly CaO and pure carbon nanoparticles from the debris cloud of a fireball, included: 1) intact fragments; 2) quenched melted grains; and 3) vapor phase condensation products. The DUSTER project was funded by the Italian Space Agency (ASI), PRIN2008/MIUR (Ministero dell'Istruzione dell'Universitá e della Ricerca), PNRA 2013(Piano Nazionale Ricerca Antartide). CNES graciously provided this flight opportunity. We thank E. Zona and S. Inarta at the Laboratorio di Fisica Cosmica INAF, Osservatorio Astronomico di Capodimonte-Universitá di Napoli Parthenope. F.J.M.R. was supported by grant NNX07AI39G from the NASA Cosmochemistry Program. We thank three anonymous reviewers who assisted us in introducing our new instrument.

Vapor condensation onto a non-volatile liquid drop

DOE Office of Scientific and Technical Information (OSTI.GOV)

Inci, Levent; Bowles, Richard K., E-mail: richard.bowles@usask.ca

2013-12-07

Molecular dynamics simulations of miscible and partially miscible binary Lennard–Jones mixtures are used to study the dynamics and thermodynamics of vapor condensation onto a non-volatile liquid drop in the canonical ensemble. When the system volume is large, the driving force for condensation is low and only a submonolayer of the solvent is adsorbed onto the liquid drop. A small degree of mixing of the solvent phase into the core of the particles occurs for the miscible system. At smaller volumes, complete film formation is observed and the dynamics of film growth are dominated by cluster-cluster coalescence. Mixing into the coremore » of the droplet is also observed for partially miscible systems below an onset volume suggesting the presence of a solubility transition. We also develop a non-volatile liquid drop model, based on the capillarity approximations, that exhibits a solubility transition between small and large drops for partially miscible mixtures and has a hysteresis loop similar to the one observed in the deliquescence of small soluble salt particles. The properties of the model are compared to our simulation results and the model is used to study the formulation of classical nucleation theory for systems with low free energy barriers.« less

Condensed phase conversion and growth of nanorods instead of from vapor

DOEpatents

Geohegan, David B.; Seals, Roland D.; Puretzky, Alex A.; Fan, Xudong

2005-08-02

Compositions, systems and methods are described for condensed phase conversion and growth of nanorods and other materials. A method includes providing a condensed phase matrix material; and activating the condensed phase matrix material to produce a plurality of nanorods by condensed phase conversion and growth from the condensed chase matrix material instead of from vacor. The compositions are very strong. The compositions and methods provide advantages because they allow (1) formation rates of nanostructures necessary for reasonable production rates, and (2) the near net shaped production of component structures.

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

PubMed

Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H 2 SO 4 ) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1 H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal and methylglyoxal have the potential to produce significant organic aerosol mass and therefore could potentially impact chemical, optical and/or cloud-forming properties of aerosols, especially if the products partition to the aerosol surface.

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities

PubMed Central

Van Wyngarden, A. L.; Pérez-Montaño, S.; Bui, J. V. H.; Li, E. S. W.; Nelson, T. E.; Ha, K. T.; Leong, L.; Iraci, L. T.

2016-01-01

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40–80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H2SO4) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance–Fourier transform infrared (ATR-FTIR) and 1H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal and methylglyoxal have the potential to produce significant organic aerosol mass and therefore could potentially impact chemical, optical and/or cloud-forming properties of aerosols, especially if the products partition to the aerosol surface. PMID:27212937

Sol–gel synthesis of MCM-41 silicas and selective vapor-phase modification of their surface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roik, N.V., E-mail: roik_nadya@ukr.net; Belyakova, L.A.

2013-11-15

Silica particles with uniform hexagonal mesopore architecture were synthesized by template directed sol–gel condensation of tetraethoxysilane or mixture of tetraethoxysilane and (3-chloropropyl)triethoxysilane in a water–ethanol–ammonia solution. Selective functionalization of exterior surface of parent materials was carried out by postsynthetic treatment of template-filled MCM-41 and Cl-MCM-41 with vapors of (3-chloropropyl)triethoxysilane and 1,2-ethylenediamine in vacuum. The chemical composition of obtained mesoporous silicas was estimated by IR spectroscopy and chemical analysis of surface products of reactions. Characteristics of porous structure of resulting materials were determined from the data of X-ray, low-temperature nitrogen ad-desorption and transmission electron microscopy measurements. Obtained results confirm invariability ofmore » highly ordered mesoporous structure of MCM-41 and Cl-MCM-41 after their selective postsynthetic modification in vapor phase. It was proved that proposed method of vapor-phase functionalization of template-filled starting materials is not accompanied by dissolution of the template and chemical modification of pores surface. This provides preferential localization of grafted functional groups onto the exterior surface of mesoporous silicas. - Graphical abstract: Sol–gel synthesis and postsynthetic chemical modification of template-filled MCM-41 and Cl-MCM-41 with (3-chloropropyl)triethoxysilane and 1,2-ethylenediamine in vapor phase. Display Omitted - Highlights: • Synthesis of MCM-41 silica by template directed sol–gel condensation. • Selective vapor-phase functionalization of template-filled silica particles. • Preferential localization of grafted groups onto the exterior surface of mesoporous silicas.« less

Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts

DOE PAGES

Song, Mijung; Liu, Pengfei; Martin, Scot T.; ...

2017-09-25

Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid–liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than ~95 %) in α-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ~95 %more » RH in the biogenic SOM particles derived from β-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter κ of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.« less

Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Mijung; Liu, Pengfei; Martin, Scot T.

Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid–liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than ~95 %) in α-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ~95 %more » RH in the biogenic SOM particles derived from β-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter κ of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.« less

Liquid-liquid phase separation in particles containing secondary organic material free of inorganic salts

NASA Astrophysics Data System (ADS)

Song, Mijung; Liu, Pengfei; Martin, Scot T.; Bertram, Allan K.

2017-09-01

Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid-liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than ˜ 95 %) in α-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ˜ 95 % RH in the biogenic SOM particles derived from β-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter κ of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.

Ultrafine Condensation Particle Counter Instrument Handbook

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuang, C.

2016-02-01

The Model 3776 Ultrafine Condensation Particle Counter (UCPC; pictured in Appendix A) is designed for researchers interested in airborne particles smaller than 20 nm. With sensitivity to particles down to 2.5 nm in diameter, this UCPC is ideally suited for atmospheric and climate research, particle formation and growth studies, combustion and engine exhaust research, and nanotechnology research.

Are Organic Aerosols Good Cloud Condensation Nuclei?

NASA Astrophysics Data System (ADS)

Abbatt, J. P.; Broekhuizen, K.; Kumar, P. P.

2002-12-01

The ability of a set of organic-containing aerosols to act as cloud condensation nuclei has been measured in the laboratory using a thermal-gradient diffusion chamber operated at a fixed supersaturation. We observe that particles composed of soluble organics, such as malonic acid and adipic acid, activate at dry particle diameters in agreement with Kohler theory predications assuming the solutes are fully soluble and the droplet has the surface tension of water. Surprisingly, we also observe that sparingly soluble azelaic acid and cis-pinonic acid particles also activate, perhaps because they are being formed in a supersaturated, amorphous state or that their activation is aided by surface uptake of water. Mixed organic/ammonium sulfate particles have also been studied, and a range of behavior is observed. Soluble species such as malonic acid enhance activation through the vapour-pressure lowering effect whereas a thick coating of stearic acid on ammonium sulfate makes the particles totally inactive. Lastly, we have observed that pure oleic acid particles, which show no indication of activation when pure, can be activated after exposure to gas-phase ozone. The atmospheric implications of our results will be discussed. An interesting issue is the degree to which we can quantitatively model our results by assuming the surface tension of the growing droplet is that of water, i.e. without the need to invoke the surface-tension-lowering effect due to surface-active organics.

Universal phase diagrams with superconducting domes for electronic flat bands

NASA Astrophysics Data System (ADS)

Löthman, Tomas; Black-Schaffer, Annica M.

2017-08-01

Condensed matter systems with flat bands close to the Fermi level generally exhibit, due to their very large density of states, extraordinarily high critical ordering temperatures of symmetry-breaking orders, such as superconductivity and magnetism. Here we show that the critical temperatures follow one of two universal curves with doping away from a flat band depending on the ordering channel, which completely dictates both the general order competition and the phase diagram. Notably, we find that orders in the particle-particle channel (superconducting orders) survive decisively farther than orders in the particle-hole channel (magnetic or charge orders) because the channels have fundamentally different polarizabilities. Thus, even if a magnetic or charge order initially dominates, superconducting domes are still likely to exist on the flanks of flat bands. We apply these general results to both the topological surface flat bands of rhombohedral ABC-stacked graphite and to the Van Hove singularity of graphene.

High multiplicity α-particle breakup measurements to study α-condensate states

NASA Astrophysics Data System (ADS)

Bishop, J.; Kokalova, Tz; Freer, M.; Assie, M.; Acosta, L.; Bailey, S.; Cardella, G.; Curtis, N.; De Filippo, E.; Dell'Aquila, D.; De Luca, S.; Francalanza, L.; Gnoffo, B.; Lanzalone, G.; Lombardo, I.; Martorana, N.; Norella, S.; Pagano, A.; Pagano, E. V.; Papa, M.; Pirrone, S.; Politi, G.; Rizzo, F.; Russotto, P.; Quattrocchi, L.; Smith, R.; Stefan, I.; Trifirò, A.; Trimarchì, M.; Verde, G.; Vigilante, M.; Wheldon, C.

2017-06-01

An experiment was performed to investigate α-condensate states via high α-particle multiplicity breakup. The nucleus of interest was 28Si therefore to measure multiplicity 7 particle breakup events, a highly granular detector with a high solid angle coverage was required. For this purpose, the CHIMERA and FARCOS detectors at INFN LNS were employed. Particle identification was achieved through ΔE-E energy loss. The α-particle multiplicity was measured at three beam energies to investigate different excitation regimes in 28Si. At a beam energy where the energy is sufficient to provide the 7 α-particles with enough energy to be identified using the ΔE-E method, multiplicity 7 events can be seen. Given these high multiplicity events, the particles can be reconstructed to investigate the breakup of α-condensate states. Analysing the decay paths of these states can elucidate whether the state of interest corresponds to a non-cluster, clustered or condensed state.

Micro-rheology and interparticle interactions in aerosols probed with optical tweezers

NASA Astrophysics Data System (ADS)

Reid, Jonathan P.; Power, Rory M.; Cai, Chen; Simpson, Stephen H.

2014-09-01

Using optical tweezers for micro-rheological investigations of a surrounding fluid has been routinely demonstrated. In this work, we will demonstrate that rheological measurements of the bulk and surface properties of aerosol particles can be made directly using optical tweezers, providing important insights into the phase behavior of materials in confined environments and the rate of molecular diffusion in viscous phases. The use of holographic optical tweezers to manipulate aerosol particles has become standard practice in recent years, providing an invaluable tool to investigate particle dynamics, including evaporation/ condensation kinetics, chemical aging and phase transformation. When combined with non-linear Raman spectroscopy, the size and refractive index of a particle can be determined with unprecedented accuracy <+/- 0.05%). Active control of the relative positions of pairs of particles can allow studies of the coalescence of particles, providing a unique opportunity to investigate the bulk and surface properties that govern the hydrodynamic relaxation in particle shape. In particular, we will show how the viscosity and surface tension of particles can be measured directly in the under-damped regime at low viscosity. In the over-damped regime, we will show that viscosity measurements can extend close to the glass transition, allowing measurements over an impressive dynamic range of 12 orders of magnitude in relaxation timescale and viscosity. Indeed, prior to the coalescence event, we will show how the Brownian trajectories of trapped particles can yield important and unique insights into the interactions of aerosol particles.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marlow, W.H.

An aerosol here is understood to be a two-component system comprised of gaseous and condensed phases with the characteristic that the condensed phase is not an equilibrium subsystem. In contrast to the usual definitions based upon geometrical or mechanical variables, this quasi-thermodynamic formulation is framed to emphasize the dynamical behavior of aerosols by allowing for coagulation and other aerosol evolutionary processes as natural consequences of the interactions and state variables appropriate to the system. As will become clear later, it also provides a point of departure for distinguishing aerosol particles from unstable gas-phase cluster systems. The question of accommodation inmore » particle collisions must be addressed as a prelude to the discussion of the role of long-range forces. Microscopic reversibility is frequently assumed for molecular collisions with either molecules or solid surfaces. In the case of aerosol collisions, the implication of this assumption is that collisions are elastic, which is contrary to the evidence from coagulation experiments and the conventional operational assumption of sticking upon collision. Gay and Berne have performed computer simulations of the collision of two clusters consisting of a total of 135 molecules interacting via Lennard-Jones potentials. That work showed that complete accommodation, accompanied by overall heating of the unified cluster, occurred. Since heating represents an irreversible degradation of the kinetic energy of the collision, the hamiltonian of the two-cluster system should be considered as dissipative and therefore microscopic reversibility does not apply.« less

Observations and implications of liquid–liquid phase separation at high relative humidities in secondary organic material produced by α-pinene ozonolysis without inorganic salts

DOE PAGES

Renbaum-Wolff, Lindsay; Song, Mijung; Marcolli, Claudia; ...

2016-07-01

Particles consisting of secondary organic material (SOM) are abundant in the atmosphere. In order to predict the role of these particles in climate, visibility and atmospheric chemistry, information on particle phase state (i.e., single liquid, two liquids and solid) is needed. Our paper focuses on the phase state of SOM particles free of inorganic salts produced by the ozonolysis of α-pinene. Phase transitions were investigated in the laboratory using optical microscopy and theoretically using a thermodynamic model at 290 K and for relative humidities ranging from < 0.5 to 100%. In the laboratory studies, a single phase was observed frommore » 0 to 95% relative humidity (RH) while two liquid phases were observed above 95% RH. For increasing RH, the mechanism of liquid–liquid phase separation (LLPS) was spinodal decomposition. The RH range over which two liquid phases were observed did not depend on the direction of RH change. In the modeling studies, the SOM took up very little water and was a single organic-rich phase at low RH values. At high RH, the SOM underwent LLPS to form an organic-rich phase and a water-rich phase, consistent with the laboratory studies. The presence of LLPS at high RH values can have consequences for the cloud condensation nuclei (CCN) activity of SOM particles. In the simulated Köhler curves for SOM particles, two local maxima were observed. Depending on the composition of the SOM, the first or second maximum can determine the critical supersaturation for activation. Recently researchers have observed inconsistencies between measured CCN properties of SOM particles and hygroscopic growth measured below water saturation (i.e., hygroscopic parameters measured below water saturation were inconsistent with hygroscopic parameters measured above water saturation). Furthermore, the work presented here illustrates that such inconsistencies are expected for systems with LLPS when the water uptake at subsaturated conditions represents the hygroscopicity of an organic-rich phase while the barrier for CCN activation can be determined by the second maximum in the Köhler curve when the particles are water rich.« less

Effect of measurement protocol on organic aerosol measurements of exhaust emissions from gasoline and diesel vehicles

NASA Astrophysics Data System (ADS)

Kim, Youngseob; Sartelet, Karine; Seigneur, Christian; Charron, Aurélie; Besombes, Jean-Luc; Jaffrezo, Jean-Luc; Marchand, Nicolas; Polo, Lucie

2016-09-01

Exhaust emissions of semi-volatile organic compounds (SVOC) from passenger vehicles are usually estimated only for the particle phase via the total particulate matter measurements. However, they also need to be estimated for the gas phase, as they are semi-volatile. To better estimate SVOC emission factors of passenger vehicles, a measurement campaign using a chassis dynamometer was conducted with different instruments: (1) a constant volume sampling (CVS) system in which emissions were diluted with filtered air and sampling was performed on filters and polyurethane foams (PUF) and (2) a Dekati Fine Particle Sampler (FPS) in which emissions were diluted with purified air and sampled with on-line instruments (PTR-ToF-MS, HR-ToF-AMS, MAAP, CPC). Significant differences in the concentrations of organic carbon (OC) measured by the instruments are observed. The differences can be explained by sampling artefacts, differences between (1) the time elapsed during sampling (in the case of filter and PUF sampling) and (2) the time elapsed from emission to measurement (in the case of on-line instruments), which vary from a few seconds to 15 min, and by the different dilution factors. To relate elapsed times and measured concentrations of OC, the condensation of SVOC between the gas and particle phases is simulated with a dynamic aerosol model. The simulation results allow us to understand the relation between elapsed times and concentrations in the gas and particle phases. They indicate that the characteristic times to reach thermodynamic equilibrium between gas and particle phases may be as long as 8 min. Therefore, if the elapsed time is less than this characteristic time to reach equilibrium, gas-phase SVOC are not at equilibrium with the particle phase and a larger fraction of emitted SVOC will be in the gas phase than estimated by equilibrium theory, leading to an underestimation of emitted OC if only the particle phase is considered or if the gas-phase SVOC are estimated by equilibrium theory. Current European emission inventories for passenger cars do not yet estimate gas-phase SVOC emissions, although they may represent 60% of total emitted SVOC (gas + particle phases).

Constraining the Volatility Distributions and Possible Diffusion Limitations of Secondary Organic Aerosols Using Laboratory Dilution Experiments

NASA Astrophysics Data System (ADS)

Ye, Q.; Robinson, E. S.; Mahfouz, N.; Sullivan, R. C.; Donahue, N. M.

2016-12-01

Secondary organic aerosols (SOA) dominate the mass of fine particles in the atmosphere. Their formation involves both oxidation of volatile organics from various sources that produce products with uncertain volatilities, and diffusion of these products into the condensed phase. Therefore, constraining volatility distribution and diffusion timescales of the constituents in SOA are important in predicting size, concentration and composition of SOA, as well as how these properties of SOA evolve in the atmosphere. In this work, we demonstrate how carefully designed laboratory isothermal dilution experiments in smog chambers can shed light into the volatility distribution and any diffusion barriers of common types of SOA over time scales relevant to atmospheric transport and diurnal cycling. We choose SOA made from mono-terpenes (alpha-pinene and limonene) and toluene to represent biogenic and anthropogenic SOA. We look into how moisture content can alter any evaporation behaviors of SOA by varying relative humidity during SOA generation and during dilution process. This provides insight into whether diffusion in the condensed phase is rate limiting in reaching gas/particle equilibrium of semi-volatile organic compounds. Our preliminary results show that SOA from alpha-pinene evaporates continuously over several hours of experiments, and there is no substantial discernible differences over wide ranges of the chamber humidity. SOA from toluene oxidation shows slower evaporation. We fit these experimental data using absorptive partitioning theory and a particle dynamic model to obtain volatility distributions and to predict particle size evolution. This in the end will help us to improve representation of SOA in large scale chemical transport models.

Oxidation flow reactors (OFRs): overview of recent field and modeling studies

NASA Astrophysics Data System (ADS)

Jimenez, Jose-Luis; Palm, Brett B.; Peng, Zhe; Hu, Weiwei; Ortega, Amber M.; Li, Rui; Campuzano-Jost, Pedro; Day, Douglas A.; Stark, Harald; Brune, William H.; de Gouw, Joost; Schroder, Jason

2016-04-01

Oxidation flow reactors (OFRs) are popular tools for studying SOA formation and aging in both laboratory and field experiments. In an OFR, the concentration of an oxidant (OH, O3, or NO3) can be increased, leading to hours-months of equivalent atmospheric oxidation during the several-minute OFR residence time. Using gas- and particle-phase measurements from several recent field campaigns, we demonstrate SOA formation after oxidation of ambient air in an OFR. Typically, more SOA formation is observed from nighttime air than daytime air. This indicates that the concentration of SOA-forming gases in ambient air is relatively higher at night. Measured ambient VOCs are not able to explain the magnitude of SOA formation in the OFR, suggesting that typically unmeasured S/IVOCs (possibly VOC oxidation products or direct emissions) play a substantial intermediary role in ambient SOA formation. We also present highlights from recent OFR oxidant chemistry modeling studies. HOx, Ox, and photolysis chemistry was modeled for two common OH production methods (utilizing 185+254 nm UV light, or 254 nm only). OH exposure (OHexp) can be estimated within a factor of ~2 using model-derived equations, and can be verified in situ using VOC decay measurements. OHexp is strongly dependent on external OH reactivity, which may cause significant OH suppression in some circumstances (e.g., lab/source studies with high precursor concentrations). UV light photolysis and reaction with oxygen atoms are typically not major reaction pathways. Modeling the fate of condensable low-volatility organic gases (LVOCs) formed in an OFR suggests that LVOC fate is dependent on particle condensational sink. E.g., for the range of particle condensational sink at a remote pine forest, anywhere from 20-80% of produced LVOCs were predicted to condense onto aerosols for an OHexp of ~1 day, with the remainder lost to OFR or sampling line walls. Similar to large chamber wall loss corrections, a correction is needed to relate OFR sampling to the atmosphere, where condensation onto aerosols is the dominant LVOC fate. At high OHexp (>20 days) in an OFR, LVOCs are predicted to be oxidized many times before they can condense onto particles, leading to formation of volatile fragmentation products that can no longer condense to form SOA. Changes to preexisting OA at high OHexp should be predominantly a result of heterogeneous oxidation. SOA yields specific to OFR oxidation were investigated using standard addition of individual VOCs into ambient air in an OFR. SOA yields in the OFR were consistent with laboratory large chamber yields.

Cloud condensation nuclei droplet growth kinetics of ultrafine particles during anthropogenic nucleation events

NASA Astrophysics Data System (ADS)

Shantz, N. C.; Pierce, J. R.; Chang, R. Y.-W.; Vlasenko, A.; Riipinen, I.; Sjostedt, S.; Slowik, J. G.; Wiebe, A.; Liggio, J.; Abbatt, J. P. D.; Leaitch, W. R.

2012-02-01

Evolution of the cloud condensation nucleus (CCN) activity of 36 ± 4 nm diameter anthropogenic aerosol particles at a water supersaturation of 1.0 ± 0.1% is examined for particle nucleation and growth. During the early stages of one event, relatively few of the anthropogenic particles at 36 nm were CCN active and their growth rates by water condensation were delayed relative to ammonium sulphate particles. As the event progressed, the particle size distribution evolved to larger sizes and the relative numbers of particles at 36 nm that were CCN active increased until all the 36 nm particles were activating at the end of the event. Based on the chemistry of larger particles and the results from an aerosol chemical microphysics box model, the increase in CCN activity of the particles was most likely the result of the condensation of sulphate in this case. Despite the increased CCN activity, a delay was observed in the initial growth of these particles into cloud droplets, which persisted even when the aerosol was most CCN active later in the afternoon. Simulations show that the delay in water uptake is explained by a reduction of the mass accommodation coefficient assuming that the composition of the 36 nm particles is the same as the measured composition of the 60-100 nm particles.

A large source of low-volatility secondary organic aerosol

NASA Astrophysics Data System (ADS)

Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B.; Jørgensen, Solvejg; Kjaergaard, Henrik G.; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R.; Wildt, Jürgen; Mentel, Thomas F.

2014-02-01

Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

A large source of low-volatility secondary organic aerosol.

PubMed

Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F

2014-02-27

Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

Impact of the Bergeron-Findeisen process on the release of aerosol particles during the evolution of cloud ice

NASA Astrophysics Data System (ADS)

Schwarzenböck, A.; Mertes, S.; Heintzenberg, J.; Wobrock, W.; Laj, P.

The paper focuses on the redistribution of aerosol particles (APs) during the artificial nucleation and subsequent growth of ice crystals in a supercooled cloud. A significant number of the supercooled cloud droplets during icing periods (seeding agents: C 3H 8, CO 2) did not freeze as was presumed prior to the experiment but instead evaporated. The net mass flux of water vapour from the evaporating droplets to the nucleating ice crystals (Bergeron-Findeisen mechanism) led to the release of residual particles that simultaneously appeared in the interstitial phase. The strong decrease of the droplet residuals confirms the nucleation of ice particles on seeding germs without natural aerosol particles serving as ice nuclei. As the number of residual particles during the seedings did not drop to zero, other processes such as heterogeneous ice nucleation, spontaneous freezing, entrainment of supercooled droplets and diffusion to the created particle-free ice germs must have contributed to the experimental findings. During the icing periods, residual mass concentrations in the condensed phase dropped by a factor of 1.1-6.7, as compared to the unperturbed supercooled cloud. As the Bergeron-Findeisen process also occurs without artificial seeding in the atmosphere, this study demonstrated that the hydrometeors in mixed-phase clouds might be much cleaner than anticipated for the simple freezing process of supercooled droplets in tropospheric mid latitude clouds.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Renbaum-Wolff, Lindsay; Song, Mijung; Marcolli, Claudia

Particles consisting of secondary organic material (SOM) are abundant in the atmosphere. In order to predict the role of these particles in climate, visibility and atmospheric chemistry, information on particle phase state (i.e., single liquid, two liquids and solid) is needed. Our paper focuses on the phase state of SOM particles free of inorganic salts produced by the ozonolysis of α-pinene. Phase transitions were investigated in the laboratory using optical microscopy and theoretically using a thermodynamic model at 290 K and for relative humidities ranging from < 0.5 to 100%. In the laboratory studies, a single phase was observed frommore » 0 to 95% relative humidity (RH) while two liquid phases were observed above 95% RH. For increasing RH, the mechanism of liquid–liquid phase separation (LLPS) was spinodal decomposition. The RH range over which two liquid phases were observed did not depend on the direction of RH change. In the modeling studies, the SOM took up very little water and was a single organic-rich phase at low RH values. At high RH, the SOM underwent LLPS to form an organic-rich phase and a water-rich phase, consistent with the laboratory studies. The presence of LLPS at high RH values can have consequences for the cloud condensation nuclei (CCN) activity of SOM particles. In the simulated Köhler curves for SOM particles, two local maxima were observed. Depending on the composition of the SOM, the first or second maximum can determine the critical supersaturation for activation. Recently researchers have observed inconsistencies between measured CCN properties of SOM particles and hygroscopic growth measured below water saturation (i.e., hygroscopic parameters measured below water saturation were inconsistent with hygroscopic parameters measured above water saturation). Furthermore, the work presented here illustrates that such inconsistencies are expected for systems with LLPS when the water uptake at subsaturated conditions represents the hygroscopicity of an organic-rich phase while the barrier for CCN activation can be determined by the second maximum in the Köhler curve when the particles are water rich.« less

Computation of Phase Equilibria, State Diagrams and Gas/Particle Partitioning of Mixed Organic-Inorganic Aerosols

NASA Astrophysics Data System (ADS)

Zuend, A.; Marcolli, C.; Peter, T.

2009-04-01

The chemical composition of organic-inorganic aerosols is linked to several processes and specific topics in the field of atmospheric aerosol science. Photochemical oxidation of organics in the gas phase lowers the volatility of semi-volatile compounds and contributes to the particulate matter by gas/particle partitioning. Heterogeneous chemistry and changes in the ambient relative humidity influence the aerosol composition as well. Molecular interactions between condensed phase species show typically non-ideal thermodynamic behavior. Liquid-liquid phase separations into a mainly polar, aqueous and a less polar, organic phase may considerably influence the gas/particle partitioning of semi-volatile organics and inorganics (Erdakos and Pankow, 2004; Chang and Pankow, 2006). Moreover, the phases present in the aerosol particles feed back on the heterogeneous, multi-phase chemistry, influence the scattering and absorption of radiation and affect the CCN ability of the particles. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy, enabling the calculation of activity coefficients. We use the group-contribution model AIOMFAC (Zuend et al., 2008) to calculate activity coefficients, chemical potentials and the total Gibbs energy of mixed organic-inorganic systems. This thermodynamic model was combined with a robust global optimization module to compute potential liquid-liquid (LLE) and vapor-liquid-liquid equilibria (VLLE) as a function of particle composition at room temperature. And related to that, the gas/particle partitioning of semi-volatile components. Furthermore, we compute the thermodynamic stability (spinodal limits) of single-phase solutions, which provides information on the process type and kinetics of a phase separation. References Chang, E. I. and Pankow, J. F.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water - Part 2: Consideration of phase separation effects by an XUNIFAC model, Atmos. Environ., 40, 6422-6436, 2006. Erdakos, G. B. and Pankow, J. F.: Gas/particle partitioning of neutral and ionizing compounds to single- and multi-phase aerosol particles. 2. Phase separation in liquid particulate matter containing both polar and low-polarity organic compounds, Atmos. Environ., 38, 1005-1013, 2004. Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559-4593, 2008.

Perspective: Aerosol microphysics: From molecules to the chemical physics of aerosols

NASA Astrophysics Data System (ADS)

Bzdek, Bryan R.; Reid, Jonathan P.

2017-12-01

Aerosols are found in a wide diversity of contexts and applications, including the atmosphere, pharmaceutics, and industry. Aerosols are dispersions of particles in a gas, and the coupling of the two phases results in highly dynamic systems where chemical and physical properties like size, composition, phase, and refractive index change rapidly in response to environmental perturbations. Aerosol particles span a wide range of sizes from 1 nm to tens of micrometres or from small molecular clusters that may more closely resemble gas phase molecules to large particles that can have similar qualities to bulk materials. However, even large particles with finite volumes exhibit distinct properties from the bulk condensed phase, due in part to their higher surface-to-volume ratio and their ability to easily access supersaturated solute states inaccessible in the bulk. Aerosols represent a major challenge for study because of the facile coupling between the particle and gas, the small amounts of sample available for analysis, and the sheer breadth of operative processes. Time scales of aerosol processes can be as short as nanoseconds or as long as years. Despite their very different impacts and applications, fundamental chemical physics processes serve as a common theme that underpins our understanding of aerosols. This perspective article discusses challenges in the study of aerosols and highlights recent chemical physics advancements that have enabled improved understanding of these complex systems.

A facility for gas- and condensed-phase measurements behind shock waves

NASA Astrophysics Data System (ADS)

Petersen, Eric L.; Rickard, Matthew J. A.; Crofton, Mark W.; Abbey, Erin D.; Traum, Matthew J.; Kalitan, Danielle M.

2005-09-01

A shock-tube facility consisting of two, single-pulse shock tubes for the study of fundamental processes related to gas-phase chemical kinetics and the formation and reaction of solid and liquid aerosols at elevated temperatures is described. Recent upgrades and additions include a new high-vacuum system, a new gas-handling system, a new control system and electronics, an optimized velocity-detection scheme, a computer-based data acquisition system, several optical diagnostics, and new techniques and procedures for handling experiments involving gas/powder mixtures. Test times on the order of 3 ms are possible with reflected-shock pressures up to 100 atm and temperatures greater than 4000 K. Applications for the shock-tube facility include the study of ignition delay times of fuel/oxidizer mixtures, the measurement of chemical kinetic reaction rates, the study of fundamental particle formation from the gas phase, and solid-particle vaporization, among others. The diagnostic techniques include standard differential laser absorption, FM laser absorption spectroscopy, laser extinction for particle volume fraction and size, temporally and spectrally resolved emission from gas-phase species, and a scanning mobility particle sizer for particle size distributions. Details on the set-up and operation of the shock tube and diagnostics are given, the results of a detailed uncertainty analysis on the accuracy of the test temperature inferred from the incident-shock velocity are provided, and some recent results are presented.

Mixing of secondary organic aerosols versus relative humidity

PubMed Central

Ye, Qing; Robinson, Ellis Shipley; Ding, Xiang; Ye, Penglin

2016-01-01

Atmospheric aerosols exert a substantial influence on climate, ecosystems, visibility, and human health. Although secondary organic aerosols (SOA) dominate fine-particle mass, they comprise myriad compounds with uncertain sources, chemistry, and interactions. SOA formation involves absorption of vapors into particles, either because gas-phase chemistry produces low-volatility or semivolatile products that partition into particles or because more-volatile organics enter particles and react to form lower-volatility products. Thus, SOA formation involves both production of low-volatility compounds and their diffusion into particles. Most chemical transport models assume a single well-mixed phase of condensing organics and an instantaneous equilibrium between bulk gas and particle phases; however, direct observations constraining diffusion of semivolatile organics into particles containing SOA are scarce. Here we perform unique mixing experiments between SOA populations including semivolatile constituents using quantitative, single-particle mass spectrometry to probe any mass-transfer limitations in particles containing SOA. We show that, for several hours, particles containing SOA from toluene oxidation resist exchange of semivolatile constituents at low relative humidity (RH) but start to lose that resistance above 20% RH. Above 40% RH, the exchange of material remains constant up to 90% RH. We also show that dry particles containing SOA from α-pinene ozonolysis do not appear to resist exchange of semivolatile compounds. Our interpretation is that in-particle diffusion is not rate-limiting to mass transfer in these systems above 40% RH. To the extent that these systems are representative of ambient SOA, we conclude that diffusion limitations are likely not common under typical ambient boundary layer conditions. PMID:27791066

Mixing of secondary organic aerosols versus relative humidity.

PubMed

Ye, Qing; Robinson, Ellis Shipley; Ding, Xiang; Ye, Penglin; Sullivan, Ryan C; Donahue, Neil M

2016-10-24

Atmospheric aerosols exert a substantial influence on climate, ecosystems, visibility, and human health. Although secondary organic aerosols (SOA) dominate fine-particle mass, they comprise myriad compounds with uncertain sources, chemistry, and interactions. SOA formation involves absorption of vapors into particles, either because gas-phase chemistry produces low-volatility or semivolatile products that partition into particles or because more-volatile organics enter particles and react to form lower-volatility products. Thus, SOA formation involves both production of low-volatility compounds and their diffusion into particles. Most chemical transport models assume a single well-mixed phase of condensing organics and an instantaneous equilibrium between bulk gas and particle phases; however, direct observations constraining diffusion of semivolatile organics into particles containing SOA are scarce. Here we perform unique mixing experiments between SOA populations including semivolatile constituents using quantitative, single-particle mass spectrometry to probe any mass-transfer limitations in particles containing SOA. We show that, for several hours, particles containing SOA from toluene oxidation resist exchange of semivolatile constituents at low relative humidity (RH) but start to lose that resistance above 20% RH. Above 40% RH, the exchange of material remains constant up to 90% RH. We also show that dry particles containing SOA from α-pinene ozonolysis do not appear to resist exchange of semivolatile compounds. Our interpretation is that in-particle diffusion is not rate-limiting to mass transfer in these systems above 40% RH. To the extent that these systems are representative of ambient SOA, we conclude that diffusion limitations are likely not common under typical ambient boundary layer conditions.

Frequency maps as a probe of secular evolution in the Milky Way

NASA Astrophysics Data System (ADS)

Valluri, Monica

2015-03-01

The frequency analysis of the orbits of halo stars and dark matter particles from a cosmological hydrodynamical simulation of a disk galaxy from the MUGS collaboration (Stinson et al. 2010) shows that even if the shape of the dark matter halo is nearly oblate, only about 50% of its orbits are on short-axis tubes, confirming a previous result: under baryonic condensation all orbit families can deform their shapes without changing orbital type (Valluri et al. 2010). Orbits of dark matter particles and halo stars are very similar reflecting their common accretion origin and the influence of baryons. Frequency maps provide a compact representation of the 6-D phase space distribution that also reveals the history of the halo (Valluri et al. 2012). The 6-D phase space coordinates for a large population of halo stars in the Milky Way that will be obtained from future surveys can be used to reconstruct the phase-space distribution function of the stellar halo. The similarity between the frequency maps of halo stars and dark matter particles (Fig. 1) implies that reconstruction of the stellar halo distribution function can reveal the phase space distribution of the unseen dark matter particles and provide evidence for secular evolution. MV is supported by NSF grant AST-0908346 and the Elizabeth Crosby grant.

Unusual olivine and pyroxene composition in interplanetary dust and unequilibrated ordinary chondrites

NASA Technical Reports Server (NTRS)

Klock, W.; Mckay, D. S.; Thomas, K. L.; Palme, H.

1989-01-01

The presence, in both a number of interplanetary dust particles (IDPs) and in meteorite matrices, of olivine and orthopyroxene grains, low in FeO but containing up to 5 wt pct MnO, is reported. The majority of olivines and pyroxenes in meteorites contain less than 0.5 wt pct MnO. The presence of these low-iron, manganese-enriched (LIME) olivines and pyroxenes in IDPs and meteorites may indicate a link between the origin and history of IDPs and the matrix material of primitive meteorites. The origin of the LIME silicates could be explained by condensation from a gas of solar composition. Forsterite is the first major silicate phase to condense from a solar nebula gas, and Mn, which is not stable as a metal under solar nebula conditions, would condense at about 1100 K as Mn2SiO4 in solid solution with forsterite.

Method for the abatement of hydrogen chloride

DOEpatents

Winston, S.J.; Thomas, T.R.

1975-11-14

A method is described for reducing the amount of hydrogen chloride contained in a gas stream by reacting the hydrogen chloride with ammonia in the gas phase so as to produce ammonium chloride. The combined gas stream is passed into a condensation and collection vessel, and a cyclonic flow is created in the combined gas stream as it passes through the vessel. The temperature of the gas stream is reduced in the vessel to below the condensation temperature of ammonium chloride in order to crystallize the ammonium chloride on the walls of the vessel. The cyclonic flow creates a turbulence which breaks off the larger particles of ammonium chloride which are, in turn, driven to the bottom of the vessel where the solid ammonium chloride can be removed from the vessel. The gas stream exiting from the condensation and collection vessel is further cleaned and additional ammonium chloride is removed by passing through additional filters.

Method for the abatement of hydrogen chloride

DOEpatents

Winston, Steven J.; Thomas, Thomas R.

1977-01-01

The present invention provides a method for reducing the amount of hydrogen chloride contained in a gas stream by reacting the hydrogen chloride with ammonia in the gas phase so as to produce ammonium chloride. The combined gas stream is passed into a condensation and collection vessel and a cyclonic flow is created in the combined gas stream as it passes through the vessel. The temperature of the gas stream is reduced in the vessel to below the condensation temperature of ammonium chloride in order to crystallize the ammonium chloride on the walls of the vessel. The cyclonic flow creates a turbulence which breaks off the larger particles of ammonium chloride which are, in turn, driven to the bottom of the vessel where the solid ammonium chloride can be removed from the vessel. The gas stream exiting from the condensation and collection vessel is further cleaned and additional ammonium chloride is removed by passing through additional filters.

Trapping of water vapor from an atmosphere by condensed silicate matter formed by high-temperature pulse vaporization

NASA Technical Reports Server (NTRS)

Gerasimov, M. V.; Dikov, Yu. P.; Yakovlev, O. I.; Wlotzka, F.

1993-01-01

The origin of planetary atmospheres is thought to be the result of bombardment of a growing planet by massive planetesimals. According to some models, the accumulation of released water vapor and/or carbon dioxide can result in the formation of a dense and hot primordial atmosphere. Among source and sink processes of atmospheric water vapor the formation of hydroxides was considered mainly as rehydration of dehydrated minerals (foresterite and enstatite). From our point of view, the formation of hydroxides is not limited to rehydration. Condensation of small silicate particles in a spreading vapor cloud and their interaction with a wet atmosphere can also result in the origin of hydrated phases which have no genetic connections with initial water bearing minerals. We present results of two experiments of a simulated interaction of condensed silicate matter which originated during vaporization of dry clinopyroxene in a wet helium atmosphere.

Thermodynamic and kinetic theory of nucleation, deliquescence and efflorescence transitions in the ensemble of droplets on soluble particles.

PubMed

Shchekin, Alexander K; Shabaev, Ilya V; Hellmuth, Olaf

2013-02-07

Thermodynamic and kinetic peculiarities of nucleation, deliquescence and efflorescence transitions in the ensemble of droplets formed on soluble condensation nuclei from a solvent vapor have been considered. The interplay of the effects of solubility and the size of condensation nuclei has been analyzed. Activation barriers for the deliquescence and phase transitions and for the reverse efflorescence transition have been determined as functions of the relative humidity of the vapor-gas atmosphere, initial size, and solubility of condensation nuclei. It has been demonstrated that, upon variations in the relative humidity of the atmosphere, the crossover in thermodynamically stable and unstable variables of the droplet state takes place. The physical meaning of stable and unstable variables has been clarified. The kinetic equations for establishing equilibrium and steady distributions of binary droplets have been solved. The specific times for relaxation, deliquescence and efflorescence transitions have been calculated.

Interaction of cationic surfactants with DNA: a single-molecule study

PubMed Central

Husale, Sudhir; Grange, Wilfried; Karle, Marc; Bürgi, Stephan; Hegner, Martin

2008-01-01

The interaction of cationic surfactants with single dsDNA molecules has been studied using force-measuring optical tweezers. For hydrophobic chains of length 12 and greater, pulling experiments show characteristic features (e.g. hysteresis between the pulling and relaxation curves, force-plateau along the force curves), typical of a condensed phase (compaction of a long DNA into a micron-sized particle). Depending on the length of the hydrophobic chain of the surfactant, we observe different mechanical behaviours of the complex (DNA-surfactants), which provide evidence for different binding modes. Taken together, our measurements suggest that short-chain surfactants, which do not induce any condensation, could lie down on the DNA surface and directly interact with the DNA grooves through hydrophobic–hydrophobic interactions. In contrast, long-chain surfactants could have their aliphatic tails pointing away from the DNA surface, which could promote inter-molecular interactions between hydrophobic chains and subsequently favour DNA condensation. PMID:18203749

Ground-State Wave Function with Interactions between Different Species in M-Component Miscible Bose-Einstein Condensates

NASA Astrophysics Data System (ADS)

Kohno, Wataru; Kirikoshi, Akimitsu; Kita, Takafumi

2018-03-01

We construct a variational ground-state wave function of weakly interacting M-component Bose-Einstein condensates beyond the mean-field theory by incorporating the dynamical 3/2-body processes, where one of the two colliding particles drops into the condensate and vice versa. Our numerical results with various masses and particle numbers show that the 3/2-body processes between different particles make finite contributions to lowering the ground-state energy, implying that many-body correlation effects between different particles are essential even in the weak-coupling regime of the Bose-Einstein condensates. We also consider the stability condition for 2-component miscible states using the new ground-state wave function. Through this calculation, we obtain the relation UAB2/UAAUBB < 1 + α , where Uij is the effective contact potential between particles i and j and α is the correction, which originates from the 3/2- and 2-body processes.

Gas-phase kinetics modifies the CCN activity of a biogenic SOA.

PubMed

Vizenor, A E; Asa-Awuku, A A

2018-02-28

Our current knowledge of cloud condensation nuclei (CCN) activity and the hygroscopicity of secondary organic aerosol (SOA) depends on the particle size and composition, explicitly, the thermodynamic properties of the aerosol solute and subsequent interactions with water. Here, we examine the CCN activation of 3 SOA systems (2 biogenic single precursor and 1 mixed precursor SOA system) in relation to gas-phase decay. Specifically, the relationship between time, gas-phase precursor decay and CCN activity of 100 nm SOA is studied. The studied SOA systems exhibit a time-dependent growth of CCN activity at an instrument supersaturation of ∼0.2%. As such, we define a critical activation time, t 50 , above which a 100 nm SOA particle will activate. The critical activation time for isoprene, longifolene and a mixture of the two precursor SOA is 2.01 hours, 2.53 hours and 3.17 hours, respectively. The activation times are then predicted with gas-phase kinetic data inferred from measurements of precursor decay. The gas-phase prediction of t 50 agrees well with CCN measured t 50 (within 0.05 hours of the actual critical times) and suggests that the gas-to-particle phase partitioning may be more significant for SOA CCN prediction than previously thought.

An efficient approach for treating composition-dependent diffusion within organic particles

DOE PAGES

O'Meara, Simon; Topping, David O.; Zaveri, Rahul A.; ...

2017-09-07

Mounting evidence demonstrates that under certain conditions the rate of component partitioning between the gas and particle phase in atmospheric organic aerosol is limited by particle-phase diffusion. To date, however, particle-phase diffusion has not been incorporated into regional atmospheric models. An analytical rather than numerical solution to diffusion through organic particulate matter is desirable because of its comparatively small computational expense in regional models. Current analytical models assume diffusion to be independent of composition and therefore use a constant diffusion coefficient. To realistically model diffusion, however, it should be composition-dependent (e.g. due to the partitioning of components that plasticise, vitrifymore » or solidify). This study assesses the modelling capability of an analytical solution to diffusion corrected to account for composition dependence against a numerical solution. Results show reasonable agreement when the gas-phase saturation ratio of a partitioning component is constant and particle-phase diffusion limits partitioning rate (<10% discrepancy in estimated radius change). However, when the saturation ratio of the partitioning component varies, a generally applicable correction cannot be found, indicating that existing methodologies are incapable of deriving a general solution. Until such time as a general solution is found, caution should be given to sensitivity studies that assume constant diffusivity. Furthermore, the correction was implemented in the polydisperse, multi-process Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) and is used to illustrate how the evolution of number size distribution may be accelerated by condensation of a plasticising component onto viscous organic particles.« less

An efficient approach for treating composition-dependent diffusion within organic particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Meara, Simon; Topping, David O.; Zaveri, Rahul A.

Mounting evidence demonstrates that under certain conditions the rate of component partitioning between the gas and particle phase in atmospheric organic aerosol is limited by particle-phase diffusion. To date, however, particle-phase diffusion has not been incorporated into regional atmospheric models. An analytical rather than numerical solution to diffusion through organic particulate matter is desirable because of its comparatively small computational expense in regional models. Current analytical models assume diffusion to be independent of composition and therefore use a constant diffusion coefficient. To realistically model diffusion, however, it should be composition-dependent (e.g. due to the partitioning of components that plasticise, vitrifymore » or solidify). This study assesses the modelling capability of an analytical solution to diffusion corrected to account for composition dependence against a numerical solution. Results show reasonable agreement when the gas-phase saturation ratio of a partitioning component is constant and particle-phase diffusion limits partitioning rate (<10% discrepancy in estimated radius change). However, when the saturation ratio of the partitioning component varies, a generally applicable correction cannot be found, indicating that existing methodologies are incapable of deriving a general solution. Until such time as a general solution is found, caution should be given to sensitivity studies that assume constant diffusivity. Furthermore, the correction was implemented in the polydisperse, multi-process Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) and is used to illustrate how the evolution of number size distribution may be accelerated by condensation of a plasticising component onto viscous organic particles.« less

Influence of Mineral Dust On New Particle Formation and Growth: A Model Study of Heterogeneous Nucleation

NASA Astrophysics Data System (ADS)

Korhonen, H.; Kulmala, M.; Lauri, A.

Analyses of nucleation events have emphasized the importance of pre-existing par- ticles in new particle formation. When coarse mode aerosol is present, it typically dominates the condensation sink for trace gases and thus inhibits the onset of nucle- ation. A monodisperse aerosol dynamical box model is applied to investigate the effect of soluble coated mineral dust particles on new particle formation. The model in- cludes ternary H2SO4­H2O­NH3 nucleation, multicomponent condensation, coagu- lation and dry deposition. As the soluble coating can significantly change the ability of dust particles to serve as a condensation sink for condensable vapours, different mech- anisms of coating, including heterogeneous nucleation of sulphuric acid, are consid- ered. Preliminary results show that the presence of micron sized soluble coated dust par- ticles can even at relatively low concentrations prevent homogeneous nucleation or growth of nucleated particles to detectable size of 3 nm. Furthermore, critical conden- sation sinks obtained by model simulations correspond to measured sinks.

Balloon-borne measurements of aerosol, condensation nuclei, and cloud particles in the stratosphere at McMurdo Station, Antarctica, during the spring of 1987

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.; Harder, J. W.; Hereford, J. V.

1989-01-01

Measurements of the vertical profile of particles with condensation nuclei counters and eight channel aerosol detectors at McMurdo Station, Antarctica, in 1987 verified observations made in 1986 concerning the absence of upwelling in the polar vortex and the presence of a condensation nuclei layer in conjunction with the ozone hole region. New observations of a bimodal aerosol size distribution, consisting of a large-particle mode mixed in with the small-particle sulfate mode, at temperatures below -79 C are consistent with the presence of nitric acid-water particles at low concentrations. Higher concentrations of large particles were observed in association with nacreous clouds. An unusual particle layer which contained enhanced concentrations of both the small-particle (sulfate) mode and the large-particle (nitric acid) mode was detected at temperatures below -85 C, suggesting simultaneous nucleation and growth phenomena. The vortex condensation nuclei layer was observed to form at the same time as the ozone hole, indicating that formation of the layer is triggered by photochemical processes and may be important in controlling ozone depletion above 22 km.

Formation of Polar Stratospheric Clouds in the Atmosphere

NASA Astrophysics Data System (ADS)

Aloyan, Artash; Yermakov, Alex; Arutyunyan, Vardan; Larin, Igor

2014-05-01

A new mathematical model of the global transport of gaseous species and aerosols in the atmosphere and the formation of polar stratospheric clouds (PSCs) in both hemispheres was constructed. PSCs play a significant role in ozone chemistry since heterogeneous reactions proceed on their particle surfaces and in the bulk, affecting the gas composition of the atmosphere, specifically, the content of chlorine and nitrogen compounds, which are actively involved in the destruction of ozone. Stratospheric clouds are generated by co-condensation of water vapor and nitric acid on sulfate particles and in some cases during the freezing of supercooled water as well as when nitric acid vapors are dissolved in sulfate aerosol particles [1]. These clouds differ in their chemical composition and microphysics [2]. In this study, we propose new kinetic equations describing the variability of species in the gas and condensed phases to simulate the formation of PSCs. Most models for the formation of PSCs use constant background values of sulfate aerosols in the lower stratosphere. This approach is too simplistic since sulfate aerosols in the stratosphere are characterized by considerably nonuniform spatial and temporal variations. Two PSC types are considered: Type 1 refers to the formation of nitric acid trihydrate (NAT) and Type 2 refers to the formation of particles composed of different proportions of H2SO4/HNO3/H2O. Their formation is coupled with the spatial problem of sulfate aerosol generation in the upper troposphere and lower stratosphere incorporating the chemical and kinetic transformation processes (photochemistry, nucleation, condensation/evaporation, and coagulation) and using a non-equilibrium particle-size distribution [3]. In this formulation, the system of equations is closed and allows an adequate description of the PSC dynamics in the stratosphere. Using the model developed, numerical experiments were performed to reproduce the spatial and temporal variability of polar clouds in both hemispheres for the winter time period. The numerical experiments were performed in the following sequence. In the first stage, we address the transport of multicomponent gaseous species, the formation of sulfate aerosols in the troposphere and lower stratosphere (spherical atmosphere), the chemical and kinetic transformations, and the biogenic and anthropogenic emissions of related chemical components [3]. This model makes it possible to reproduce the distribution of sulfate particles in the size range from 3 nm to 1 mcm. Next, the base model was improved by using a new module describing the dynamics of phase transition of substances in gaseous and condensed phases that are typical for different types of PSCs. Here, we used the methods of thermodynamics. Conclusions •The model developed allow us to reproduce the size distribution of sulfate particles generated from precursor gases in the troposphere and stratosphere; •The numerical experiments show that the model adequately reproduces the spatial characteristics of the PSC formation in the atmosphere. References 1.Carslaw K.S., Peter T., Clegg S.L. Modeling the composition of liquid stratospheric clouds. Rev. Geophys. 35, 125, 1997 2.Drdla, K., Shoeberl, M.R., and Browell, E.V., Microphysical modeling of the 1999-2000 Arctic winter. J. Geophys. Res., 2003, vol. 108, No. D5, p. 8312. 3.Aloyan, A.E., Yermakov, A.N., Arutyunyan, V.O., Sulfate aerosol formation in the troposphere and lower stratosphere, in Possibilities of Climate Stabilization by Using Novel Technologies, Moscow: Rosgidromet, 2012, pp. 75-98.

Initial Stage of Aerosol Formation from Oversaturated Vapors

NASA Astrophysics Data System (ADS)

Lushnikov, A. A.; Zagainov, V. A.; Lyubovtseva, Yu. S.

2018-03-01

The formation of aerosol particles from oversaturated vapor was considered assuming that the stable nuclei of the new phase contain two (dimers) or three (trimers) condensing vapor molecules. Exact expressions were derived and analyzed for the partition functions of the dimer and trimer suspended in a carrier gas for the rectangular well and repulsive core intermolecular potentials. The equilibrium properties of these clusters and the nucleation rate of aerosol particles were discussed. The bound states of clusters were introduced using a limitation on their total energy: molecular clusters with a negative total energy were considered to exclude configurations with noninteracting fragments.

Condensation and transport in the totally asymmetric inclusion process (TASIP)

NASA Astrophysics Data System (ADS)

Knebel, Johannes; Weber, Markus F.; Krueger, Torben; Frey, Erwin

Transport phenomena are often modeled by the hopping of particles on regular lattices or networks. Such models describe, e.g., the exclusive movement of molecular motors along microtubules: no two motors may occupy the same site. In our work, we study inclusion processes that are the bosonic analogues of the fermionic exclusion processes. In inclusion processes, many particles may occupy a single site and hopping rates depend linearly on the occupation of departure and arrival sites. Particles thus attract other particles to their own site. Condensation occurs when particles collectively cluster in one or multiple sites, whereas other sites become depleted.We showed that inclusion processes describe both the selection of strategies in evolutionary zero-sum games and the condensation of non-interacting bosons into multiple quantum states in driven-dissipative systems. The condensation is captured by the antisymmetric Lotka-Volterra equation (ALVE), which constitutes a nonlinearly coupled dynamical system. We derived an algebraic method to analyze the ALVE and to determine the condensates. Our approach allows for the design of networks that result in condensates with oscillating occupations, and yields insight into the interplay between network topology and transport properties. Deutsche Forschungsgemeinschaft (SFB-TR12), German Excellence Initiative (Nanosystems Initiative Munich), Center for NanoScience Munich.

Uncertainties in SOA Formation from the Photooxidation of α-pinene

NASA Astrophysics Data System (ADS)

McVay, R.; Zhang, X.; Aumont, B.; Valorso, R.; Camredon, M.; La, S.; Seinfeld, J.

2015-12-01

Explicit chemical models such as GECKO-A (the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere) enable detailed modeling of gas-phase photooxidation and secondary organic aerosol (SOA) formation. Comparison between these explicit models and chamber experiments can provide insight into processes that are missing or unknown in these models. GECKO-A is used to model seven SOA formation experiments from α-pinene photooxidation conducted at varying seed particle concentrations with varying oxidation rates. We investigate various physical and chemical processes to evaluate the extent of agreement between the experiments and the model predictions. We examine the effect of vapor wall loss on SOA formation and how the importance of this effect changes at different oxidation rates. Proposed gas-phase autoxidation mechanisms are shown to significantly affect SOA predictions. The potential effects of particle-phase dimerization and condensed-phase photolysis are investigated. We demonstrate the extent to which SOA predictions in the α-pinene photooxidation system depend on uncertainties in the chemical mechanism.

Self-assembly and electrostriction of arrays and chains of hopfion particles in chiral liquid crystals

PubMed Central

Ackerman, Paul J.; van de Lagemaat, Jao; Smalyukh, Ivan I.

2015-01-01

Some of the most exotic condensed matter phases, such as twist grain boundary and blue phases in liquid crystals and Abrikosov phases in superconductors, contain arrays of topological defects in their ground state. Comprised of a triangular lattice of double-twist tubes of magnetization, the so-called ‘A-phase’ in chiral magnets is an example of a thermodynamically stable phase with topologically nontrivial solitonic field configurations referred to as two-dimensional skyrmions, or baby-skyrmions. Here we report that three-dimensional skyrmions in the form of double-twist tori called ‘hopfions’, or ‘torons’ when accompanied by additional self-compensating defects, self-assemble into periodic arrays and linear chains that exhibit electrostriction. In confined chiral nematic liquid crystals, this self-assembly is similar to that of liquid crystal colloids and originates from long-range elastic interactions between particle-like skyrmionic torus knots of molecular alignment field, which can be tuned from isotropic repulsive to weakly or highly anisotropic attractive by low-voltage electric fields. PMID:25607778

Product study of oleic acid ozonolysis as function of humidity

NASA Astrophysics Data System (ADS)

Vesna, O.; Sax, M.; Kalberer, M.; Gaschen, A.; Ammann, M.

The heterogeneous reaction of ozone with oleic acid (OA) aerosol particles was studied as function of humidity and reaction time in an aerosol flow reactor using an off-line gas chromatography mass spectrometry (GC-MS) technique. We report quantitative yields of the major C9 ozonolysis products in both gas and condensed phases and the effect of relative humidity on the product distribution. The measurements were carried out with OA aerosol particles at room temperature. The results indicate that the product yields are increasing with increasing relative humidity during the reaction. Nonanal (NN) was detected as the major gas-phase product (55.6 ± 2.3%), with 94.5 ± 2.4% of the NN yield in the gas, and 5.5 ± 2.7% in the particulate phase, whereas nonanoic, oxononanoic and azelaic acids were detected exclusively in the particulate phase. Using UV-spectrometry, we observed that peroxides make up the largest fraction of products, about half of the product aerosol mass, and their concentration decreased with increasing humidity.

Laboratory studies of aqueous-phase oxidation of polyols in submicron particles

NASA Astrophysics Data System (ADS)

Daumit, K. E.; Carrasquillo, A. J.; Hunter, J. F.; Kroll, J. H.

2013-12-01

Aqueous-phase oxidation has received recent attention as a potential pathway for the formation of highly oxidized organic aerosol. However most aqueous oxidation studies are performed in bulk solutions rather than aqueous droplets. Here we describe experiments in which aqueous oxidation is carried out within submicron particles, allowing for gas-particle partitioning of reactants, intermediates, and products. Using Fenton chemistry as a source of hydroxyl radicals, and a high-resolution aerosol mass spectrometer (AMS) for online characterization of particle composition, we find that aqueous oxidation can be quite rapid. The formation of high concentrations of oxalic acid is observed in the particle phase with some loss of carbon to the gas phase, indicating the formation of volatile products. We see a rapid degradation of condensed-phase oxidation products upon exposure to ultraviolet lights (centered at 350 nm) suggesting that these products may exist as iron(III)-oxalate complexes. Similar results are also seen when oxidation is carried out in bulk solution (with AMS analysis of the atomized solution); however in some cases the mass loss is less than is observed for submicron particles, likely due to differences in partitioning of early-generation products. Such products can partition out of the aqueous phase at the low liquid water contents in the chamber but remain in solution for further aqueous processing in bulk oxidation experiments. This work suggests that the product distributions from oxidation in aqueous aerosol may be substantially different than those in bulk oxidation, pointing to the need to carry out aqueous oxidation studies under atmospherically relevant partitioning conditions (with liquid water contents mimicking those of cloud droplets or wet aerosol).

Synthesis of condensed phases containing polycyclic aromatic hydrocarbons fullerenes and nanotubes

DOEpatents

Reilly, Peter T. A.

2004-10-19

The invention relates to methods for producing polycyclic aromatic hydrocarbons, fullerenes, and nanotubes, comprising: a. heating at least one carbon-containing material to form a condensed phase comprising at least one polycyclic aromatic hydrocarbon; b. collecting at least some of the condensed phase; c. reacting the condensed phase to form fullerenes and/or nanotubes.

Insight into winter haze formation mechanisms based on aerosol hygroscopicity and effective density measurements

NASA Astrophysics Data System (ADS)

Xie, Yuanyuan; Ye, Xingnan; Ma, Zhen; Tao, Ye; Wang, Ruyu; Zhang, Ci; Yang, Xin; Chen, Jianmin; Chen, Hong

2017-06-01

We characterize a representative particulate matter (PM) episode that occurred in Shanghai during winter 2014. Particle size distribution, hygroscopicity, effective density, and single particle mass spectrometry were determined online, along with offline analysis of water-soluble inorganic ions. The mass ratio of SNA / PM1. 0 (sulfate, nitrate, and ammonium) fluctuated slightly around 0.28, suggesting that both secondary inorganic compounds and carbonaceous aerosols contributed substantially to the haze formation, regardless of pollution level. Nitrate was the most abundant ionic species during hazy periods, indicating that NOx contributed more to haze formation in Shanghai than did SO2. During the representative PM episode, the calculated PM was always consistent with the measured PM1. 0, indicating that the enhanced pollution level was attributable to the elevated number of larger particles. The number fraction of the near-hydrophobic group increased as the PM episode developed, indicating the accumulation of local emissions. Three banana-shaped particle evolutions were consistent with the rapid increase of PM1. 0 mass loading, indicating that the rapid size growth by the condensation of condensable materials was responsible for the severe haze formation. Both hygroscopicity and effective density of the particles increased considerably with growing particle size during the banana-shaped evolutions, indicating that the secondary transformation of NOx and SO2 was one of the most important contributors to the particle growth. Our results suggest that the accumulation of gas-phase and particulate pollutants under stagnant meteorological conditions and subsequent rapid particle growth by secondary processes were primarily responsible for the haze pollution in Shanghai during wintertime.

Towards the identification of molecular constituents associated with the surfaces of isoprene-derived secondary organic aerosol (SOA) particles

NASA Astrophysics Data System (ADS)

Ebben, C. J.; Strick, B. F.; Upshur, M. A.; Chase, H. M.; Achtyl, J. L.; Thomson, R. J.; Geiger, F. M.

2014-03-01

Secondary organic aerosol (SOA) particle formation ranks among the least understood chemical processes in the atmosphere, rooted in part in the lack of knowledge about chemical composition and structure at the particle surface, and little availability of reference compounds needed for benchmarking and chemical identification in pure and homogenous form. Here, we synthesize and characterize SOA particle constituents consisting of the isoprene oxidation products α-, δ-, and cis- and trans-β-IEPOX (isoprene epoxide), as well as syn- and anti-2-methyltetraol. Paying particular attention to their phase state (condensed vs. vapor), we carry out a surface-specific and orientationally selective chemical analysis by vibrational sum frequency generation (SFG) spectroscopy of these compounds in contact with a fused silica window. Comparison to the vibrational SFG spectra of synthetic isoprene-derived SOA particle material prepared at the Harvard Environmental Chamber yields a plausible match with trans-β-IEPOX, suggesting it is an abundant species on their surfaces, while the other species studied here, if present, appear to be SFG inactive and thus likely to be localized in a centrosymmetric environment, e.g., the particle bulk. No match is found for authentic SOA particle material collected at the site of the Amazonian Aerosol Characterization Experiment (AMAZE-08) with the surface SFG spectra of the compounds surveyed here, yet we cannot rule out this mismatch being attributable to differences in molecular orientation. The implications of our findings for SOA formation are discussed in the context of condensational particle growth and reactivity.

Potential origin of organic CNN observed at a marine site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrews, E.; Kreidenweis, S.M.; Penner, J.E.

1995-12-31

Observations by Novakov and Penner (1993) suggest that organic aerosol particles may make up a significant portion of cloud condensation nuclei (CCN) comparable, perhaps, to the sulfate aerosol contribution to CCN. Because organic CCN would influence the albedo and radiative properties of clouds and play a role in climate change, it is important to identify the sources of these aerosols. In their research Novakov and Penner assumed that particles larger than 0.05 {mu}m could act as CCN. Therefore the origins of nucleation mode aerosol (0.03 < dp < 0.1 {mu}m) are the focus of our research. In our research, wemore » apply a dynamic aerosol model (MAEROS) to explore potential sources of the nucleation mode organic aerosol observed at a marine site in Puerto Rico. Novakov and Penner measured the size segregated mass and composition of the atmospheric aerosol at this site and found that organic aerosol mass dominated the sulfate mass in the nucleation size range. The presence of organics in this size range suggests that these organic aerosol particles were generated by nucleation of a gas phase organic followed by condensational processes, i.e., identifying sources of the gas phase precursors is important to determining the organic CCN origins. Back trajectory analysis shows that the air mass was without continental contact for 12 days prior to being sampled. This implicates two possible sources for the gas phase organic: biogenic emissions from the Puerto Rican forest and emissions from the ocean surface. In this research we explore both the forest and ocean source scenarios, showing that the forest is more likely to be the ultimate source of the observed organic aerosol particles. Using MAEROS (modified to include nucleation) and reasonable input parameters taken from the literature we were able to show that an organic vapor flux very similar to the measured biogenic fluxes reported by Zimmerman et al. generated size distributions similar to the observed aerosol.« less

Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

NASA Astrophysics Data System (ADS)

Metcalf, A. R.; Dutcher, C. S.

2014-12-01

Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures containing ammonium salts (e.g., (NH4)2SO4, NH4NO3) and dicarboxylic acids (e.g., malonic, glutaric, and maleic acid) as well as important mimic compounds such as sucrose - water systems.

Selenium Partitioning and Removal Across a Wet FGD Scrubber at a Coal-Fired Power Plant.

PubMed

Senior, Constance L; Tyree, Corey A; Meeks, Noah D; Acharya, Chethan; McCain, Joseph D; Cushing, Kenneth M

2015-12-15

Selenium has unique fate and transport through a coal-fired power plant because of high vapor pressures of oxide (SeO2) in flue gas. This study was done at full-scale on a 900 MW coal-fired power plant with electrostatic precipitator (ESP) and wet flue gas desulfurization (FGD) scrubber. The first objective was to quantify the partitioning of selenium between gas and condensed phases at the scrubber inlet and outlet. The second objective was to determine the effect of scrubber operation conditions (pH, mass transfer, SO2 removal) on Se removal in both particulate and vapor phases. During part of the testing, hydrated lime (calcium hydroxide) was injected upstream of the scrubber. Gas-phase selenium and particulate-bound selenium were measured as a function of particle size at the inlet and outlet of the scrubber. The total (both phases) removal of Se across the scrubber averaged 61%, and was enhanced when hydrated lime sorbent was injected. There was evidence of gas-to-particle conversion of selenium across the scrubber, based on the dependence of selenium concentration on particle diameter downstream of the scrubber and on thermodynamic calculations.

Shock wave induced condensation in fuel-rich gaseous and gas-particles mixtures

NASA Astrophysics Data System (ADS)

Fomin, P. A.

2018-03-01

The possibility of fuel vapor condensation in shock waves in fuel-rich (cyclohexane-oxygen) gaseous mixtures and explosion safety aspects of this effect are discussed. It is shown, that condensation process can essentially change the chemical composition of the gas. For example, the molar fraction of the oxidizer can increase in a few times. As a result, mixtures in which the initial concentration of fuel vapor exceeds the Upper Flammability Limit can, nevertheless, explode, if condensation shifts the composition of the mixture into the ignition region. The rate of the condensation process is estimated. This process can be fast enough to significantly change the chemical composition of the gas and shift it into the flammable range during the compression phase of blast waves, generated by explosions of fuel-vapor clouds or rapture of pressurized chemical reactors, with characteristic size of a few meters. It is shown that the presence of chemically inert microparticles in the gas mixtures under consideration increases the degree of supercooling and the mass of fuel vapors that have passed into the liquid and reduces the characteristic condensation time in comparison with the gas mixture without microparticles. The fuel vapor condensation should be taken into account in estimation the explosion hazard of chemical reactors, industrial and civil constructions, which may contain fuel-rich gaseous mixtures of heavy hydrocarbons with air.

A Numerical Study of Convection in a Condensing CO2 Atmosphere under Early Mars-Like Conditions

NASA Astrophysics Data System (ADS)

Nakajima, Kensuke; Yamashita, Tatsuya; Odaka, Masatsugu; Sugiyama, Ko-ichiro; Ishiwatari, Masaki; Nishizawa, Seiya; Takahashi, Yoshiyuki O.; Hayashi, Yoshi-Yuki

2017-10-01

Cloud convection of a CO2 atmosphere where the major constituent condenses is numerically investigated under a setup idealizing a possible warm atmosphere of early Mars, utilizing a two-dimensional cloud-resolving model forced by a fixed cooling profile as a substitute for a radiative process. The authors compare two cases with different critical saturation ratios as condensation criteria and also examine sensitivity to number mixing ratio of condensed particles given externally.When supersaturation is not necessary for condensation, the entire horizontal domain above the condensation level is continuously covered by clouds irrespective of number mixing ratio of condensed particles. Horizontal-mean cloud mass density decreases exponentially with height. The circulations below and above the condensation level are dominated by dry cellular convection and buoyancy waves, respectively.When 1.35 is adopted as the critical saturation ratio, clouds appear exclusively as intense, short-lived, quasi-periodic events. Clouds start just above the condensation level and develop upward, but intense updrafts exist only around the cloud top; they do not extend to the bottom of the condensation layer. The cloud layer is rapidly warmed by latent heat during the cloud events, and then the layer is slowly cooled by the specified thermal forcing, and supersaturation gradually develops leading to the next cloud event. The periodic appearance of cloud events does not occur when number mixing ratio of condensed particles is large.

The Effect of Organic Compounds on the Hygroscopic Properties of Inorganic Aerosol

NASA Astrophysics Data System (ADS)

Krieger, U. K.; Zardini, A. A.; Marcolli, C.

2006-12-01

The hygroscopicity of the aerosols plays a major role for the direct and indirect effect on the climate. It is known that aerosols are often a mixture of inorganic and organic matter. A significant fraction of the organic matter is water soluble (WSOC) and affects light scattering, water uptake and phase transitions of multicomponent aerosols. Additionally, organic matter can act as a surfactant around an inorganic particle, affecting the evaporation-condensation time scale. This research project benefits from the combined measurements performed by two different instrumentations: the electrodynamic trap at IACETH, Zürich, Switzerland, and a Tandem Differential Mobility Analizer (TDMA) at the Paul Scherrer Institute, Switzerland. The Electrodynamic Trap consists of a chamber in which a levitated particle can experience all the atmospherically relevant conditions of temperature, pressure, and humidity. All these parameters can be continuously varied so that the hygroscopic curve of the aerosol particle can be measured. Additional tools help to better characterize the aerosol particle: 90 degrees angular scattering of lasers (for radius measurements) and intensity fluctuation of the scattered light with time (for phase changes detection). In this poster the results obtained through the electrodynamic balance technique will be shown and compared with the TDMA. In particular, bicomponent ammonium sulphate with adipic acid bicomponent particles are studied, with different mixing ratios. Particular emphasis is put on assessing the water uptake and the phase changes of the particles.

Laboratory Studies of Optical Characteristics and Condensation Processes of Cosmic Dust Particles

NASA Technical Reports Server (NTRS)

Spann, J. F., Jr.; Abbas, M. M.; Venturini, C. C.

2000-01-01

Information about the optical characteristics and physical processes involving cosmic dust particles is vital for interpretation of astronomical observations and an understanding of the formation and processing of dust in the evolutionary cycle of matter in the interstellar medium. Cosmic dust particles are formed in a variety of astrophysical environments such as in cool stellar outflows and circumstellar envelopes. Definitive knowledge of the nature, composition, and physical processes of cosmic dust grains, however, can only be inferred from astronomical observations through laboratory experiments on the analogs of hypothesized dust particles and with modeling calculations. Laboratory investigations of the nature, composition, and optical characteristics of cosmic dust particles are being, carried out at many institutions with a variety of experimental techniques. Despite a wealth of available data, however, many basic issues remain unresolved. An experimental facility based on suspension of dust particles in electrodynamic balance in a pressure/temperature controlled environment in a cavity has been operational at the NASA Marshall Space Flight Center, and is currently being employed for studies of dust particle charging mechanisms using electron beams and with UV radiation. In this paper, we discuss two general classes of experiments under planning stages that may be simultaneously carried out on this facility for cosmic dust investigations (i) Infrared optical characteristics (extinction coefficients and scattering phase functions) of the analogs of hypothesized of cosmic dust particles, such as natural and synthetic amorphous silicates with varying compositions, amorphous carbon grains, polycyclic aromatic hydrocarbons (PAHs), and icy core-mantle particles etc. The initial spectral range under consideration is 1-25 micrometers, to be extended to the far infrared region in the future (ii) Condensation of volatile gases on nucleus dust particles to be investigated for planetary and astrophysical environments.

Propagation of a Chemical Reaction through Heterogeneous Lithium- Polytetrafluoroethylene Mixtures

DTIC Science & Technology

1975-12-11

Condensed Phases ........... ............... 9 1.2.1 Lithium-Gas Surface Reactions. .......... 10 1.2.2 Composite Solid Propellant Combustion. . .. 13...f:- the o:cu:=ence _A a surface reaction was developed, but no analyti7al reaction zate model was presented- 1.2.2 Composite S’-lid Propellant...Combustion Composite solid propellants are plastic-like materials consisting of small oxidizer particles embedded in a fuel matrix. Ammonium perchlorate is

From particle condensation to polymer aggregation

NASA Astrophysics Data System (ADS)

Janke, Wolfhard; Zierenberg, Johannes

2018-01-01

We draw an analogy between droplet formation in dilute particle and polymer systems. Our arguments are based on finite-size scaling results from studies of a two-dimensional lattice gas to three-dimensional bead-spring polymers. To set the results in perspective, we compare with in part rigorous theoretical scaling laws for canonical condensation in a supersaturated gas at fixed temperature, and derive corresponding scaling predictions for an undercooled gas at fixed density. The latter allows one to efficiently employ parallel multicanonical simulations and to reach previously not accessible scaling regimes. While the asymptotic scaling can not be observed for the comparably small polymer system sizes, they demonstrate an intermediate scaling regime also observable for particle condensation. Altogether, our extensive results from computer simulations provide clear evidence for the close analogy between particle condensation and polymer aggregation in dilute systems.

Probing exoplanet clouds with optical phase curves.

PubMed

Muñoz, Antonio García; Isaak, Kate G

2015-11-03

Kepler-7b is to date the only exoplanet for which clouds have been inferred from the optical phase curve--from visible-wavelength whole-disk brightness measurements as a function of orbital phase. Added to this, the fact that the phase curve appears dominated by reflected starlight makes this close-in giant planet a unique study case. Here we investigate the information on coverage and optical properties of the planet clouds contained in the measured phase curve. We generate cloud maps of Kepler-7b and use a multiple-scattering approach to create synthetic phase curves, thus connecting postulated clouds with measurements. We show that optical phase curves can help constrain the composition and size of the cloud particles. Indeed, model fitting for Kepler-7b requires poorly absorbing particles that scatter with low-to-moderate anisotropic efficiency, conclusions consistent with condensates of silicates, perovskite, and silica of submicron radii. We also show that we are limited in our ability to pin down the extent and location of the clouds. These considerations are relevant to the interpretation of optical phase curves with general circulation models. Finally, we estimate that the spherical albedo of Kepler-7b over the Kepler passband is in the range 0.4-0.5.

Ignition and Combustion of Bulk Metals in a Microgravity Environment

NASA Technical Reports Server (NTRS)

Branch, Melvyn C.; Daily, John W.; Abbud-Madrid, Angel

1999-01-01

Results of a study of heterogeneous and homogeneous combustion of metals in reduced gravity are presented. Cylindrical titanium and magnesium samples are radiatively ignited in pure-oxygen at 1 atm. Qualitative observations, propagation rates, and burning times are extracted from high-speed cinematography. Time-resolved emission spectra of gas-phase reactions are acquired with an imaging spectrograph. Lower propagation rates of the reacting mass on titanium and of ignition waves on magnesium are obtained at reduced gravity. These rates are compared to theoretical results from fire-spread analyses with a diffusion/convection controlled reaction. The close agreement found between experimental and theoretical propagation rates indicates the strong influence of natural-convection-enhanced oxygen transp6rt on burning rates. Lower oxygen flux and lack of condensed product removal appear to be responsible for longer burning times of magnesium gas-phase diffusion flames in reduced gravity. Spherically symmetric explosions in magnesium flames at reduced gravity (termed radiation-induced metal explosions, or RIME) may be driven by increased radiation heat transfer from accumulated condensed products to an evaporating metal core covered by a porous, flexible oxide coating. In titanium specimens, predominantly heterogeneous burning characterizes the initial steady propagation of the molten mass, while homogeneous gas-phase reactions are detected around particles ejected from the molten mixture. In magnesium specimens, band and line reversal of all the UV spectral systems of Mg and MgO are attributed to the interaction between small oxide particles and the principal gaseous emitters.

Ship Tracks

Atmospheric Science Data Center

2013-04-19

... into a moist layer of atmosphere. The particles become cloud condensation nuclei (CCN), which may either produce new cloud particles where ... visualization of the vertical structure of the condensation trails. It was created using a combination of red band data from ...

Condensation heat transfer and flow friction in silicon microchannels

NASA Astrophysics Data System (ADS)

Wu, Huiying; Wu, Xinyu; Qu, Jian; Yu, Mengmeng

2008-11-01

An experimental investigation was performed on heat transfer and flow friction characteristics during steam condensation flow in silicon microchannels. Three sets of trapezoidal silicon microchannels, with hydraulic diameters of 77.5 µm, 93.0 µm and 128.5 µm respectively, were tested under different flow and cooling conditions. It was found that both the condensation heat transfer Nusselt number (Nu) and the condensation two-phase frictional multiplier (phi2Lo) were dependent on the steam Reynolds number (Rev), condensation number (Co) and dimensionless hydraulic diameter (Dh/L). With the increase in the steam Reynolds number, condensation number and dimensionless hydraulic diameter, the condensation Nusselt number increased. However, different variations were observed for the condensation two-phase frictional multiplier. With the increase in the steam Reynolds number and dimensionless hydraulic diameter, the condensation two-phase frictional multiplier decreased, while with the increase in the condensation number, the condensation two-phase frictional multiplier increased. Based on the experimental results, dimensionless correlations for condensation heat transfer and flow friction in silicon microchannels were proposed for the first time. These correlations can be used to determine the condensation heat transfer coefficient and pressure drop in silicon microchannels if the steam mass flow rate, cooling rate and geometric parameters are fixed. It was also found that the condensation heat transfer and flow friction have relations to the injection flow (a transition flow pattern from the annular flow to the slug/bubbly flow), and with injection flow moving toward the outlet, both the condensation heat transfer coefficient and the condensation two-phase frictional multiplier increased.

Direct Lattice Shaking of Bose Condensates: Finite Momentum Superfluids

DOE PAGES

Anderson, Brandon M.; Clark, Logan W.; Crawford, J

2017-05-31

Here, we address band engineering in the presence of periodic driving by numerically shaking a lattice containing a bosonic condensate. By not restricting to simplified band structure models we are able to address arbitrary values of the shaking frequency, amplitude, and interaction strengths g. For "near-resonant" shaking frequencies with moderate g, a quantum phase transition to a finite momentum superfluid is obtained with Kibble-Zurek scaling and quantitative agreement with experiment. We use this successful calibration as a platform to support a more general investigation of the interplay between (one particle) Floquet theory and the effects associated with arbitrary g. Bandmore » crossings lead to superfluid destabilization, but where this occurs depends on g in a complicated fashion.« less

Emergent phases of fractonic matter

NASA Astrophysics Data System (ADS)

Prem, Abhinav; Pretko, Michael; Nandkishore, Rahul M.

2018-02-01

Fractons are emergent particles which are immobile in isolation, but which can move together in dipolar pairs or other small clusters. These exotic excitations naturally occur in certain quantum phases of matter described by tensor gauge theories. Previous research has focused on the properties of small numbers of fractons and their interactions, effectively mapping out the "standard model" of fractons. In the present work, however, we consider systems with a finite density of either fractons or their dipolar bound states, with a focus on the U (1 ) fracton models. We study some of the phases in which emergent fractonic matter can exist, thereby initiating the study of the "condensed matter" of fractons. We begin by considering a system with a finite density of fractons, which we show can exhibit microemulsion physics, in which fractons form small-scale clusters emulsed in a phase dominated by long-range repulsion. We then move on to study systems with a finite density of mobile dipoles, which have phases analogous to many conventional condensed matter phases. We focus on two major examples: Fermi liquids and quantum Hall phases. A finite density of fermionic dipoles will form a Fermi surface and enter a Fermi liquid phase. Interestingly, this dipolar Fermi liquid exhibits a finite-temperature phase transition, corresponding to an unbinding transition of fractons. Finally, we study chiral two-dimensional phases corresponding to dipoles in "quantum Hall" states of their emergent magnetic field. We study numerous aspects of these generalized quantum Hall systems, such as their edge theories and ground state degeneracies.

Size distributions of secondary and primary aerosols in Asia: A 3-D modeling

NASA Astrophysics Data System (ADS)

Yu, F.; Luo, G.; Wang, Z.

2009-12-01

Asian aerosols have received increasing attention because of their potential health and climate effects and the rapid increasing of Asian emissions associated with accelerating economic expansion. Aerosol particles appear in the atmosphere due to either in-situ nucleation (i.e, secondary particles) or direct emissions (i.e., primary particles), and their environmental impacts depend strongly on their concentrations, sizes, compositions, and mixing states. A size-resolved (sectional) particle microphysics model with a number of computationally efficient schemes has been incorporated into a global chemistry transport model (GEOS-Chem) to simulate the number size distributions of secondary and primary particles in the troposphere (Yu and Luo, Atmos. Chem. Phys. Discuss., 9, 10597-10645, 2009). The growth of nucleated particles through the condensation of sulfuric acid vapor and equilibrium uptake of nitrate, ammonium, and secondary organic aerosol is explicitly simulated, along with the coating of primary particles (dust, black carbon, organic carbon, and sea salt) by volatile components via condensation and coagulation with secondary particles. Here we look into the spatiotemporal variations of the size distributions of secondary and primary aerosols in Asia. The annual mean number concentration of the accumulation mode particles (dry diameter > ~ 100 nm) in the lower troposphere over Asia (especially China) is very high and is dominated (~70-90%) by carbonaceous primary particles (with coated condensable species). Coagulation and condensation turn the primary particles into mixed particles and on average increase the dry sizes of primary particles by a factor of ~ 2-2.5. Despite of high condensation sink, sulfuric acid vapor concentration in many parts of Asian low troposphere is very high (annual mean values above 1E7/cm3) and significant new particle formation still occurs. Secondary particles generally dominate the particles small than 100 nm and the equilibrium uptake of nitrate, ammonium, and secondary organic aerosol contributes significantly to the growth of these particles. The vertical profiles of particle number size distributions at representative locations show significant spatial variations (both horizontally and vertically). Our simulations also indicate substantial seasonal variations of particle size distributions.

Simulation of the effects of aerosol on mixed-phase orographic clouds using the WRF model with a detailed bin microphysics scheme

NASA Astrophysics Data System (ADS)

Xiao, Hui; Yin, Yan; Jin, Lianji; Chen, Qian; Chen, Jinghua

2015-08-01

The Weather Research Forecast (WRF) mesoscale model coupled with a detailed bin microphysics scheme is used to investigate the impact of aerosol particles serving as cloud condensation nuclei and ice nuclei on orographic clouds and precipitation. A mixed-phase orographic cloud developed under two scenarios of aerosol (a typical continental background and a relatively polluted urban condition) and ice nuclei over an idealized mountain is simulated. The results show that, when the initial aerosol condition is changed from the relatively clean case to the polluted scenario, more droplets are activated, leading to a delay in precipitation, but the precipitation amount over the terrain is increased by about 10%. A detailed analysis of the microphysical processes indicates that ice-phase particles play an important role in cloud development, and their contribution to precipitation becomes more important with increasing aerosol particle concentrations. The growth of ice-phase particles through riming and Wegener-Bergeron-Findeisen regime is more effective under more polluted conditions, mainly due to the increased number of droplets with a diameter of 10-30 µm. Sensitivity tests also show that a tenfold increase in the concentration of ice crystals formed from ice nucleation leads to about 7% increase in precipitation, and the sensitivity of the precipitation to changes in the concentration and size distribution of aerosol particles is becoming less pronounced when the concentration of ice crystals is also increased.

Particle-bound benzene from diesel engine exhaust.

PubMed

Muzyka, V; Veimer, S; Shmidt, N

1998-12-01

The large surface area of the carbon core of diesel exhaust particles may contribute to the adsorption or condensation of such volatile carcinogenic organic compounds as benzene. The attention of this study focused on determining the distribution of benzene between the gas and particulate phases in the breathing zone of bus garage workers. Benzene and suspended particulate matter were evaluated jointly in the air of a municipal bus garage. Personal passive monitors were used for benzene sampling in the breathing zone of the workers. Active samplers were used for sampling diesel exhaust particles and the benzene associated with them. The benzene levels were measured by gas chromatography. Diesel engine exhaust from buses was the main source of air pollution caused by benzene and particles in this study. The concentration of benzene in the gas and particulate phases showed a wide range of variation, depending on the distance of the workplace from the operating diesel engine. Benzene present in the breathing zone of the workers was distributed between the gas and particulate phases. The amounts of benzene associated with particles were significantly lower in summer than in winter. The particulate matter of diesel exhaust contains benzene in amounts comparable to the concentrations of carcinogenic polycyclic aromatic hydrocarbons (PAH) and the usually found nitro-PAH. The concentration of benzene in the gas phase and in the suspended particulate matter of air can serve as an additional indicator of exposure to diesel exhaust and its carcinogenicity.

Influence of organic films on the evaporation and condensation of water in aerosol

PubMed Central

Davies, James F.; Miles, Rachael E. H.; Haddrell, Allen E.; Reid, Jonathan P.

2013-01-01

Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [CnH(2n+1)OH], with the value decreasing from 2.4 × 10−3 to 1.7 × 10−5 as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid. PMID:23674675

Influence of organic films on the evaporation and condensation of water in aerosol.

PubMed

Davies, James F; Miles, Rachael E H; Haddrell, Allen E; Reid, Jonathan P

2013-05-28

Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [C(n)H(2n+1)OH], with the value decreasing from 2.4 × 10(-3) to 1.7 × 10(-5) as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid.

Control of dispersed-phase temperature in plasma flows by the spectral-brightness pyrometry method

NASA Astrophysics Data System (ADS)

Dolmatov, A. V.; Gulyaev, I. P.; Gulyaev, P. Yu; Iordan, V. I.

2016-02-01

In the present work, we propose a new method for measuring the distribution of temperature in the ensembles of condensed-phase particles in plasma spray flows. Interrelation between the spectral temperature of the particles and the distribution of camera brightness signal is revealed. The established inter-relation enables an in-situ calibration of measuring instruments using the objects under study. The spectral-brightness pyrometry method was approbated on a Plazer plasma-arc wire spraying facility at the Paton Institute of Electrical Welding (Ukrainian Academy of Sciences, Kiev) and on the Thermoplasma 50-1 powder spraying facility at the Institute of Theoretical and Applied Mechanics (Russian Academy of Sciences, Siberian Branch, Novosibirsk). The work was supported by the Russian Foundation for Basic Research (Grants Nos. 14-08-90428 and 15-48-00100).

Effect of Morphology and Composition on the Hygroscopicity of Soot Aerosols

NASA Astrophysics Data System (ADS)

Williams, L.; Slowik, J.; Davidovits, P.; Jayne, J.; Kolb, C.; Worsnop, D.; Rudich, Y.

2003-12-01

Freshly generated soot aerosols are initially hydrophobic and unlikely to act as cloud condensation nuclei (CCN). However, during combustion many low vapor pressure gas products are formed that may then condense on existing soot aerosols. Additionally, soot particles may acquire coatings as they age, such as acids, salts, and oxygenated organics. An understanding of this aging process and its effect on soot hygroscopicity is necessary to address the potential of soot to act as a CCN. The transformation of soot from hydrophobic to hydrophilic is the focus of this work. An aim here is to determine the minimum coating required for hygroscopic growth. Soot particles produced by combustion of mixtures of fuel and air are size selected by a Differential Mobility Analyzer (DMA) and entrained in a laminar flow passing through a flow tube. The size selected soot particles are mixed with a controlled amount of the gas phase precursors to produce the coatings to be studied. Initial studies are focused on coatings of H2SO4, NH4NO3, and selected organics. The number of particles per unit volume of air is counted by a Condensation Particle Counter (CPC) and the particles are isokinetically sampled into an Aerosol Mass Spectrometer (AMS). Two distinct types of soot aerosols have been observed depending on the type of fuel and air mixture. With soot produced by the combustion of propane and air, the AMS shows a polydisperse particle size distribution with aerodynamic diameters ranging from 100 nm to 400 nm. The aerodynamic diameter is linearly related to the DMA-determined mobility diameter with the product density x shape factor = 1.2. The organic molecules in this soot are mostly PAH compounds. However, when kerosene is added to the propane flame, the soot particle morphology and composition is strikingly altered. While the DMA shows an essentially unchanged mobility diameter distribution, in the range 100 nm to 400, aerodynamic particle diameter is constant at about 100 nm, independent of the mobility diameter. This type of constancy of the aerodynamic diameter has been observed for soot particles in diesel engine exhaust and has been interpreted in terms of a size-dependent effective density. The soot chemical composition is also altered. In this soot the organics are mainly linear hydrocarbons. The differences between these two types of soot with respect to hygroscopicity and effective area are being investigated.

The Influence of Monoterpene and Isoprene Nitrates on the Chemistry and Phase State of Secondary Organic Aerosol in a Low-NOx Mixed Deciduous/Coniferous Forest

NASA Astrophysics Data System (ADS)

Slade, J. H., Jr.; Shepson, P. B.; Desrochers, S. J.; Harvey, R. M.; Wallace, W.; Bui, A.; Griffin, R. J.; Kavassalis, S.; Shi, Q.; Murphy, J. G.; Cook, R.; Connor, M.; Ault, A. P.; Pratt, K.; Alwe, H. D.; Millet, D. B.; Bertman, S. B.; Stevens, P. S.; Wennberg, P. O.; Boor, B.; Petrucci, G.

2016-12-01

Particle phase state plays a key role in secondary organic aerosol (SOA) growth, reactive uptake of gas-phase radicals, and condensed phase reactions, influencing atmospheric composition and clouds. While biogenic SOA derived from isoprene and monoterpene oxidation can exhibit glassy or highly viscous semisolid phase states depending on relative humidity, the lifetimes of important SOA precursors including organic nitrates (ON) can depend on the liquid water content (LWC) and particle acidity. Reactions such as acid-catalyzed hydrolysis of particulate ON (pON) are especially sensitive to changes in aerosol LWC. However, the role of particle phase state on the chemistry of pON, and the chemical transformations of pON on the phase of SOA are poorly understood. During the summer of 2016, as part of the PROPHET - Atmospheric Measurements of Oxidants in Summer (AMOS) field study in a northern Michigan mixed deciduous/coniferous forest, we investigated the production of isoprene (IN) and monoterpene nitrates (MTN) at the ground and canopy levels and their role in particle formation, growth, and phase using a combination of high-resolution chemical ionization and aerosol mass spectrometry techniques, size distribution measurements, and particle bounce factors (BF) using two electrical low pressure impactors operating in parallel. Preliminary derived BF suggest the particles may be in a liquid-like state similar to those measured in other high-humidity and isoprene-rich regions such as the Amazon and Southeastern US. However, maxima in BF are observed during periods of high pON, NO, and IN during the day and high NO2 and MTN at night. Some periods were marked with low pON followed by an increase in particulate organic sulfate (pOS), and decrease in BF. Based on these observations, we hypothesize that acid-catalyzed hydrolysis of pON from IN- and MTN-derived SOA may be driving the transition of pON to pOS, leading to a change in the phase state of SOA. Preliminary results also indicate that the smallest particles can be acidic. We will further explore the role of LWC on the phase state of the particles applying ISORROPIA analysis. Although the PROPHET forest is generally NOx-limited, the work presented here highlights the potential importance of NOx and pON chemistry in dictating the phase state of SOA.

Aerosol simulation including chemical and nuclear reactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marwil, E.S.; Lemmon, E.C.

1985-01-01

The numerical simulation of aerosol transport, including the effects of chemical and nuclear reactions presents a challenging dynamic accounting problem. Particles of different sizes agglomerate and settle out due to various mechanisms, such as diffusion, diffusiophoresis, thermophoresis, gravitational settling, turbulent acceleration, and centrifugal acceleration. Particles also change size, due to the condensation and evaporation of materials on the particle. Heterogeneous chemical reactions occur at the interface between a particle and the suspending medium, or a surface and the gas in the aerosol. Homogeneous chemical reactions occur within the aersol suspending medium, within a particle, and on a surface. These reactionsmore » may include a phase change. Nuclear reactions occur in all locations. These spontaneous transmutations from one element form to another occur at greatly varying rates and may result in phase or chemical changes which complicate the accounting process. This paper presents an approach for inclusion of these effects on the transport of aerosols. The accounting system is very complex and results in a large set of stiff ordinary differential equations (ODEs). The techniques for numerical solution of these ODEs require special attention to achieve their solution in an efficient and affordable manner. 4 refs.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhardwaj, Lakshya; Gaiotto, Davide; Kapustin, Anton

It is possible to describe fermionic phases of matter and spin-topological field theories in 2+1d in terms of bosonic “shadow” theories, which are obtained from the original theory by “gauging fermionic parity”. Furthemore, the fermionic/spin theories are recovered from their shadow by a process of fermionic anyon condensation: gauging a one-form symmetry generated by quasi-particles with fermionic statistics. We apply the formalism to theories which admit gapped boundary conditions. We obtain Turaev-Viro-like and Levin-Wen-like constructions of fermionic phases of matter. Here, we describe the group structure of fermionic SPT phases protected by Z 2f × G. The quaternion group makesmore » a surprise appearance.« less

RESPIRATORY CARCINOGENICITY OF DIESEL FUEL EMISSIONS. FINAL REPORT

EPA Science Inventory

An experiment was carried out to compare the carcinogenicity of diesel exhaust particles (administered by fifteen weekly intratracheal instillations) to that of organic extracts of diesel particles, coke oven emissions, roofing tar condensate and cigarette smoke condensate. Appro...

Dust in brown dwarfs and extra-solar planets. I. Chemical composition and spectral appearance of quasi-static cloud layers

NASA Astrophysics Data System (ADS)

Helling, Ch.; Woitke, P.; Thi, W.-F.

2008-07-01

Aims: Brown dwarfs are covered by dust cloud layers which cause inhomogeneous surface features and move below the observable τ = 1 level during the object's evolution. The cloud layers have a strong influence on the structure and spectral appearance of brown dwarfs and extra-solar planets, e.g. by providing high local opacities and by removing condensable elements from the atmosphere causing a sub-solar metalicity in the atmosphere. We aim at understanding the formation of cloud layers in quasi-static substellar atmospheres that consist of dirty grains composed of numerous small islands of different solid condensates. Methods: The time-dependent description is a kinetic model describing nucleation, growth and evaporation. It is extended to treat gravitational settling and is applied to the static-stationary case of substellar model atmospheres. From the solution of the dust moments, we determine the grain size distribution function approximately which, together with the calculated material volume fractions, provides the basis for applying effective medium theory and Mie theory to calculate the opacities of the composite dust grains. Results: The cloud particles in brown dwarfs and hot giant-gas planets are found to be small in the high atmospheric layers (a ≈ 0.01 μm), and are composed of a rich mixture of all considered condensates, in particular MgSiO3[s], Mg2SiO4[s] and SiO2[s]. As the particles settle downward, they increase in size and reach several 100 μm in the deepest layers. The more volatile parts of the grains evaporate and the particles stepwise purify to form composite particles of high-temperature condensates in the deeper layers, mainly made of Fe[s] and Al2O3[s]. The gas phase abundances of the elements involved in the dust formation process vary by orders of magnitudes throughout the atmosphere. The grain size distribution is found to be relatively broad in the upper atmospheric layers but strongly peaked in the deeper layers. This reflects the cessation of the nucleation process at intermediate heights. The spectral appearance of the cloud layers in the mid IR (7-20 μm) is close to a grey body with only weak broad features of a few percent, mainly caused by MgSiO3[s], and Mg2SiO4[s]. These features are, nevertheless, a fingerprint of the dust in the higher atmospheric layers that can be probed by observations. Conclusions: Our models predict that the gas phase depletion is much weaker than phase-equilibrium calculations in the high atmospheric layers. Because of the low densities, the dust formation process is incomplete there, which results in considerable amounts of left-over elements that might produce stronger and broader neutral metallic lines.

An LES-PBE-PDF approach for modeling particle formation in turbulent reacting flows

NASA Astrophysics Data System (ADS)

Sewerin, Fabian; Rigopoulos, Stelios

2017-10-01

Many chemical and environmental processes involve the formation of a polydispersed particulate phase in a turbulent carrier flow. Frequently, the immersed particles are characterized by an intrinsic property such as the particle size, and the distribution of this property across a sample population is taken as an indicator for the quality of the particulate product or its environmental impact. In the present article, we propose a comprehensive model and an efficient numerical solution scheme for predicting the evolution of the property distribution associated with a polydispersed particulate phase forming in a turbulent reacting flow. Here, the particulate phase is described in terms of the particle number density whose evolution in both physical and particle property space is governed by the population balance equation (PBE). Based on the concept of large eddy simulation (LES), we augment the existing LES-transported probability density function (PDF) approach for fluid phase scalars by the particle number density and obtain a modeled evolution equation for the filtered PDF associated with the instantaneous fluid composition and particle property distribution. This LES-PBE-PDF approach allows us to predict the LES-filtered fluid composition and particle property distribution at each spatial location and point in time without any restriction on the chemical or particle formation kinetics. In view of a numerical solution, we apply the method of Eulerian stochastic fields, invoking an explicit adaptive grid technique in order to discretize the stochastic field equation for the number density in particle property space. In this way, sharp moving features of the particle property distribution can be accurately resolved at a significantly reduced computational cost. As a test case, we consider the condensation of an aerosol in a developed turbulent mixing layer. Our investigation not only demonstrates the predictive capabilities of the LES-PBE-PDF model but also indicates the computational efficiency of the numerical solution scheme.

Combustion of a polymer (PMMA) sphere in microgravity

NASA Technical Reports Server (NTRS)

Yang, Jiann C.; Hamins, Anthony

1995-01-01

Polymer combustion is a highly complicated process where chemical reactions may occur not only in the gas phase, but also in the condensed phase as well as at the solid-gas interphase. The chemistry depends strongly on the coupling between the condensed phase and gas phase phenomena. For some polymers, additional complications arise due to the formation of char layers. For others, the behavior of the condensed phase involves swelling, bubbling, melting, sputtering, and multi-stage combustion. Some of these features bear resemblance to the phenomena observed in coal particle combustion. In addition to its relevance to spacecraft fire safety, the combustion of polymeric materials is related to many applications including solid and hybrid rocket propulsion, and of recent interest, waste incineration . The burning rate is one of the most important parameters used to characterize the combustion of polymers. It has been used to rank the polymer flammability under the same experimental conditions and to evaluate various modes of inhibiting polymer flammability. The main objective of this work is to measure the burning rates of a polymeric material in low gravity. Because of inherent logistical difficulties involved in microgravity experiments, it is impossible to examine a wide spectrum of polymeric materials. It is desirable to investigate a polymer whose combustion is less complicated, and yet will lead to a better understanding of the burning characteristics of other more complicated materials. Therefore, a typical non-charring polymer is selected for use in this experimental study. PMMA (polymethylmethacrylate) has been chosen because its thermo-physical properties are well characterized. Although the combustion of PMMA has been extensively studied in 1G experiments, only a limited amount of work has been conducted in low gravity. A spherical sample geometry is chosen in this study because it is the simplest configuration in terms of the microgravity hardware design requirements. Furthermore, a burning PMMA sphere in microgravity represents a one-dimensional flame with overall combustion characteristics expected to be analogous to the combustion of a liquid fuel droplet, a field with many well-developed theories and models. However, differences can also be expected such as the flame-front standoff ratios and the condensed phase processes occurring during combustion.

The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients

DOE Office of Scientific and Technical Information (OSTI.GOV)

Preston, Thomas C.; Davies, James F.; Wilson, Kevin R.

A new method for measuring diffusion in the condensed phase of single aerosol particles is proposed and demonstrated. The technique is based on the frequency-dependent response of a binary particle to oscillations in the vapour phase of one of its chemical components. Here, we discuss how this physical situation allows for what would typically be a non-linear boundary value problem to be approximately reduced to a linear boundary value problem. For the case of aqueous aerosol particles, we investigate the accuracy of the closed-form analytical solution to this linear problem through a comparison with the numerical solution of the fullmore » problem. Then, using experimentally measured whispering gallery modes to track the frequency-dependent response of aqueous particles to relative humidity oscillations, we determine diffusion coefficients as a function of water activity. The measured diffusion coefficients are compared to previously reported values found using the two common experiments: (i) the analysis of the sorption/desorption of water from a particle after a step-wise change to the surrounding relative humidity and (ii) the isotopic exchange of water between a particle and the vapour phase. The technique presented here has two main strengths: first, when compared to the sorption/desorption experiment, it does not require the numerical evaluation of a boundary value problem during the fitting process as a closed-form expression is available. Second, when compared to the isotope exchange experiment, it does not require the use of labeled molecules. Therefore, the frequency-dependent experiment retains the advantages of these two commonly used methods but does not suffer from their drawbacks.« less

The frequency-dependent response of single aerosol particles to vapour phase oscillations and its application in measuring diffusion coefficients

DOE PAGES

Preston, Thomas C.; Davies, James F.; Wilson, Kevin R.

2017-01-13

A new method for measuring diffusion in the condensed phase of single aerosol particles is proposed and demonstrated. The technique is based on the frequency-dependent response of a binary particle to oscillations in the vapour phase of one of its chemical components. Here, we discuss how this physical situation allows for what would typically be a non-linear boundary value problem to be approximately reduced to a linear boundary value problem. For the case of aqueous aerosol particles, we investigate the accuracy of the closed-form analytical solution to this linear problem through a comparison with the numerical solution of the fullmore » problem. Then, using experimentally measured whispering gallery modes to track the frequency-dependent response of aqueous particles to relative humidity oscillations, we determine diffusion coefficients as a function of water activity. The measured diffusion coefficients are compared to previously reported values found using the two common experiments: (i) the analysis of the sorption/desorption of water from a particle after a step-wise change to the surrounding relative humidity and (ii) the isotopic exchange of water between a particle and the vapour phase. The technique presented here has two main strengths: first, when compared to the sorption/desorption experiment, it does not require the numerical evaluation of a boundary value problem during the fitting process as a closed-form expression is available. Second, when compared to the isotope exchange experiment, it does not require the use of labeled molecules. Therefore, the frequency-dependent experiment retains the advantages of these two commonly used methods but does not suffer from their drawbacks.« less

Photoelectron resonance capture ionization-aerosol mass spectrometry of the ozonolysis products of oleic acid particles: Direct measure of higher molecular weight oxygenates

NASA Astrophysics Data System (ADS)

Zahardis, James; Lafranchi, Brian W.; Petrucci, Giuseppe A.

2005-04-01

The heterogeneous reaction of particle-phase 9-octadecenoic acid (oleic acid) and gas-phase ozone in a flow reactor was studied by photoelectron resonance capture ionization (PERCI) mass spectrometry. This soft ionization technique facilitated one of the first simultaneous, direct observations of all four of the major products predicted for this reaction: nonanal, nonanoic acid, 9-oxononanoic acid, and azelaic acid. In addition, a series of higher molecular weight oxygenated compounds were observed directly for the first time. The proposed structures are all cyclic oxygenates and contain the oxygen-oxygen moiety, including secondary ozonides and cyclic geminal diperoxides. Mechanisms for the formation of these products are proposed. The mechanisms are generally 1,3-dipolar cycloadditions that lead to five- and six-member oxygen-containing rings. The mechanisms are shown to involve short-lived Criegee intermediates reacting with aldehydes and other Criegee intermediates. Atmospheric implications of these higher molecular weight compounds are suggested and include enhancing the fatty acid medium's capacity to act as a source of radicals due to the prominence of the peroxide moiety. The low volatility coupled with the high polarity of these compounds may alter particle phase hygroscopicity that can enhance the cloud condensation nuclei properties of these particles.

Numerical investigation of the effects of iron oxidation reactions on the fume formation mechanism in arc welding

NASA Astrophysics Data System (ADS)

Sanibondi, Paolo

2015-09-01

Fume formation during arc welding has been modelled using a stochastic approach taking into account iron oxidation reactions. The model includes the nucleation and condensation of Fe and FeO vapours, the reaction of gaseous O2 and O on the nanoparticle surface, the coagulation of the nanoparticles including a sintering time as a function of temperature and composition, assuming chemical equilibrium for species in the gaseous phase. Results suggest that fumes generated in gas metal arc welding with oxidizing shielding mixtures are composed of aggregates of primary particles that are nucleated from gas-phase FeO and further oxidized to Fe3O4 and Fe2O3 in the liquid and solid phase, respectively. The composition of the fumes at the end of the formation process depends on the relative initial concentration of Fe and O2 species in the gas mixture and on the diameter of the primary particles that compose the aggregates: as the oxidation reactions are driven by deposition of oxygen on nanoparticle surface, the oxidation of larger particles is slower than that of smaller particles because of their lower surface to volume ratio. Solid-state diffusion is limiting the oxidation process at temperatures lower than 1500 K, inducing the formation of not fully oxidized particles composed of Fe3O4.

Evolution of vehicle exhaust particles in the atmosphere.

PubMed

Canagaratna, Manjula R; Onasch, Timothy B; Wood, Ezra C; Herndon, Scott C; Jayne, John T; Cross, Eben S; Miake-Lye, Richard C; Kolb, Charles E; Worsnop, Douglas R

2010-10-01

Aerosol mass spectrometer (AMS) measurements are used to characterize the evolution of exhaust particulate matter (PM) properties near and downwind of vehicle sources. The AMS provides time-resolved chemically speciated mass loadings and mass-weighted size distributions of nonrefractory PM smaller than 1 microm (NRPM1). Source measurements of aircraft PM show that black carbon particles inhibit nucleation by serving as condensation sinks for the volatile and semi-volatile exhaust gases. Real-world source measurements of ground vehicle PM are obtained by deploying an AMS aboard a mobile laboratory. Characteristic features of the exhaust PM chemical composition and size distribution are discussed. PM mass and number concentrations are used with above-background gas-phase carbon dioxide (CO2) concentrations to calculate on-road emission factors for individual vehicles. Highly variable ratios between particle number and mass concentrations are observed for individual vehicles. NRPM1 mass emission factors measured for on-road diesel vehicles are approximately 50% lower than those from dynamometer studies. Factor analysis of AMS data (FA-AMS) is applied for the first time to map variations in exhaust PM mass downwind of a highway. In this study, above-background vehicle PM concentrations are highest close to the highway and decrease by a factor of 2 by 200 m away from the highway. Comparison with the gas-phase CO2 concentrations indicates that these vehicle PM mass gradients are largely driven by dilution. Secondary aerosol species do not show a similar gradient in absolute mass concentrations; thus, their relative contribution to total ambient PM mass concentrations increases as a function of distance from the highway. FA-AMS of single particle and ensemble data at an urban receptor site shows that condensation of these secondary aerosol species onto vehicle exhaust particles results in spatial and temporal evolution of the size and composition of vehicle exhaust PM on urban and regional scales.

Spin Order and Phase Transitions in Chains of Polariton Condensates.

PubMed

Ohadi, H; Ramsay, A J; Sigurdsson, H; Del Valle-Inclan Redondo, Y; Tsintzos, S I; Hatzopoulos, Z; Liew, T C H; Shelykh, I A; Rubo, Y G; Savvidis, P G; Baumberg, J J

2017-08-11

We demonstrate that multiply coupled spinor polariton condensates can be optically tuned through a sequence of spin-ordered phases by changing the coupling strength between nearest neighbors. For closed four-condensate chains these phases span from ferromagnetic (FM) to antiferromagnetic (AFM), separated by an unexpected crossover phase. This crossover phase is composed of alternating FM-AFM bonds. For larger eight-condensate chains, we show the critical role of spatial inhomogeneities and demonstrate a scheme to overcome them and prepare any desired spin state. Our observations thus demonstrate a fully controllable nonequilibrium spin lattice.

Single step, phase controlled, large scale synthesis of ferrimagnetic iron oxide polymorph nanoparticles by thermal plasma route and their rheological properties

NASA Astrophysics Data System (ADS)

Raut, Suyog A.; Mutadak, Pallavi R.; Kumar, Shiv; Kanhe, Nilesh S.; Huprikar, Sameer; Pol, Harshawardhan V.; Phase, Deodatta M.; Bhoraskar, Sudha V.; Mathe, Vikas L.

2018-03-01

In this paper we report single step large scale synthesis of highly crystalline iron oxide nanoparticles viz. magnetite (Fe3O4) and maghemite (γ-Fe2O3) via gas phase condensation process, where micron sized iron metal powder was used as a precursor. Selective phases of iron oxide were obtained by variation of gas flow rate of oxygen and hence partial pressure of oxygen inside the plasma reactor. Most of the particles were found to possesses average crystallite size of about 20-30 nm. The DC magnetization curves recorded indicate almost super-paramagnetic nature of the iron oxide magnetic nanoparticles. Further, iron oxide nanoparticles were analyzed using Raman spectroscopy, X-ray photoelectron spectroscopy and Mossbauer spectroscopy. In order to explore the feasibility of these nanoparticles for magnetic damper application, rheological studies have been carried out and compared with commercially available Carbonyl Iron (CI) particles. The nanoparticles obtained by thermal plasma route show improved dispersion which is useful for rheological applications.

Simulation of Deformation, Momentum and Energy Coupling Particles Deformed by Intense Shocks

NASA Astrophysics Data System (ADS)

Lieberthal, B.; Stewart, D. S.; Bdzil, J. B.; Najjar, F. M.; Balachandar, S.; Ling, Y.

2011-11-01

Modern energetic materials have embedded solids and inerts in an explosive matrix. A detonation in condensed phase materials, generates intense shocks that deform particles as the incident shock diffracts around them. The post-shock flow generates a wake behind the particle that is influenced by the shape changes of the particle. The gasdynamic flow in the explosive products and its interaction with the deformation of the particle must be treated simultaneously. Direct numerical simulations are carried out that vary the particle-to-surrounding density and impedance ratios to consider heavier and lighter particle. The vorticity deposited on the interface due to shock interaction with the particle, the resulting particle deformation and the net momentum and energy transferred to the particle, on the acoustic and longer viscous time scale are considered. The LLNL multi-physics hydrodynamic code ALE3D is used to carry out the simulations. BL, DSS and JBB supported by AFRL/RW AF FA8651-10-1-0004 & DTRA, HDTRA1-10-1-0020 Off Campus. FMN's work supported by the U.S. DOE/ LLNL, Contract DE-AC52-07NA27344. LLNL-ABS-491794.

Indoor air condensate as a novel matrix for monitoring inhalable organic contaminants.

PubMed

Roll, Isaac B; Halden, Rolf U; Pycke, Benny F G

2015-05-15

With the population of developed nations spending nearly 90% of their time indoors, indoor air quality (IAQ) is a critical indicator of human health risks from inhalation of airborne contaminants. We present a novel approach for qualitative monitoring of IAQ through the collection and analysis of indoor air condensate discharged from heat exchangers of heating, ventilation, and air conditioning (HVAC) systems. Condensate samples were collected from six suburban homes and one business in Maricopa County, Arizona, concentrated via solid-phase extraction, analyzed for 10 endocrine disrupting chemicals (EDCs) by liquid chromatography-tandem mass spectrometry (LC-MS/MS), and screened for additional organic compounds by gas chromatography-mass spectrometry (GC-MS). All 10 EDCs were detected in at least one of the sampled buildings. More than 100 additional compounds were detected by GC-MS, of which 40 were tentatively identified using spectral database searches. Twelve compounds listed as designated chemicals for biomonitoring by the California Environmental Contaminant Biomonitoring Program were detected. Microfiltration of condensate samples prior to extraction had no discernable effect on contaminant concentration, suggesting that contaminants were freely dissolved or associated with inhalable, submicron particles. This study is the first to document the utility of HVAC condensate for the qualitative assessment of indoor air for pollutants. Copyright © 2015 Elsevier B.V. All rights reserved.

Many-body Quantum Control of a Spin-1 BEC

NASA Astrophysics Data System (ADS)

Hoang, Thai; Anquez, Martin; Robbins, Bryce; Yang, Xiaoyun; Land, Benjamin; Hamley, Christopher; Chapman, Michael

2014-05-01

Spin-1 condensates provide a useful platform for investigations of atom squeezing, generation of non-Gaussian states, and dynamical control. We demonstrate dynamic control of a quantum many-body spin-1 system that is enabled by strong collisional interactions. In contrast to the usual single-particle quantum control techniques, the method demonstrated here is intrinsically many-body, exploiting the strong collisional interactions. The experiment uses a spin-1 87Rb condensate initialized in the | F = 1 , mF = 0 > polar state at a high magnetic field above the quantum phase transition, and then prepared in a coherent state using a rf rotation. The many-body control is implemented by time-varying the relative strength of the Zeeman and spin interaction energies of the condensate at multiples of the natural coherent oscillation frequency of the system. This is a parametric excitation method relying on time varying changes to the Hamiltonian. We will present our experimental results, which compare well to theory, and will discuss future directions and applications.

Marine aerosol formation from biogenic iodine emissions.

PubMed

O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

2002-06-06

The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing.

Aging induced changes on NEXAFS fingerprints in individual combustion particles

NASA Astrophysics Data System (ADS)

Zelenay, V.; Mooser, R.; Tritscher, T.; Křepelová, A.; Heringa, M. F.; Chirico, R.; Prévôt, A. S. H.; Weingartner, E.; Baltensperger, U.; Dommen, J.; Watts, B.; Raabe, J.; Huthwelker, T.; Ammann, M.

2011-11-01

Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS) and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated particles could be detected. Because such small amounts of water uptake do not lead to measurable changes in particle diameter, it may remain beyond the limits of volume growth measurements, especially for larger agglomerated particles.

Self-Assembly and Electrostriction of Arrays and Chains of Hopfion Particles in Chiral Liquid Crystals

DOE PAGES

Ackerman, P. J.; van de Lagemaat, J.; Smalyukh, I. I.

2015-01-21

Some of the most exotic condensed matter phases, such as twist grain boundary and blue phases in liquid crystals and Abrikosov phases in superconductors, contain arrays of topological defects in their ground state. Comprised of a triangular lattice of double-twist tubes of magnetization, the so-called ‘A-phase’ in chiral magnets is an example of a thermodynamically stable phase with topologically nontrivial solitonic field configurations referred to as two-dimensional skyrmions, or baby-skyrmions. Here we report that three-dimensional skyrmions in the form of double-twist tori called ‘hopfions’, or ‘torons’ when accompanied by additional self-compensating defects, self-assemble into periodic arrays and linear chains thatmore » exhibit electrostriction. In confined chiral nematic liquid crystals, this self-assembly is similar to that of liquid crystal colloids and originates from long-range elastic interactions between particle-like skyrmionic torus knots of molecular alignment field, which can be tuned from isotropic repulsive to weakly or highly anisotropic attractive by low-voltage electric fields.« less

Stimulated Desorption from Icy Aerosol Particles: A Possible Relevance To Titan's Ionospheric Conditions

NASA Astrophysics Data System (ADS)

Bordalo, Vinicius; Mejia, Christian; da Silveira, Enio F.; Seperuelo Duarte, Eduardo; Pilling, Sergio

Saturn's largest moon, Titan, has a dense atmosphere primarily composed of molecular nitro-gen (N2 , 96%) and methane (CH4 , 4%). Its atmospheric structure has been intensively studied recently due to the large amount of data obtained in situ by the Huygens probe during its de-cent to the surface on 14 January 2005. The probe could diagnose the composition of the haze particles made up organic chains containing H, C and N. Hydrocarbons and nitriles produced by photolysis of CH4 at high altitudes (˜ 2,000 km) act as embryos of aerosols of Titan as they fall to the surface. It is expected that CH4 condenses on these particles forming a layer of ice by adsorption or nucleation. Due to the high abundance of these aerosols throughout the atmo-sphere of Titan, their presence are relevant for the ionic balance of the atmosphere, especially the lower ionosphere promoted mainly by the flux of galactic cosmic rays (GCR). We have investigated the production of ions by electronic sputtering process due to the bombardment of the surfaces of aerosols by heavy ions. Time-of-flight (TOF) technique was used to obtain ion sputtering yields. An ice layer of CH4 was grown by condensation over a pre-condensed N2 ice in high vacuum chamber (1 × 10-7 mbar) at cryogenic temperature (10 K). Relative sputtering yields due to fast projectiles (252 Cf fission fragment ˜ 65 MeV) on the ice surfaces were measured. The bombardment was continued during the successive growth of both con-densed layers; the negative and positive sputtered ions were identified by TOF. Hybrid species including NH+ (17 u), HCN+ (27 u) and CN- (26 u) were formed, as well as the acetonitrile 3 ion (CH3 CN+ , 41 u). We argue that a similar process of continued ion replenishment into the gas phase by sputtering in aerosols ubiquitous in the lower ionosphere of Titan may occur and should be further investigated.

Sensitivity of Aerosol Mass and Microphysics to varying treatments of Condensational Growth of Secondary Organic Compounds in a regional model

NASA Astrophysics Data System (ADS)

Lowe, Douglas; Topping, David; McFiggans, Gordon

2017-04-01

Gas to particle partitioning of atmospheric compounds occurs through disequilibrium mass transfer rather than through instantaneous equilibrium. However, it is common to treat only the inorganic compounds as partitioning dynamically whilst organic compounds, represented by the Volatility Basis Set (VBS), are partitioned instantaneously. In this study we implement a more realistic dynamic partitioning of organic compounds in a regional framework and assess impact on aerosol mass and microphysics. It is also common to assume condensed phase water is only associated with inorganic components. We thus also assess sensitivity to assuming all organics are hygroscopic according to their prescribed molecular weight. For this study we use WRF-Chem v3.4.1, focusing on anthropogenic dominated North-Western Europe. Gas-phase chemistry is represented using CBM-Z whilst aerosol dynamics are simulated using the 8-section MOSAIC scheme, including a 9-bin VBS treatment of organic aerosol. Results indicate that predicted mass loadings can vary significantly. Without gas phase ageing of higher volatility compounds, dynamic partitioning always results in lower mass loadings downwind of emission sources. The inclusion of condensed phase water in both partitioning models increases the predicted PM mass, resulting from a larger contribution from higher volatility organics, if present. If gas phase ageing of VBS compounds is allowed to occur in a dynamic model, this can often lead to higher predicted mass loadings, contrary to expected behaviour from a simple non-reactive gas phase box model. As descriptions of aerosol phase processes improve within regional models, the baseline descriptions of partitioning should retain the ability to treat dynamic partitioning of organics compounds. Using our simulations, we discuss whether derived sensitivities to aerosol processes in existing models may be inherently biased. This work was supported by the Natural Environment Research Council within the RONOCO (NE/F004656/1) and CCN-Vol (NE/L007827/1) projects.

Sensitivity of Aerosol Mass and Microphysics to Treatments of Condensational Growth of Secondary Organic Compounds in a Regional Model

NASA Astrophysics Data System (ADS)

Topping, D. O.; Lowe, D.; McFiggans, G.; Zaveri, R. A.

2016-12-01

Gas to particle partitioning of atmospheric compounds occurs through disequilibrium mass transfer rather than through instantaneous equilibrium. However, it is common to treat only the inorganic compounds as partitioning dynamically whilst organic compounds, represented by the Volatility Basis Set (VBS), are partitioned instantaneously. In this study we implement a more realistic dynamic partitioning of organic compounds in a regional framework and assess impact on aerosol mass and microphysics. It is also common to assume condensed phase water is only associated with inorganic components. We thus also assess sensitivity to assuming all organics are hygroscopic according to their prescribed molecular weight.For this study we use WRF-Chem v3.4.1, focusing on anthropogenic dominated North-Western Europe. Gas-phase chemistry is represented using CBM-Z whilst aerosol dynamics are simulated using the 8-section MOSAIC scheme, including a 9-bin volatility basis set (VBS) treatment of organic aerosol. Results indicate that predicted mass loadings can vary significantly. Without gas phase ageing of higher volatility compounds, dynamic partitioning always results in lower mass loadings downwind of emission sources. The inclusion of condensed phase water in both partitioning models increases the predicted PM mass, resulting from a larger contribution from higher volatility organics, if present. If gas phase ageing of VBS compounds is allowed to occur in a dynamic model, this can often lead to higher predicted mass loadings, contrary to expected behaviour from a simple non-reactive gas phase box model. As descriptions of aerosol phase processes improve within regional models, the baseline descriptions of partitioning should retain the ability to treat dynamic partitioning of organic compounds. Using our simulations, we discuss whether derived sensitivities to aerosol processes in existing models may be inherently biased.This work was supported by the Nature Environment Research Council within the RONOCO (NE/F004656/1) and CCN-Vol (NE/L007827/1) projects.

Probing exoplanet clouds with optical phase curves

PubMed Central

Muñoz, Antonio García; Isaak, Kate G.

2015-01-01

Kepler-7b is to date the only exoplanet for which clouds have been inferred from the optical phase curve—from visible-wavelength whole-disk brightness measurements as a function of orbital phase. Added to this, the fact that the phase curve appears dominated by reflected starlight makes this close-in giant planet a unique study case. Here we investigate the information on coverage and optical properties of the planet clouds contained in the measured phase curve. We generate cloud maps of Kepler-7b and use a multiple-scattering approach to create synthetic phase curves, thus connecting postulated clouds with measurements. We show that optical phase curves can help constrain the composition and size of the cloud particles. Indeed, model fitting for Kepler-7b requires poorly absorbing particles that scatter with low-to-moderate anisotropic efficiency, conclusions consistent with condensates of silicates, perovskite, and silica of submicron radii. We also show that we are limited in our ability to pin down the extent and location of the clouds. These considerations are relevant to the interpretation of optical phase curves with general circulation models. Finally, we estimate that the spherical albedo of Kepler-7b over the Kepler passband is in the range 0.4–0.5. PMID:26489652

Modeling the Phase Composition of Gas Condensate in Pipelines

NASA Astrophysics Data System (ADS)

Dudin, S. M.; Zemenkov, Yu D.; Shabarov, A. B.

2016-10-01

Gas condensate fields demonstrate a number of thermodynamic characteristics to be considered when they are developed, as well as when gas condensate is transported and processed. A complicated phase behavior of the gas condensate system, as well as the dependence of the extracted raw materials on the phase state of the deposit other conditions being equal, is a key aspect. Therefore, when designing gas condensate lines the crucial task is to select the most appropriate methods of calculating thermophysical properties and phase equilibrium of the transported gas condensate. The paper describes a physical-mathematical model of a gas-liquid flow in the gas condensate line. It was developed based on balance equations of conservation of mass, impulse and energy of the transported medium within the framework of a quasi-1D approach. Constitutive relationships are given separately, and practical recommendations on how to apply the research results are provided as well.

Landau Levels of Majorana Fermions in a Spin Liquid.

PubMed

Rachel, Stephan; Fritz, Lars; Vojta, Matthias

2016-04-22

Majorana fermions, originally proposed as elementary particles acting as their own antiparticles, can be realized in condensed-matter systems as emergent quasiparticles, a situation often accompanied by topological order. Here we propose a physical system which realizes Landau levels-highly degenerate single-particle states usually resulting from an orbital magnetic field acting on charged particles-for Majorana fermions. This is achieved in a variant of a quantum spin system due to Kitaev which is distorted by triaxial strain. This strained Kitaev model displays a spin-liquid phase with charge-neutral Majorana-fermion excitations whose spectrum corresponds to that of Landau levels, here arising from a tailored pseudomagnetic field. We show that measuring the dynamic spin susceptibility reveals the Landau-level structure by a remarkable mechanism of probe-induced bound-state formation.

Development of Octyl Methoxy Cinnamates (OMC)/Silicon Dioxide (SiO₂) Nanoparticles by Sol-Gel Emulsion Method.

PubMed

Wu, Pey-Shiuan; Lee, Yi-Ching; Kuo, Yi-Ching; Lin, Chih-Chien

2017-12-07

Although octyl methoxy cinnamates (OMC) is the most used Ultraviolet B (UVB) filter in sunscreen, it has poor light stability in emulsion system. In this study, OMC/SiO₂ nanoparticles were prepared via sol-gel emulsion method. Tetraethoxy silane (TEOS) was used as the silica source to encapsulate OMC. Modification of experimental parameters such as stirring speed of condensation reaction and emulsion condition, pH value of acid-catalyzed, surfactant and different percentage of TEOS and OMC, adding of OMC and surfactant to different phase may affect the particle size, and yield and entrapment efficiency in preparation process of OMC/SiO₂ nanoparticles. Concluding all the parameter, we found that when condensation reaction and emulsion conditions are at 1000 rpm, pH 1.5, Span 80/Tween 20, TEOS/OMC ratios 1:1, OMC and surfactants added in oil phase, resulting in smaller particle sizes 476.5 nm, higher yield 95.8%, and higher entrapment efficiency 61.09%. Fourier transform infrared (FTIR) analysis demonstrated that OMC/SiO₂ nanoparticles were successfully prepared. In vitro release profile supposed that OMC/SiO₂ nanoparticles can delay OMC releasing and had 60.83% decreasing of cumulative amount. Therefore, the OMC/SiO₂ nanoparticles have the potential to develop as new sunscreen materials in the use for cosmetics field in the future.

STORMVEX. Ice Nuclei and Cloud Condensation Nuclei Characterization Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cziczo, D.

2016-03-01

The relationship between aerosol particles and the formation of clouds is among the most uncertain aspects in our current understanding of climate change. Warm clouds have been the most extensively studied, in large part because they are normally close to the Earth’s surface and only contain large concentrations of liquid droplets. Ice and mixed-phase clouds have been less studied even though they have extensive global coverage and dominate precipitation formation. Because they require low temperatures to form, both cloud types are infrequently found at ground level, resulting in more difficult field studies. Complex mixtures of liquid and ice elements, normallymore » at much lower concentrations than found in warm clouds, require precise separation techniques and accurate identification of phase. Because they have proved so difficult to study, the climatic impact of ice-containing clouds remains unresolved. In this study, cloud condensation nuclei (CCN) concentrations and associated single particles’ composition and size were measured at a high-elevation research site—Storm Peak Lab, east of Steamboat Springs, Colorado, operated by the Desert Research Institute. Detailed composition analyses were presented to compare CCN activation with single-particle composition. In collaboration with the scientists of the Storm Peak Lab Cloud Property Validation Experiment (STORMVEX), our goal was to relate these findings to the cloud characteristics and the effect of anthropogenic activities.« less

Autoxidation as a source of gas-phase highly-oxidized multifunctional compounds (HOM) - measured by chemical ionization spectrometry (CIMS) utilizing various reagent ion chemistries

NASA Astrophysics Data System (ADS)

Rissanen, M.; Kurten, T.; Mauldin, L.; Ehn, M.

2017-12-01

Secondary organic aerosol (SOA) constitutes the largest fraction of atmospheric submicron particulate matter. Despite its importance to the Earth's radiative balance, mainly by acting as a source of cloud condensation nuclei (CCN), the molecular details of the first-steps of atmospheric new particle formation keep eluding researchers. Recently a gas-phase autocatalytic oxidation mechanism (=autoxidation) was invoked to explain the very fast formation of highly-oxidized multifunctional organic compounds (HOMs), and it was shown to provide the needed prompt condensable matter that forms the smallest of the atmospheric particles. Of detailed autoxidation progressions, only cyclohexene ozonolysis initiated oxidation has been described by quantum chemical computations, and it was quickly recognized that further reaction steps are needed (such as endoperoxidation) to explain the formation of the observed HOM products from biogenic terpenes. Also it was realized that the simplest group additivity principles commonly applied to derive saturation vapor pressures do not suffice to determine the vapor pressures of multiple hydroperoxide and other oxidized functionalities containing HOM products. Thereby the fraction of the lowest volatility products is less than previously assumed, which could indicate reactive uptake of HOM products. In the AGU fall meeting I will present our most recent findings on resolving the (i) detailed molecular mechanisms generating HOMs, (ii) their actual vapor pressures, and (iii) their interaction with the environment.

String Theory Methods for Condensed Matter Physics

NASA Astrophysics Data System (ADS)

Nastase, Horatiu

2017-09-01

Preface; Acknowledgments; Introduction; Part I. Condensed Matter Models and Problems: 1. Lightning review of statistical mechanics, thermodynamics, phases and phase transitions; 2. Magnetism in solids; 3. Electrons in solids: Fermi gas vs. Fermi liquid; 4. Bosonic quasi-particles: phonons and plasmons; 5. Spin-charge separation in 1+1 dimensional solids: spinons and holons; 6. The Ising model and the Heisenberg spin chain; 7. Spin chains and integrable systems; 8. The thermodynamic Bethe ansatz; 9. Conformal field theories and quantum phase transitions; 10. Classical vs. quantum Hall effect; 11. Superconductivity: Landau-Ginzburg, London and BCS; 12. Topology and statistics: Berry and Chern-Simons, anyons and nonabelions; 13. Insulators; 14. The Kondo effect and the Kondo problem; 15. Hydrodynamics and transport properties: from Boltzmann to Navier-Stokes; Part II. Elements of General Relativity and String Theory: 16. The Einstein equation and the Schwarzschild solution; 17. The Reissner-Nordstrom and Kerr-Newman solutions and thermodynamic properties of black holes; 18. Extra dimensions and Kaluza-Klein; 19. Electromagnetism and gravity in various dimensions. Consistent truncations; 20. Gravity plus matter: black holes and p-branes in various dimensions; 21. Weak/strong coupling dualities in 1+1, 2+1, 3+1 and d+1 dimensions; 22. The relativistic point particle and the relativistic string; 23. Lightcone strings and quantization; 24. D-branes and gauge fields; 25. Electromagnetic fields on D-branes. Supersymmetry and N = 4 SYM. T-duality of closed strings; 26. Dualities and M theory; 27. The AdS/CFT correspondence: definition and motivation; Part III. Applying String Theory to Condensed Matter Problems: 28. The pp wave correspondence: string Hamiltonian from N = 4 SYM; 29. Spin chains from N = 4 SYM; 30. The Bethe ansatz: Bethe strings from classical strings in AdS; 31. Integrability and AdS/CFT; 32. AdS/CFT phenomenology: Lifshitz, Galilean and Schrodinger symmetries and their gravity duals; 33. Finite temperature and black holes; 34. Hot plasma equilibrium thermodynamics: entropy, charge density and chemical potential of strongly coupled theories; 35. Spectral functions and transport properties; 36. Dynamic and nonequilibrium properties of plasmas: electric transport, Langevin diffusion and thermalization via black hole quasi-normal modes; 37. The holographic superconductor; 38. The fluid-gravity correspondence: conformal relativistic fluids from black hole horizons; 39. Nonrelativistic fluids: from Einstein to Navier-Stokes and back; Part IV. Advanced Applications: 40. Fermi gas and liquid in AdS/CFT; 41. Quantum Hall effect from string theory; 42. Quantum critical systems and AdS/CFT; 43. Particle-vortex duality and ABJM vs. AdS4 X CP3 duality; 44. Topology and non-standard statistics from AdS/CFT; 45. DBI scalar model for QGP/black hole hydro- and thermo-dynamics; 46. Holographic entanglement entropy in condensed matter; 47. Holographic insulators; 48. Holographic strange metals and the Kondo problem; References; Index.

Organic Condensation and Particle Growth to CCN Sizes in the Summertime Marine Arctic Is Driven by Materials More Semivolatile Than at Continental Sites

NASA Astrophysics Data System (ADS)

Burkart, Julia; Hodshire, Anna L.; Mungall, Emma L.; Pierce, Jeffrey R.; Collins, Douglas B.; Ladino, Luis A.; Lee, Alex K. Y.; Irish, Victoria; Wentzell, Jeremy J. B.; Liggio, John; Papakyriakou, Tim; Murphy, Jennifer; Abbatt, Jonathan

2017-10-01

Ship-based aerosol measurements in the summertime Arctic indicate elevated concentrations of ultrafine particles with occasional growth to cloud condensation nuclei (CCN) sizes. Focusing on one episode with two continuously growing modes, growth occurs faster for a large, preexisting mode (dp ≈ 90 nm) than for a smaller nucleation mode (dp ≈ 20 nm). We use microphysical modeling to show that growth is largely via organic condensation. Unlike results for midlatitude forested regions, most of these condensing species behave as semivolatile organics, as lower volatility organics would lead to faster growth of the smaller mode. The magnitude of the CCN hygroscopicity parameter for the growing particles, 0.1, is also consistent with organic species constituting a large fraction of the particle composition. Mixing ratios of common aerosol growth precursors, such as isoprene and sulfur dioxide, are not elevated during the episode, indicating that an unidentified aerosol growth precursor is present in this high-latitude marine environment.

Characterization of pure Ni ultrafine/nanoparticles synthesized by electromagnetic levitational gas condensation method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Khodaei, Azin, E-mail: Azin.Khodaei@gmail.com; Hasannasab, Malihe; Amousoltani, Narges

2016-02-15

Highlights: • Ni ultrafine/nanoparticles were produced using the single-step ELGC method. • Ar and He–20%Ar gas mixtures were used as the condensing gas under 1 atm. • Effects of gas type and flow rate on particle size distribution were investigated. • The nanoparticles showed both high saturation magnetization and low coercivity. - Abstract: In this work, Ni ultrafine/nanoparticles were directly produced using the one-step, relatively large-scale electromagnetic levitational gas condensation method. In this process, Ni vapors ascending from the levitated droplet were condensed by Ar and He–20%Ar gas mixtures under atmospheric pressure. Effects of type and flow rate of themore » condensing gas on the size, size distribution and crystallinity of Ni particles were investigated. The particles were characterized by scanning electron microscopy, X-ray diffraction and vibrating sample magnetometer (VSM). The process parameters for the synthesis of the crystalline Ni ultrafine/nanoparticles were determined.« less

Self-consistent phonon theory of the crystallization and elasticity of attractive hard spheres.

PubMed

Shin, Homin; Schweizer, Kenneth S

2013-02-28

We propose an Einstein-solid, self-consistent phonon theory for the crystal phase of hard spheres that interact via short-range attractions. The approach is first tested against the known behavior of hard spheres, and then applied to homogeneous particles that interact via short-range square well attractions and the Baxter adhesive hard sphere model. Given the crystal symmetry, packing fraction, and strength and range of attractive interactions, an effective harmonic potential experienced by a particle confined to its Wigner-Seitz cell and corresponding mean square vibrational amplitude are self-consistently calculated. The crystal free energy is then computed and, using separate information about the fluid phase free energy, phase diagrams constructed, including a first-order solid-solid phase transition and its associated critical point. The simple theory qualitatively captures all the many distinctive features of the phase diagram (critical and triple point, crystal-fluid re-entrancy, low-density coexistence curve) as a function of attraction range, and overall is in good semi-quantitative agreement with simulation. Knowledge of the particle localization length allows the crystal shear modulus to be estimated based on elementary ideas. Excellent predictions are obtained for the hard sphere crystal. Expanded and condensed face-centered cubic crystals are found to have qualitatively different elastic responses to varying attraction strength or temperature. As temperature increases, the expanded entropic solid stiffens, while the energy-controlled, fully-bonded dense solid softens.

State sum constructions of spin-TFTs and string net constructions of fermionic phases of matter

DOE PAGES

Bhardwaj, Lakshya; Gaiotto, Davide; Kapustin, Anton

2017-04-18

It is possible to describe fermionic phases of matter and spin-topological field theories in 2+1d in terms of bosonic “shadow” theories, which are obtained from the original theory by “gauging fermionic parity”. Furthemore, the fermionic/spin theories are recovered from their shadow by a process of fermionic anyon condensation: gauging a one-form symmetry generated by quasi-particles with fermionic statistics. We apply the formalism to theories which admit gapped boundary conditions. We obtain Turaev-Viro-like and Levin-Wen-like constructions of fermionic phases of matter. Here, we describe the group structure of fermionic SPT phases protected by Z 2f × G. The quaternion group makesmore » a surprise appearance.« less

The rate of equilibration of viscous aerosol particles

NASA Astrophysics Data System (ADS)

O'Meara, Simon; Topping, David O.; McFiggans, Gordon

2016-04-01

The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1-90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1 × 10-25 m2 s-1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

Surfactants from the gas phase may promote cloud droplet formation.

PubMed

Sareen, Neha; Schwier, Allison N; Lathem, Terry L; Nenes, Athanasios; McNeill, V Faye

2013-02-19

Clouds, a key component of the climate system, form when water vapor condenses upon atmospheric particulates termed cloud condensation nuclei (CCN). Variations in CCN concentrations can profoundly impact cloud properties, with important effects on local and global climate. Organic matter constitutes a significant fraction of tropospheric aerosol mass, and can influence CCN activity by depressing surface tension, contributing solute, and influencing droplet activation kinetics by forming a barrier to water uptake. We present direct evidence that two ubiquitous atmospheric trace gases, methylglyoxal (MG) and acetaldehyde, known to be surface-active, can enhance aerosol CCN activity upon uptake. This effect is demonstrated by exposing acidified ammonium sulfate particles to 250 parts per billion (ppb) or 8 ppb gas-phase MG and/or acetaldehyde in an aerosol reaction chamber for up to 5 h. For the more atmospherically relevant experiments, i.e., the 8-ppb organic precursor concentrations, significant enhancements in CCN activity, up to 7.5% reduction in critical dry diameter for activation, are observed over a timescale of hours, without any detectable limitation in activation kinetics. This reduction in critical diameter enhances the apparent particle hygroscopicity up to 26%, which for ambient aerosol would lead to cloud droplet number concentration increases of 8-10% on average. The observed enhancements exceed what would be expected based on Köhler theory and bulk properties. Therefore, the effect may be attributed to the adsorption of MG and acetaldehyde to the gas-aerosol interface, leading to surface tension depression of the aerosol. We conclude that gas-phase surfactants may enhance CCN activity in the atmosphere.

Photochemistry of Glyoxal in Wet Aerosols: Smog Chamber Study

NASA Astrophysics Data System (ADS)

Lim, Y. B.; Kim, H.; Turpin, B. J.

2015-12-01

Aqueous chemistry is an important pathway for the formation of secondary organic aerosol (SOA). Reaction vessel studies provide evidence that in the aqueous phase photooxidation of water soluble organic compounds (e.g., glyoxal, methylglyoxal) form multifunctional organic products and oligomers. In this work, we extend this bulk-phase chemistry to the condensed-phase chemistry that occurs in/on aerosols by conducting smog chamber experiments — photooxidation of ammonium sulfate and sulfuric acid aerosols containing glyoxal and hydrogen peroxide in the presence of NOx under dry/humid conditions. Particles were analyzed using ultra performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). In the irradiated chamber, photooxidation products of glyoxal as seen in reaction vessel experiments (e.g., oxalic acids and tartaric acids) were also formed in both ammonium sulfate aerosols and sulfuric acid aerosols at humid and even dry conditions. However, the major products were organosulfurs (CHOS), organonitrogens (CHON), and nitrooxy-organosulfates (CHONS), which were also dominantly formed in the dark chamber. These products were formed via non-radical reactions, which depend on acidity and humidity. However, the real-time profiles in the dark chamber and the irradiated chamber were very different, suggesting photochemistry substantially affects non-radical formation in the condensed phase.

Goldstone mode and pair-breaking excitations in atomic Fermi superfluids

NASA Astrophysics Data System (ADS)

Hoinka, Sascha; Dyke, Paul; Lingham, Marcus G.; Kinnunen, Jami J.; Bruun, Georg M.; Vale, Chris J.

2017-10-01

Spontaneous symmetry breaking is a central paradigm of elementary particle physics, magnetism, superfluidity and superconductivity. According to Goldstone's theorem, phase transitions that break continuous symmetries lead to the existence of gapless excitations in the long-wavelength limit. These Goldstone modes can become the dominant low-energy excitation, showing that symmetry breaking has a profound impact on the physical properties of matter. Here, we present a comprehensive study of the elementary excitations in a homogeneous strongly interacting Fermi gas through the crossover from a Bardeen-Cooper-Schrieffer (BCS) superfluid to a Bose-Einstein condensate (BEC) of molecules using two-photon Bragg spectroscopy. The spectra exhibit a discrete Goldstone mode, associated with the broken-symmetry superfluid phase, as well as pair-breaking single-particle excitations. Our techniques yield a direct determination of the superfluid pairing gap and speed of sound in close agreement with strong-coupling theories.

PT -symmetric gain and loss in a rotating Bose-Einstein condensate

NASA Astrophysics Data System (ADS)

Haag, Daniel; Dast, Dennis; Cartarius, Holger; Wunner, Günter

2018-03-01

PT -symmetric quantum mechanics allows finding stationary states in mean-field systems with balanced gain and loss of particles. In this work we apply this method to rotating Bose-Einstein condensates with contact interaction which are known to support ground states with vortices. Due to the particle exchange with the environment transport phenomena through ultracold gases with vortices can be studied. We find that even strongly interacting rotating systems support stable PT -symmetric ground states, sustaining a current parallel and perpendicular to the vortex cores. The vortices move through the nonuniform particle density and leave or enter the condensate through its borders creating the required net current.

The global impact of mineral dust on cloud droplet number concentration

NASA Astrophysics Data System (ADS)

Karydis, V.; Tsimpidi, A.; Bacer, S.; Pozzer, A.; Nenes, A.; Lelieveld, J.

2016-12-01

This study assesses the importance of mineral dust for cloud droplet formation by taking into account i) the adsorption of water on the surface of insoluble dust particles, ii) the coating of soluble material on the surface of mineral particles which augments their cloud condensation nuclei activity, and iii) the effect of dust on the inorganic aerosol concentrations through thermodynamic interactions with mineral cations. Simulations are carried out with the EMAC chemistry climate model that calculates the global atmospheric aerosol composition using the ISORROPIA-II thermodynamic equilibrium model and considers the gas phase interactions with K+-Ca2+-Mg2+-NH4+-Na+-SO42-NO3-Cl-H2O particle components. Emissions of the inert mineral dust and the reactive dust aerosol components are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide (Karydis et al., 2016). We have implemented the "unified dust activation parameterization" (Kumar et al., 2011; Karydis et al., 2011) to calculate the droplet number concentration by taking into account the inherent hydrophilicity from adsorption and the acquired hygroscopicity from soluble salts by dust particles. Our simulations suggest that mineral dust significantly increases the cloud droplet number concentration (CDNC) over the main deserts and the adjacent oceans. However, over polluted areas the CDNC decreases significantly in the presence of dust. Furthermore, we investigate the role of adsorption activation of insoluble aerosols and the mineral dust thermodynamic interactions with inorganic anions on the cloud droplet formation. The CDNC sensitivity to the emission load, chemical composition, and inherent hydrophilicity of mineral dust is also tested. ReferencesKarydis, et al. (2011). "On the effect of dust particles on global cloud condensation nuclei and cloud droplet number." J. Geophys. Res. Atmos. 116. Karydis, et al. (2016). "Effects of mineral dust on global atmospheric nitrate concentrations." Atmos. Chem. Phys. 16(3): 1491-1509. Kumar, et al. (2011). "Measurements of cloud condensation nuclei activity and droplet activation kinetics of wet processed regional dust samples and minerals." Atmos. Chem. Phys. Discuss. 11(4): 12561-12605.

Condensation-nuclei (Aitken Particle) measurement system used in NASA global atmospheric sampling program

NASA Technical Reports Server (NTRS)

Nyland, T. W.

1979-01-01

The condensation-nuclei (Aitken particle) measuring system used in the NASA Global Atmospheric Sampling Program is described. Included in the paper is a description of the condensation-nuclei monitor sensor, the pressurization system, and the Pollack-counter calibration system used to support the CN measurement. The monitor has a measurement range to 1000 CN/cm cubed and a noise level equivalent to 5 CN/cm cubed at flight altitudes between 6 and 13 km.

Organic condensation: A vital link connecting aerosol formation to climate forcing (Invited)

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petdjd, T. T.; Slowik, J. G.; Chang, R. Y.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M. T.

2010-12-01

Aerosol-cloud interactions represent the largest uncertainty in calculations of Earth’s radiative forcing. Number concentrations of atmospheric aerosol particles are in the core of this uncertainty, as they govern the numbers of cloud condensation nuclei (CCN) and influence the albedo and lifetime of clouds. Aerosols also impair air quality through their adverse effects on atmospheric visibility and human health. The ultrafine fraction (<100 nm) of atmospheric aerosol particles often dominates the total aerosol numbers, and nucleation of atmospheric vapours is one of the most important sources of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size, and consequently their climatic importance remains to be quantified (see Fig. 1). We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapours is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations; we propose a new modelling approach that is consistent with the measurements. Finally, we demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapours and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models. Figure 1. Organic emissions and the dynamic processes governing the climatic importance of ultrafine aerosol. Condensable vapours are produced upon oxidation of volatile organic compounds (VOCs) and can 1) nucleate to form new small particles; 2) grow freshly formed particles to larger sizes and increase their probability to serve as CCN; 3) condense on the background aerosol (> 100 nm) and enhance the loss of ultrafine particles. Primary organic aerosol (POA) contributes to the large end of the aerosol size distribution, enhancing the scavenging of the ultrafine particles.

Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

NASA Astrophysics Data System (ADS)

Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

2011-07-01

Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

Molecular Modeling of Three Phase Contact for Static and Dynamic Contact Angle Phenomena

NASA Astrophysics Data System (ADS)

Malani, Ateeque; Amat, Miguel; Raghavanpillai, Anilkumar; Wysong, Ernest; Rutledge, Gregory

2012-02-01

Interfacial phenomena arise in a number of industrially important situations, such as repellency of liquids on surfaces, condensation, etc. In designing materials for such applications, the key component is their wetting behavior, which is characterized by three-phase static and dynamic contact angle phenomena. Molecular modeling has the potential to provide basic insight into the detailed picture of the three-phase contact line resolved on the sub-nanometer scale which is essential for the success of these materials. We have proposed a computational strategy to study three-phase contact phenomena, where buoyancy of a solid rod or particle is studied in a planar liquid film. The contact angle is readily evaluated by measuring the position of solid and liquid interfaces. As proof of concept, the methodology has been validated extensively using a simple Lennard-Jones (LJ) fluid in contact with an LJ surface. In the dynamic contact angle analysis, the evolution of contact angle as a function of force applied to the rod or particle is characterized by the pinning and slipping of the three phase contact line. Ultimately, complete wetting or de-wetting is observed, allowing molecular level characterization of the contact angle hysteresis.

Organic Aerosol Formation Photoenhanced by the Formation of Secondary Photo-sensitizers in ageing Aerosols

NASA Astrophysics Data System (ADS)

Aregahegn, Kifle; Nozière, Barbara; George, Christian

2013-04-01

Humankind is facing a changing environment possibly due to anthropogenic stress on the atmosphere. In this context, aerosols play a key role by affecting the radiative climate forcing, hydrological cycle, and by their adverse effect on health. The role of organic compounds in these processes is however still poorly understood because of their massive chemical complexity and numerous transformations. This is particularly true for Secondary Organic Aerosol (SOA), which are produced in the atmosphere by organic gases. Traditionally, the driving forces for SOA growth is believed to be the partitioning onto aerosol seeds of condensable gases, either emitted primarily or resulting from the gas phase oxidation of organic gases. However, even the most up-to-date models based on such mechanisms can not account for the SOA mass observed in the atmosphere, suggesting the existence of other, yet unknown formation processes. The present study shows experimental evidence that particulate phase chemistry produces photo-sensitizers that lead to photo-induced formation and growth of secondary organic aerosol in the near UV and the presence of volatile organic compounds (VOC) such as terpenes. By means of an aerosol flow tube reactor equipped with Scanning Mobility Particle Sizer (SMPS) having Kr-85 source aerosol neutralizer, Differential Mobility Analyser (DMA) and Condensation Particle Sizer (CPC), we identified that traces of the aerosol phase product of glyoxal chemistry as is explained in Gallway et al., and Yu et al., namely imidazole-2-carboxaldehyde (IC) is a strong photo-sensitizer when irradiated by near-UV in the presence of volatile organic compounds such as terpenes. Furthermore, the influence of pH, type and concentration of VOCs, composition of seed particles, relative humidity and irradiation intensity on particle growth were studied. This novel photo-sensitizer contributed to more than 30% of SOA growth in 19min irradiation time in the presence of terpenes in the system and has linear relationship with the irradiation intensity. These results demonstrate that, upon ageing, organic aerosols can produce photo-sensitizers which auto-photo-catalyses their SOA growth.

Single-Particle Properties of a Strongly Interacting Bose-Fermi Mixture Above the BEC Phase Transition Temperature

NASA Astrophysics Data System (ADS)

Kharga, D.; Inotani, D.; Hanai, R.; Ohashi, Y.

2017-06-01

We theoretically investigate the normal state properties of a Bose-Fermi mixture with a strong attractive interaction between Fermi and Bose atoms. We extend the ordinary T-matrix approximation (TMA) with respect to Bose-Fermi pairing fluctuations, to include the Hugenholtz-Pines' relation for all Bose Green's functions appearing in TMA self-energy diagrams. This extension is shown to be essentially important to correctly describe the physical properties of the Bose-Fermi mixture, especially near the Bose-Einstein condensation instability. Using this improved TMA, we clarify how the formation of composite fermions affects Bose and Fermi single-particle excitation spectra, over the entire interaction strength.

Maxwell's Demon at work: Two types of Bose condensate fluctuations in power-law traps.

PubMed

Grossmann, S; Holthaus, M

1997-11-10

After discussing the idea underlying the Maxwell's Demon ensemble, we employ this ensemble for calculating fluctuations of ideal Bose gas condensates in traps with power-law single-particle energy spectra. Two essentially different cases have to be distinguished. If the heat capacity is continuous at the condensation point, the fluctuations of the number of condensate particles vanish linearly with temperature, independent of the trap characteristics. In this case, microcanonical and canonical fluctuations are practically indistinguishable. If the heat capacity is discontinuous, the fluctuations vanish algebraically with temperature, with an exponent determined by the trap, and the micro-canonical fluctuations are lower than their canonical counterparts.

Evaluation of a coupled dispersion and aerosol process model against measurements near a major road

NASA Astrophysics Data System (ADS)

Pohjola, M. A.; Pirjola, L.; Karppinen, A.; Härkönen, J.; Ketzel, M.; Kukkonen, J.

2007-02-01

A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17-20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm-10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3-50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible at this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm-3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the concentration of condensable organic vapour of 109-1010 molecules cm-3 resulted in particle sizes that were closest to the measured values.

Observations of condensation nuclei in the 1987 airborne Antarctic ozone experiment

NASA Technical Reports Server (NTRS)

Wilson, J. C.; Smith, S. D.; Ferry, G. V.; Loewenstein, M.

1988-01-01

The condensation nucleus counter (CNC) flown of the NASA ER-2 in the Airborne Antarctic Ozone Experiment provides a measurement of the number mixing ratio of particles which can be grown by exposure to supersaturated n-butyl alcohol vapor to diameters of a few microns. Such particles are referred to as condensation nuclei (CN). The ER-2 CNC was calibrated with aerosols of known size and concentration and was found to provide an accurate measure of the number concentration of particles larger than about 0.02 micron. Since the number distribution of stratospheric aerosols is usually dominated by particles less than a few tenths of micron in diameter, the upper cutoff of the ER-2 CNC has not been determined experimentally. However, theory suggests that the sampling and counting efficiency should remain near one for particles as large as 1 micron in diameter. Thus, the CN mixing ratio is usually a good measure of the mixing ratio of submicron particles.

Fluctuations in non-ideal pion gas with dynamically fixed particle number

NASA Astrophysics Data System (ADS)

Kolomeitsev, E. E.; Voskresensky, D. N.

2018-05-01

We consider a non-ideal hot pion gas with the dynamically fixed number of particles in the model with the λϕ4 interaction. The effective Lagrangian for the description of such a system is obtained after dropping the terms responsible for the change of the total particle number. Reactions π+π- ↔π0π0, which determine the isospin balance of the medium, are permitted. Within the self-consistent Hartree approximation we compute the effective pion mass, thermodynamic characteristics of the system and the variance of the particle number at temperatures above the critical point of the induced Bose-Einstein condensation when the pion chemical potential reaches the value of the effective pion mass. We analyze conditions for the condensate formation in the process of thermalization of an initially non-equilibrium pion gas. The normalized variance of the particle number increases with a temperature decrease but remains finite in the critical point of the Bose-Einstein condensation. This is due to the non-perturbative account of the interaction and is in contrast to the ideal-gas case. In the kinetic regime of the condensate formation the variance is shown to stay finite also.

Decay of ultralight axion condensates

DOE PAGES

Eby, Joshua; Ma, Michael; Suranyi, Peter; ...

2018-01-15

Axion particles can form macroscopic condensates, whose size can be galactic in scale for models with very small axion massesmore » $$m\\sim10^{-22}$$ eV, and which are sometimes referred to under the name of Fuzzy Dark Matter. Many analyses of these condensates are done in the non-interacting limit, due to the weakness of the self-interaction coupling of axions. We investigate here how certain results change upon inclusion of these interactions, finding a decreased maximum mass and a modified mass-radius relationship. Further, these condensates are, in general, unstable to decay through number-changing interactions. We analyze the stability of galaxy-sized condensates of axion-like particles, and sketch the parameter space of stable configurations as a function of a binding energy parameter. As a result, we find a strong lower bound on the size of Fuzzy Dark Matter condensates which are stable to decay, with lifetimes longer than the age of the universe.« less

Decay of ultralight axion condensates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eby, Joshua; Ma, Michael; Suranyi, Peter

Axion particles can form macroscopic condensates, whose size can be galactic in scale for models with very small axion massesmore » $$m\\sim10^{-22}$$ eV, and which are sometimes referred to under the name of Fuzzy Dark Matter. Many analyses of these condensates are done in the non-interacting limit, due to the weakness of the self-interaction coupling of axions. We investigate here how certain results change upon inclusion of these interactions, finding a decreased maximum mass and a modified mass-radius relationship. Further, these condensates are, in general, unstable to decay through number-changing interactions. We analyze the stability of galaxy-sized condensates of axion-like particles, and sketch the parameter space of stable configurations as a function of a binding energy parameter. As a result, we find a strong lower bound on the size of Fuzzy Dark Matter condensates which are stable to decay, with lifetimes longer than the age of the universe.« less

Matter wave coupling of spatially separated and unequally pumped polariton condensates

NASA Astrophysics Data System (ADS)

Kalinin, Kirill P.; Lagoudakis, Pavlos G.; Berloff, Natalia G.

2018-03-01

Spatial quantum coherence between two separated driven-dissipative polariton condensates created nonresonantly and with a different occupation is studied. We identify the regions where the condensates remain coherent with the phase difference continuously changing with the pumping imbalance and the regions where each condensate acquires its own chemical potential with phase differences exhibiting time-dependent oscillations. We show that in the mutual coherence limit the coupling consists of two competing contributions: a symmetric Heisenberg exchange and the Dzyloshinskii-Moriya asymmetric interactions that enable a continuous tuning of the phase relation across the dyad and derive analytic expressions for these types of interactions. The introduction of nonequal pumping increases the complexity of the type of problems that can be solved by polariton condensates arranged in a graph configuration. If equally pumped polaritons condensates arrange their phases to solve the constrained quadratic minimisation problem with a real symmetric matrix, the nonequally pumped condensates solve that problem for a general Hermitian matrix.

Magnetic Majorana Fermions

NASA Astrophysics Data System (ADS)

Moessner, Roderich

Condensed matter systems provide emergent mini-universes in which quasiparticles may exist which do not correspond to any experimentally detected elementary particle. Topological quantum materials have been particularly productive in this regard, with the present search focussing on Majorana fermions, known theoretically already for decades. Here, we discuss manifestations of magnetic Majorana fermions in the Kitaev model. We place particular emphasis on their fate when perturbations, such as Heisenberg terms, are added to the ideal model system, and address experimental signatures of their vestiges in phases adjacent to the spin liquid.

New applications of the renormalization group method in physics: a brief introduction.

PubMed

Meurice, Y; Perry, R; Tsai, S-W

2011-07-13

The renormalization group (RG) method developed by Ken Wilson more than four decades ago has revolutionized the way we think about problems involving a broad range of energy scales such as phase transitions, turbulence, continuum limits and bifurcations in dynamical systems. The Theme Issue provides articles reviewing recent progress made using the RG method in atomic, condensed matter, nuclear and particle physics. In the following, we introduce these articles in a way that emphasizes common themes and the universal aspects of the method.

Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch

NASA Astrophysics Data System (ADS)

Cozic, J.; Verheggen, B.; Mertes, S.; Connolly, P.; Bower, K.; Petzold, A.; Baltensperger, U.; Weingartner, E.

2006-11-01

The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (drops and ice particles) as well as interstitial aerosol particles; an interstitial inlet which collected only interstitial (unactivated) aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the cloud phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~10% in mixed-phase clouds with IMF>0.2. This is explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.

Condenser-free contrast methods for transmitted-light microscopy

PubMed Central

WEBB, K F

2015-01-01

Phase contrast microscopy allows the study of highly transparent yet detail-rich specimens by producing intensity contrast from phase objects within the sample. Presented here is a generalized phase contrast illumination schema in which condenser optics are entirely abrogated, yielding a condenser-free yet highly effective method of obtaining phase contrast in transmitted-light microscopy. A ring of light emitting diodes (LEDs) is positioned within the light-path such that observation of the objective back focal plane places the illuminating ring in appropriate conjunction with the phase ring. It is demonstrated that true Zernike phase contrast is obtained, whose geometry can be flexibly manipulated to provide an arbitrary working distance between illuminator and sample. Condenser-free phase contrast is demonstrated across a range of magnifications (4–100×), numerical apertures (0.13–1.65NA) and conventional phase positions. Also demonstrated is condenser-free darkfield microscopy as well as combinatorial contrast including Rheinberg illumination and simultaneous, colour-contrasted, brightfield, darkfield and Zernike phase contrast. By providing enhanced and arbitrary working space above the preparation, a range of concurrent imaging and electrophysiological techniques will be technically facilitated. Condenser-free phase contrast is demonstrated in conjunction with scanning ion conductance microscopy (SICM), using a notched ring to admit the scanned probe. The compact, versatile LED illumination schema will further lend itself to novel next-generation transmitted-light microscopy designs. The condenser-free illumination method, using rings of independent or radially-scanned emitters, may be exploited in future in other electromagnetic wavebands, including X-rays or the infrared. PMID:25226859

Two Impurities in a Bose-Einstein Condensate: From Yukawa to Efimov Attracted Polarons

NASA Astrophysics Data System (ADS)

Naidon, Pascal

2018-04-01

The well-known Yukawa and Efimov potentials are two different mediated interaction potentials. The first one arises in quantum field theory from the exchange of virtual particles. The second one is mediated by a real particle resonantly interacting with two other particles. This Letter shows how two impurities immersed in a Bose-Einstein condensate can exhibit both phenomena. For a weak attraction with the condensate, the two impurities form two polarons that interact through a weak Yukawa attraction mediated by virtual excitations. For a resonant attraction with the condensate, the exchanged excitation becomes a real boson and the mediated interaction changes to a strong Efimov attraction that can bind the two polarons. The resulting bipolarons turn into in-medium Efimov trimers made of the two impurities and one boson. Evidence of this physics could be seen in ultracold mixtures of atoms.

Thermal Oxidation of a Carbon Condensate Formed in High-Frequency Carbon and Carbon-Nickel Plasma Flow

NASA Astrophysics Data System (ADS)

Churilov, G. N.; Nikolaev, N. S.; Cherepakhin, A. V.; Dudnik, A. I.; Tomashevich, E. V.; Trenikhin, M. V.; Bulina, N. G.

2018-02-01

We have reported on the comparative characteristics of thermal oxidation of a carbon condensate prepared by high-frequency arc evaporation of graphite rods and a rod with a hollow center filled with nickel powder. In the latter case, along with different forms of nanodisperse carbon, nickel particles with nickel core-carbon shell structures are formed. It has been found that the processes of the thermal oxidation of carbon condensates with and without nickel differ significantly. Nickel particles with the carbon shell exhibit catalytic properties with respect to the oxidation of nanosized carbon structures. A noticeable difference between the temperatures of the end of the oxidation process for various carbon nanoparticles and nickel particles with the carbon shell has been established. The study is aimed at investigations of the effect of nickel nanoparticles on the dynamics of carbon condensate oxidation upon heating in the argon-oxygen flow.

Novel insight on photochemistry at interfaces: potential impact on Seconday Aerosol Formation?

NASA Astrophysics Data System (ADS)

Rossignol, S.; George, C.; Aregahegn, K.

2014-12-01

Traditionally, the driving forces for SOA growth is believed to be the partitioning onto aerosol seeds of condensable gases, either emitted primarily or resulting from the gas phase oxidation of organic gases. However, even the most up-to-date models based on such mechanisms cannot account for the SOA mass observed in the atmosphere, suggesting the existence of other, yet unknown formation processes. The present study shows experimental evidence that particulate phase chemistry produces photo-sensitizers that lead to photo-induced formation and growth of secondary organic aerosol in the near UV and the presence of volatile organic compounds (VOC) such as terpenes. By means of an aerosol flow tube reactor equipped with Scanning Mobility Particle Sizer (SMPS), Differential Mobility Analyzer (DMA) and Condensation Particle Sizer (CPC), we identified that traces in the aerosol phase of glyoxal chemistry products, namely imidazole-2-carboxaldehyde (IC) are strong photo-sensitizers when irradiated with near-UV. In the presence of volatile organic compounds such as terpenes, this chemistry leads to a fast aerosol growth. Given the potential importance of this new photosensitized growth pathway for ambient OA, the related reaction mechanism was investigated at a molecular level. Bulk and flow tube experiments were performed to identify major products of the reaction of limonene with the triplet state of IC by direct (+/-)ESI-HRMS and UPLC/(+/-)HESI-HRMS analysis. Detection of recombination products of IC with limonene or with itself, in bulk and flow tube experiment ts, showed that IC is able to initiate a radical chemistry in the aerosol phase under realistic irradiation conditions. Furthermore, highly oxygenated limonene reaction products were detected, clearly explaining the observed OA growth. The chemistry of peroxy radicals derived from limonene upon addition of oxygen explains the formation of such low-volatile compounds without any traditional gas phase oxidant. These results demonstrate that, upon ageing, organic aerosols can produce photo-sensitizers which auto-photo-catalyse their SOA growth.

A water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pinterich, Tamara; Spielman, Steven R.; Hering, Susanne

We developed a water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range. The WFIMS builds on two established technologies: the fast integrated mobility spectrometer and laminar flow water-based condensation methodology. Inside WFIMS, particles of differing electrical mobility are separated in a drift tube and subsequently enlarged through water condensation. Particle size and concentration are measured via digital imaging at a frame rate of 10 Hz. When we measure particles of different mobilities simultaneously, the WFIMS resolves particle diameters ranging from 8 to 580 nm within 1 s or less. The performance of WFIMS was characterized with differential mobilitymore » analyzer (DMA) classified (NH 4) 2SO 2 particles with diameters ranging from 8 to 265 nm. The mean particle diameters measured by WFIMS were found to be in excellent agreement with DMA centroid diameters. Furthermore, detection efficiency of WFIMS was characterized using a condensation particle counter as a reference and is nearly 100% for particles with diameter greater than 8 nm. In general, measured and simulated WFIMS mobility resolutions are in good agreement. But, some deviations are observed at low particle mobilities, likely due to the non-idealities of the WFIMS electric field.« less

A water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range

DOE PAGES

Pinterich, Tamara; Spielman, Steven R.; Hering, Susanne; ...

2017-06-08

We developed a water-based fast integrated mobility spectrometer (WFIMS) with enhanced dynamic size range. The WFIMS builds on two established technologies: the fast integrated mobility spectrometer and laminar flow water-based condensation methodology. Inside WFIMS, particles of differing electrical mobility are separated in a drift tube and subsequently enlarged through water condensation. Particle size and concentration are measured via digital imaging at a frame rate of 10 Hz. When we measure particles of different mobilities simultaneously, the WFIMS resolves particle diameters ranging from 8 to 580 nm within 1 s or less. The performance of WFIMS was characterized with differential mobilitymore » analyzer (DMA) classified (NH 4) 2SO 2 particles with diameters ranging from 8 to 265 nm. The mean particle diameters measured by WFIMS were found to be in excellent agreement with DMA centroid diameters. Furthermore, detection efficiency of WFIMS was characterized using a condensation particle counter as a reference and is nearly 100% for particles with diameter greater than 8 nm. In general, measured and simulated WFIMS mobility resolutions are in good agreement. But, some deviations are observed at low particle mobilities, likely due to the non-idealities of the WFIMS electric field.« less

Gas-phase hydrolysis of triplet SO2: A possible direct route to atmospheric acid formation

NASA Astrophysics Data System (ADS)

Donaldson, D. James; Kroll, Jay A.; Vaida, Veronica

2016-07-01

Sulfur chemistry is of great interest to the atmospheric chemistry of several planets. In the presence of water, oxidized sulfur can lead to new particle formation, influencing climate in significant ways. Observations of sulfur compounds in planetary atmospheres when compared with model results suggest that there are missing chemical mechanisms. Here we propose a novel mechanism for the formation of sulfurous acid, which may act as a seed for new particle formation. In this proposed mechanism, the lowest triplet state of SO2 (3B1), which may be accessed by near-UV solar excitation of SO2 to its excited 1B1 state followed by rapid intersystem crossing, reacts directly with water to form H2SO3 in the gas phase. For ground state SO2, this reaction is endothermic and has a very high activation barrier; our quantum chemical calculations point to a facile reaction being possible in the triplet state of SO2. This hygroscopic H2SO3 molecule may act as a condensation nucleus for water, giving rise to facile new particle formation (NPF).

Non-equilibrium Properties of a Pumped-Decaying Bose-Condensed Electron–Hole Gas in the BCS–BEC Crossover Region

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hanai, R.; Littlewood, P. B.; Ohashi, Y.

2016-03-01

We theoretically investigate a Bose-condensed exciton gas out of equilibrium. Within the framework of the combined BCS-Leggett strong-coupling theory with the non-equilibrium Keldysh formalism, we show how the Bose-Einstein condensation (BEC) of excitons is suppressed to eventually disappear, when the system is in the non-equilibrium steady state. The supply of electrons and holes from the bath is shown to induce quasi-particle excitations, leading to the partial occupation of the upper branch of Bogoliubov single-particle excitation spectrum. We also discuss how this quasi-particle induction is related to the suppression of exciton BEC, as well as the stability of the steady state.

Focusing particle concentrator with application to ultrafine particles

DOEpatents

Hering, Susanne; Lewis, Gregory; Spielman, Steven R.

2013-06-11

Technology is presented for the high efficiency concentration of fine and ultrafine airborne particles into a small fraction of the sampled airflow by condensational enlargement, aerodynamic focusing and flow separation. A nozzle concentrator structure including an acceleration nozzle with a flow extraction structure may be coupled to a containment vessel. The containment vessel may include a water condensation growth tube to facilitate the concentration of ultrafine particles. The containment vessel may further include a separate carrier flow introduced at the center of the sampled flow, upstream of the acceleration nozzle of the nozzle concentrator to facilitate the separation of particle and vapor constituents.

Size distributions of hydrophilic and hydrophobic fractions of water-soluble organic carbon in an urban atmosphere in Hong Kong

NASA Astrophysics Data System (ADS)

Wang, Nijing; Yu, Jian Zhen

2017-10-01

Water-soluble organic carbon (WSOC) is a significant part of ambient aerosol and plays an active role in contributing to aerosol's effect on visibility degradation and radiation budget through its interactions with atmospheric water. Size-segregated aerosol samples in the range of 0.056-18 μm were collected using a ten-stage impactor sampler at an urban site in Hong Kong over one-year period. The WSOC samples were separated into hydrophilic (termed WSOC_h) and hydrophobic fractions (i.e., the humic-like substances (HULIS) fraction) through solid-phase extraction procedure. Carbon in HULIS accounted for 40 ± 14% of WSOC. The size distribution of HULIS was consistently characterized in all seasons with a dominant droplet mode (46-71%) and minor condensation (9.0-18%) and coarse modes (20-35%). The droplet mode had a mass median aerodynamic diameter in the range of 0.7-0.8 μm. This size mode showed the largest seasonal variation in abundance, lowest in the summer (0.41 μg/m3) and highest in the winter (3.3 μg/m3). WSOC_h also had a dominant droplet mode, but was more evenly distributed among different size modes. Inter-species correlations within the same size mode suggest that the condensation-mode HULIS was partly associated with combustion sources and the droplet-mode was strongly associated with secondary sulfate formation and biomass burning particle aging processes. There is evidence to suggest that the coarse-mode HULIS largely originated from coagulation of condensation-mode HULIS with coarse soil/sea salt particles. The formation process and possible sources of WSOC_h was more complicated and multiple than HULIS and need further investigation. Our measurements indicate that WSOC components contributed a dominant fraction of water-soluble aerosol mass in particles smaller than 0.32 μm while roughly 20-30% in the larger particles.

Glass Frit Filters for Collecting Metal Oxide Nanoparticles

NASA Technical Reports Server (NTRS)

Ackerman, John; Buttry, Dan; Irvine, Geoffrey; Pope, John

2005-01-01

Filter disks made of glass frit have been found to be effective as means of high-throughput collection of metal oxide particles, ranging in size from a few to a few hundred nanometers, produced in gas-phase condensation reactors. In a typical application, a filter is placed downstream of the reactor and a valve is used to regulate the flow of reactor exhaust through the filter. The exhaust stream includes a carrier gas, particles, byproducts, and unreacted particle-precursor gas. The filter selectively traps the particles while allowing the carrier gas, the byproducts, and, in some cases, the unreacted precursor, to flow through unaffected. Although the pores in the filters are much larger than the particles, the particles are nevertheless trapped to a high degree: Anecdotal information from an experiment indicates that 6-nm-diameter particles of MnO2 were trapped with greater than 99-percent effectiveness by a filtering device comprising a glass-frit disk having pores 70 to 100 micrometer wide immobilized in an 8-cm-diameter glass tube equipped with a simple twist valve at its downstream end.

Trace element geochemistry of volcanic gases and particles from 1983--1984 eruptive episodes of Kilauea volcano

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crowe, B.M.; Finnegan, D.L.; Zoller, W.H.

1987-12-10

Compositional data have been obtained for volcanic gases and particles collected from fume emitted at the Pu'u O'o vent on the east rift zone of Kilauea volcano. The samples were collected by pumping fume through a filter pack system consisting of a front stage particulate filter followed by four base-treated filters (/sup 7/LiOH). Particles and condensed phases are trapped on the particulate filter, and acidic gases are collected on the treated filters. The filters are analyzed for 30 elements by instrumental neutron activation analysis. Fume samples were collected from the Pu'u O'o vent for two eruptive episodes: (1) 7 daysmore » after episode 11 (cooling vent samples) and (2) the stage of episode 13 (active vent samples).« less

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

NASA Astrophysics Data System (ADS)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

Morphological transformation of soot: investigation of microphysical processes during the condensation of sulphuric acid and limonene ozonolysis products vapours

NASA Astrophysics Data System (ADS)

Pathak, R. K. P.; Pei, X.; Hallquist, M.; Pagels, J. H.

2017-12-01

Morphological transformation of soot particle by condensation of low volatility materials on it is a dominant atmospheric process with serious implications for its optical and hygroscopic properties, and atmospheric lifetime. In this study, the morphological transformation of soot agglomerate under the influence of condensation of vapours of sulphuric acid, and/or limonene ozonolysis products were investigated systematically using a Differential Mobility Analyser-Aerosol Particle Mass Analyser (DMA-APM) and the Tandem DMA techniques integrated with a laminar flow-tube system. We discovered that the morphology transformation of soot in general was a sequence of two-step process, i.e. (i) filling of void space within soot agglomerate; (ii) growth of particle diameter. These two steps followed and complimented each other. In the very beginning the filling was the dominant process followed by growth until it led to the accumulation of enough material that in turn exerted surface forces that eventually facilitated the further filling. The filling of void space was constrained by the initial morphology of fresh soot and the nature and amount of the material condensed. This process continued in several sequential steps until all void space within the soot agglomerate was filled completely and then growth of a spherical particle continued as long as mass was condensed on it. In this study, we developed a framework to quantify the microphysical transformation of soot upon the condensation of various materials. The framework utilized experimental data and hypothesis of ideal sphere growth and filling of voids to quantify the distribution of condensed materials in these two processes complimenting each other. Using this framework, we have quantified the percentage of material that went into processes of particle growth and void filling at each step. Using the same framework, we further estimated the fraction of internal voids and open voids and used this information to derive the volume equivalent diameter of soot agglomerate containing internal voids and calculated in-situ dynamic shape factor. Our study is the first study that tracks in situ microphysical changes in soot morphology quantitatively, providing the detailed status of both fresh and coated soot particles.

Antimicrobial activity of silica coated silicon nano-tubes (SCSNT) and silica coated silicon nano-particles (SCSNP) synthesized by gas phase condensation.

PubMed

Tank, Chiti; Raman, Sujatha; Karan, Sujoy; Gosavi, Suresh; Lalla, Niranjan P; Sathe, Vasant; Berndt, Richard; Gade, W N; Bhoraskar, S V; Mathe, Vikas L

2013-06-01

Silica-coated, silicon nanotubes (SCSNTs) and silica-coated, silicon nanoparticles (SCSNPs) have been synthesized by catalyst-free single-step gas phase condensation using the arc plasma process. Transmission electron microscopy and scanning tunneling microscopy showed that SCSNTs exhibited a wall thickness of less than 1 nm, with an average diameter of 14 nm and a length of several 100 nm. Both nano-structures had a high specific surface area. The present study has demonstrated cheaper, resistance-free and effective antibacterial activity in silica-coated silicon nano-structures, each for two Gram-positive and Gram-negative bacteria. The minimum inhibitory concentration (MIC) was estimated, using the optical densitometric technique, and by determining colony-forming units. The MIC was found to range in the order of micrograms, which is comparable to the reported MIC of metal oxides for these bacteria. SCSNTs were found to be more effective in limiting the growth of multidrug-resistant Staphylococcus aureus over SCSNPs at 10 μg/ml (IC 50 = 100 μg/ml).

Velocity and void distribution in a counter-current two-phase flow

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gabriel, S.; Schulenberg, T.; Laurien, E.

2012-07-01

Different flow regimes were investigated in a horizontal channel. Simulating a hot leg injection in case of a loss of coolant accident or flow conditions in reflux condenser mode, the hydraulic jump and partially reversed flow were identified as major constraints for a high amount of entrained water. Trying to simulate the reflux condenser mode, the test section now includes an inclined section connected to a horizontal channel. The channel is 90 mm high and 110 mm wide. Tests were carried out for water and air at ambient pressure and temperature. High speed video-metry was applied to obtain velocities frommore » flow pattern maps of the rising and falling fluid. In the horizontal part of the channel with partially reversed flow the fluid velocities were measured by planar particle image velocimetry. To obtain reliable results for the gaseous phase, this analysis was extended by endoscope measurements. Additionally, a new method based on the optical refraction at the interface between air and water in a back-light was used to obtain time-averaged void fraction. (authors)« less

Ultrafine particle and fiber production in microgravity

NASA Technical Reports Server (NTRS)

Webb, George W. (Inventor)

1988-01-01

In a system and method for producing ultrafine particles and ultrafine fibers of a given source material by evaporating and condensing the material in a gas atmosphere that includes inert gas. A smaller, more narrow size distribution is accomplished by producing the particles and fibers in a microgravity environment in order to reduce particle coalescence caused by convection currents. Particle coalescence also is reduced in an Earth gravity environment by controlling the convection currents. Condensed particles are collected either by providing an electrostatic field or a spatially varying magnetic field or by causing the gas to move through a filter which collects the particles. Nonferromagnetic material fibers are produced and collected by electrodes which produce an electro- static field. Ferromagnetic particles are collected by spatially varying magnetic fields.

The origins of particle size effects in heterogeneous catalysis

NASA Astrophysics Data System (ADS)

Bond, Geoffrey C.

1985-06-01

Model calculations are presented to show how the fraction of atoms at the surface of small metal particles increases as their size diminishes in the range 10 to 2 nm. Such particles are prepared either by condensing atoms or aggregates from the vapour phase onto a support, or by chemical methods in the liquid phase, i.e. the traditional routes for preparing supported metal catalysts. The first group of methods leads to artificially pure materials in which the contact between metal and support is poor. The second group of methods leads to the introduction of impurities, to a greater variety of forms of particle, but to a generally firmer binding of metal to support: this permits electronic interactions between the components to occur. Recent literature on the chemisorptive and catalytic properties of metal particles, usually less than 10 nm in size, suggests that certain classes of reaction may be designated as "structure-insensitive" in that their rates depend only minimally on particle size, whereas others, denoted as "structure-sensitive", have rates which either increase or decrease with size. After discounting trivial effects, a hard core of results remains, demanding explanation. Although certain hydrocarbon transformations appear to need sites comprising more than a certain minimum number of atoms, it is thought that the electronic character of surface atoms plays a greater role than their geometric disposition.

Occurrence and possible significance of rare Ti oxides (Magneli phases) in carbonaceous chondrite matrices

NASA Technical Reports Server (NTRS)

Brearley, Adrian J.

1993-01-01

Rare, ultrafine-grained Ti oxides (Ti3O5 and the Magneli phases, Ti5O9 and Ti8O15) have been identified by TEM in the CM2 carbonaceous chondrite, Bells, and a carbonaceous chondrite matrix clast from the Nilpena polymict ureilite. In both meteorites the Ti oxides occur in the matrix as isolated grains and clusters of two or more grains. They are euhedral in shape and have grain sizes of 0.05-0.3 micron. Magneli phases have been recently shown to be a common component in some interplanetary dust particles, but this is the first reported occurrence in a meteorite. The morphological properties and grain size of the Ti oxides are consistent with formation by vapor phase condensation either within the solar nebula or possibly in a presolar environment.

Low-energy excitations of a Bose-Einstein condensate of rigid rotor molecules

NASA Astrophysics Data System (ADS)

Smith, Joseph; Jones, Evan; Rittenhouse, Seth; Wilson, Ryan; Peden, Brandon

2017-04-01

We investigate the properties of the ground state and low-lying excitations of an oblate Bose-Einstein condensate composed of rigid rotor molecules in the presence of an external polarizing electric field. We build in a quantum model of molecular polarizability by including the full manifold of rotational states. The interplay between spatial and microscopic degrees of freedom via feedback between the molecular polarizability and inter-molecular dipole-dipole interactions leads to a rich quasi-particle spectrum. Under large applied fields, we reproduce the well-understood density-wave rotonization that appears in a fully polarized dipolar BEC, but under smaller applied fields, we predict the emergence of a spin wave instability and possible new stable ground state phases. We gratefully acknowledge support from the National Science Foundation under Grant No. PHYS-1516421.

Efimov-driven phase transitions of the unitary Bose gas.

PubMed

Piatecki, Swann; Krauth, Werner

2014-03-20

Initially predicted in nuclear physics, Efimov trimers are bound configurations of three quantum particles that fall apart when any one of them is removed. They open a window into a rich quantum world that has become the focus of intense experimental and theoretical research, as the region of 'unitary' interactions, where Efimov trimers form, is now accessible in cold-atom experiments. Here we use a path-integral Monte Carlo algorithm backed up by theoretical arguments to show that unitary bosons undergo a first-order phase transition from a normal gas to a superfluid Efimov liquid, bound by the same effects as Efimov trimers. A triple point separates these two phases and another superfluid phase, the conventional Bose-Einstein condensate, whose coexistence line with the Efimov liquid ends in a critical point. We discuss the prospects of observing the proposed phase transitions in cold-atom systems.

Size-controlled, magnetic, and core-shell nanoparticles synthesized by inert-gas condensation

NASA Astrophysics Data System (ADS)

Koten, Mark A.

Interest in nanoparticles (2 to 100 nm in diameter) and clusters of atoms (0.5 to 2 nm in diameter) has heightened over the past two and a half decades on both fundamental and functional levels. Nanoparticles and clusters of atoms are an exciting branch of materials science because they do not behave like normal bulk matter, nor do they act like molecules. They can have shockingly different physical, chemical, optical, or magnetic properties from the same material at a larger scale. In the case of nanoparticles, the surface-to-volume ratio can change fundamental properties like melting temperature, binding energy, or electron affinity. The definitions of markers used to distinguish between metallic, semiconducting, and insulating bulk condensed matter, such as the band gap and polarizability, can even be blurred or confused on the nanoscale. Similarly, clusters of atoms can form in structures that are only stable at finite sizes, and do not translate to bulk condensed matter. Thermodynamics of finite systems changes dramatically in nanovolumes such as wires, rods, cubes, and spheres, which can lead to complex core-shell and onion-like nanostructures. Consequently, these changes in properties and structure have led to many new possibilities in the field of materials engineering. Inert-gas condensation (IGC) is a well-established method of producing nanoparticles that condense from the gas phase. Its first use dates back to the early 1990s, and it has been used to fabricate nanoparticles both commercially and in research and development for applications in magnetism, biomedicine, and catalysts. In this dissertation, IGC was used to produce a wide variety of nanoparticles. First, control over the size distributions of Cu nanoparticles and how it relates to the plasma properties inside the nucleation chamber was investigated. Next, the formation of phase pure WFe2 nanoparticles revealed that this Laves phase is ferromagnetic instead of non-magnetic. Finally, core-shell nanoparticles were produced using three thermodynamically different systems, which showed that IGC could be used to produce a wide variety of core-shell particles. These three projects are presented in the context of size-dependent structural and magnetic properties.

Toward the Characterization of Mixed-Phase Clouds Using Remote Sensing

NASA Astrophysics Data System (ADS)

Andronache, C.

2015-12-01

Mixed-phase clouds consist of a mixture of ice particles and liquid droplets at temperatures below 0 deg C. They are present in all seasons in many regions of the world, account for about 30% of the global cloud coverage, and are linked to cloud electrification and aircraft icing. The mix of ice particles, liquid droplets, and water vapor is unstable, and such clouds are thought to have a short lifetime. A characteristic parameter is the phase composition of mixed-phase clouds. It affects the cloud life cycle and the rate of precipitation. This parameter is important for cloud parameters retrievals by radar, lidar, and satellite and is relevant for climate modeling. The phase transformation includes the remarkable Wegener-Bergeron-Findeisen (WBF) process. The direction and the rate of the phase transformations depend on the local thermodynamic and microphysical properties. Cloud condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and the dynamic response of clouds to aerosols. The complexity of dynamics and microphysics involved in mixed-phase clouds requires a set of observational and modeling tools that continue to be refined. Among these techniques, the remote sensing methods provide an increasing number of parameters, covering large regions of the world. Thus, a series of studies were dedicated to stratiform mixed-phase clouds revealing longer lifetime than previously thought. Satellite data and aircraft in situ measurements in deep convective clouds suggest that highly supercooled water often occurs in vigorous continental convective storms. In this study, we use cases of convective clouds to discuss the feasibility of mixed-phase clouds characterization and potential advantages of remote sensing.

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water content and increases the cloud glaciation temperature, while increasing CCN has the opposite effect with much smaller significance.« less

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE PAGES

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; ...

2017-01-23

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water content and increases the cloud glaciation temperature, while increasing CCN has the opposite effect with much smaller significance.« less

Geometry-induced phase transition in fluids: Capillary prewetting

NASA Astrophysics Data System (ADS)

Yatsyshin, Petr; Savva, Nikos; Kalliadasis, Serafim

2013-02-01

We report a new first-order phase transition preceding capillary condensation and corresponding to the discontinuous formation of a curved liquid meniscus. Using a mean-field microscopic approach based on the density functional theory we compute the complete phase diagram of a prototypical two-dimensional system exhibiting capillary condensation, namely that of a fluid with long-ranged dispersion intermolecular forces which is spatially confined by a substrate forming a semi-infinite rectangular pore exerting long-ranged dispersion forces on the fluid. In the T-μ plane the phase line of the new transition is tangential to the capillary condensation line at the capillary wetting temperature Tcw. The surface phase behavior of the system maps to planar wetting with the phase line of the new transition, termed capillary prewetting, mapping to the planar prewetting line. If capillary condensation is approached isothermally with T>Tcw, the meniscus forms at the capping wall and unbinds continuously, making capillary condensation a second-order phenomenon. We compute the corresponding critical exponent for the divergence of adsorption.

Fermion masses through four-fermion condensates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ayyar, Venkitesh; Chandrasekharan, Shailesh

Fermion masses can be generated through four-fermion condensates when symmetries prevent fermion bilinear condensates from forming. This less explored mechanism of fermion mass generation is responsible for making four reduced staggered lattice fermions massive at strong couplings in a lattice model with a local four-fermion coupling. The model has a massless fermion phase at weak couplings and a massive fermion phase at strong couplings. In particular there is no spontaneous symmetry breaking of any lattice symmetries in both these phases. Recently it was discovered that in three space-time dimensions there is a direct second order phase transition between the twomore » phases. Here we study the same model in four space-time dimensions and find results consistent with the existence of a narrow intermediate phase with fermion bilinear condensates, that separates the two asymptotic phases by continuous phase transitions.« less

3D mixing in hot Jupiters atmospheres. I. Application to the day/night cold trap in HD 209458b

NASA Astrophysics Data System (ADS)

Parmentier, Vivien; Showman, Adam P.; Lian, Yuan

2013-10-01

Context. Hot Jupiters exhibit atmospheric temperatures ranging from hundreds to thousands of Kelvin. Because of their large day-night temperature differences, condensable species that are stable in the gas phase on the dayside - such as TiO and silicates - may condense and gravitationally settle on the nightside. Atmospheric circulation may counterbalance this tendency to gravitationally settle. This three-dimensional (3D) mixing of condensable species has not previously been studied for hot Jupiters, yet it is crucial to assess the existence and distribution of TiO and silicates in the atmospheres of these planets. Aims: We investigate the strength of the nightside cold trap in hot Jupiters atmospheres by investigating the mechanisms and strength of the vertical mixing in these stably stratified atmospheres. We apply our model to the particular case of TiO to address the question of whether TiO can exist at low pressure in sufficient abundances to produce stratospheric thermal inversions despite the nightside cold trap. Methods: We modeled the 3D circulation of HD 209458b including passive (i.e. radiatively inactive) tracers that advect with the 3D flow, with a source and sink term on the nightside to represent their condensation into haze particles and their gravitational settling. Results: We show that global advection patterns produce strong vertical mixing that can keep condensable species aloft as long as they are trapped in particles of sizes of a few microns or less on the nightside. We show that vertical mixing results not from small-scale convection but from the large-scale circulation driven by the day-night heating contrast. Although this vertical mixing is not diffusive in any rigorous sense, a comparison of our results with idealized diffusion models allows a rough estimate of the effective vertical eddy diffusivities in these atmospheres. The parametrization Kzz=5 × 104/ Pbar m2s-1, valid from ~1 bar to a few μbar, can be used in 1D models of HD 209458b. Moreover, our models exhibit strong spatial and temporal variability in the tracer concentration that could result in observable variations during either transit or secondary eclipse measurements. Finally, we apply our model to the case of TiO in HD 209458b and show that the day-night cold trap would deplete TiO if it condenses into particles bigger than a few microns on the planet's nightside, keeping it from creating the observed stratosphere of the planet. Appendix A is available in electronic form at http://www.aanda.org

Heat storage system utilizing phase change materials government rights

DOEpatents

Salyer, Ival O.

2000-09-12

A thermal energy transport and storage system is provided which includes an evaporator containing a mixture of a first phase change material and a silica powder, and a condenser containing a second phase change material. The silica powder/PCM mixture absorbs heat energy from a source such as a solar collector such that the phase change material forms a vapor which is transported from the evaporator to the condenser, where the second phase change material melts and stores the heat energy, then releases the energy to an environmental space via a heat exchanger. The vapor is condensed to a liquid which is transported back to the evaporator. The system allows the repeated transfer of thermal energy using the heat of vaporization and condensation of the phase change material.

Condensed matter analogues of cosmology

NASA Astrophysics Data System (ADS)

Kibble, Tom; Srivastava, Ajit

2013-10-01

It is always exciting when developments in one branch of physics turn out to have relevance in a quite different branch. It would be hard to find two branches farther apart in terms of energy scales than early-universe cosmology and low-temperature condensed matter physics. Nevertheless ideas about the formation of topological defects during rapid phase transitions that originated in the context of the very early universe have proved remarkably fruitful when applied to a variety of condensed matter systems. The mathematical frameworks for describing these systems can be very similar. This interconnection has led to a deeper understanding of the phenomena in condensed matter systems utilizing ideas from cosmology. At the same time, one can view these condensed matter analogues as providing, at least in a limited sense, experimental access to the phenomena of the early universe for which no direct probe is possible. As this special issue well illustrates, this remains a dynamic and exciting field. The basic idea is that when a system goes through a rapid symmetry-breaking phase transition from a symmetric phase into one with spontaneously broken symmetry, the order parameter may make different choices in different regions, creating domains that when they meet can trap defects. The scale of those domains, and hence the density of defects, is constrained by the rate at which the system goes through the transition and the speed with which order parameter information propagates. This is what has come to be known as the Kibble-Zurek mechanism. The resultant scaling laws have now been tested in a considerable variety of different systems. The earliest experiments illustrating the analogy between cosmology and condensed matter were in liquid crystals, in particular on the isotropic-to-nematic transition, primarily because it is very easy to induce the phase transition (typically at room temperature) and to image precisely what is going on. This field remains one of the liveliest. A number of new experiments are reported here studying the dynamical evolution of domains and defects. Another phenomenon that played a key early role was the formation of vortices in the normal-to-superfluid transition in liquid helium-3. The complicated nature of the order parameter energy surface gives rise to a variety of intriguing effects. This too is still a vigorous field. Superconductivity is a special case because the symmetry that is broken is a gauge symmetry. This is also true in fundamental particle physics theories of relevance to cosmology, and for that reason experiments on superconductors are of particular interest to cosmologists. The situation in this case is more complicated because there are competing mechanisms of defect formation. Experiments in the field have not proved easy, either to perform or to interpret, but the papers in this collection show that good progress has been made of late. In recent years a new type of system has proved immensely fruitful, namely atomic Bose-Einstein or Fermi-gas condensates. Experiments on condensates with tunable parameters have in general provided broad support for the theory, and have also revealed a wide range of interesting and novel features, with intriguing possible analogues in cosmology (e.g. causal horizons and particle creation). The basic idea of the Kibble-Zurek mechanism has been shown to be relevant in this whole range of systems. But numerous complexities have also emerged, concerned for example with the role of inhomogeneity or the existence of composite defects. The field is still developing rapidly. Acknowledgments Finally, we would like to thank all the authors who have contributed to this issue, and the staff of Journal of Physics: Condensed Matter who have made it possible. Condensed matter analogues of cosmology contents Condensed matter analogues of cosmologyTom Kibble and Ajit Srivastava Symmetry breaking in nematic liquid crystals: analogy with cosmology and magnetismR Repnik, A Ranjkesh, V Simonka, M Ambrozic, Z Bradac and S Kralj Morphogenesis of defects and tactoids during isotropic-nematic phase transition in self-assembled lyotropic chromonic liquid crystalsYoung-Ki Kim, Sergij V Shiyanovskii and Oleg D Lavrentovich Annihilation dynamics of stringlike topological defects in a nematic lyotropic liquid crystalR R Guimarães, R S Mendes, P R G Fernandes and H Mukai Duality between the dynamics of line-like brushes of point defects in 2D and strings in 3D in liquid crystalsSanatan Digal, Rajarshi Ray, P S Saumia and Ajit M Srivastava The multiuniverse transition in superfluid 3HeYury Bunkov Coherent topological defect dynamics and collective modes in superconductors and electronic crystalsD Mihailovic, T Mertelj, V V Kabanov and S Brazovskii Gaussianity revisited: exploring the Kibble-Zurek mechanism with superconducting ringsD J Weir, R Monaco, V P Koshelets, J Mygind and R J Rivers The Kibble-Zurek mechanism in a subcritical bifurcationM A Miranda, D Laroze and W González-Viñas Topological relics of symmetry breaking: winding numbers and scaling tilts from random vortex-antivortex pairsW H Zurek Causality and non-equilibrium second-order phase transitions in inhomogeneous systemsA del Campo, T W B Kibble and W H Zurek The role of causality in tunable Fermi gas condensatesJen-Tsung Hsiang, Chi-Yong Lin, Da-Shin Lee and Ray J Rivers Kibble-Zurek mechanism in a trapped ferromagnetic Bose-Einstein condensateHiroki Saito, Yuki Kawaguchi and Masahito Ueda D-brane solitons and boojums in field theory and Bose-Einstein condensatesKenichi Kasamatsu, Hiromitsu Takeuchi and Muneto Nitta Kibble-Zurek scaling and string-net coarsening in topologically ordered systemsAnushya Chandran, F J Burnell, Vedika Khemani and S L Sondhi Universal frozen spectra after time-dependent symmetry restoring phase transitionsFriedemann Queisser, Patrick Navez and Ralf Schützhold Microscopic theory of non-adiabatic response in real and imaginary timeC De Grandi, A Polkovnikov and A W Sandvik

Modelling compressible dense and dilute two-phase flows

NASA Astrophysics Data System (ADS)

Saurel, Richard; Chinnayya, Ashwin; Carmouze, Quentin

2017-06-01

Many two-phase flow situations, from engineering science to astrophysics, deal with transition from dense (high concentration of the condensed phase) to dilute concentration (low concentration of the same phase), covering the entire range of volume fractions. Some models are now well accepted at the two limits, but none are able to cover accurately the entire range, in particular regarding waves propagation. In the present work, an alternative to the Baer and Nunziato (BN) model [Baer, M. R. and Nunziato, J. W., "A two-phase mixture theory for the deflagration-to-detonation transition (DDT) in reactive granular materials," Int. J. Multiphase Flow 12(6), 861 (1986)], initially designed for dense flows, is built. The corresponding model is hyperbolic and thermodynamically consistent. Contrarily to the BN model that involves 6 wave speeds, the new formulation involves 4 waves only, in agreement with the Marble model [Marble, F. E., "Dynamics of a gas containing small solid particles," Combustion and Propulsion (5th AGARD Colloquium) (Pergamon Press, 1963), Vol. 175] based on pressureless Euler equations for the dispersed phase, a well-accepted model for low particle volume concentrations. In the new model, the presence of pressure in the momentum equation of the particles and consideration of volume fractions in the two phases render the model valid for large particle concentrations. A symmetric version of the new model is derived as well for liquids containing gas bubbles. This model version involves 4 characteristic wave speeds as well, but with different velocities. Last, the two sub-models with 4 waves are combined in a unique formulation, valid for the full range of volume fractions. It involves the same 6 wave speeds as the BN model, but at a given point of space, 4 waves only emerge, depending on the local volume fractions. The non-linear pressure waves propagate only in the phase with dominant volume fraction. The new model is tested numerically on various test problems ranging from separated phases in a shock tube to shock-particle cloud interaction. Its predictions are compared to BN and Marble models as well as against experimental data showing clear improvements.

Condensational Droplet Growth in Rarefied Quiescent Vapor and Forced Convective Conditions

NASA Astrophysics Data System (ADS)

Anand, Sushant

Multiphase Heat transfer is ubiquitous in diverse fields of application such as cooling systems, micro and mini power systems and many chemical processes. By now, single phase dynamics are mostly understood in their applications in vast fields, however multiphase systems especially involving phase changes are still a challenge. Present study aims to enhance understanding in this domain especially in the field of condensation heat transfer. Of special relevance to present studies is study of condensation phenomenon for detection of airborne nanoparticles using heterogeneous nucleation. Detection of particulate matter in the environment via heterogeneous condensation is based on the droplet growth phenomenon where seeding particles in presence of supersaturated vapor undergo condensation on their surface and amplify in size to micrometric ranges, thereby making them optically visible. Previous investigations show that condensation is a molecular exchange process affected by mean free path of vapor molecules (lambda) in conjunction with size of condensing droplet (d), which is measured in terms of Knudsen number (Kn=lambda/ d). In an event involving heterogeneous nucleation with favorable thermodynamic conditions for condensation to take place, the droplet growth process begins with accretion of vapor molecules on a surface through random molecular collision (Kn>1) until diffusive forces start dominating the mass transport process (Kn<<1). Knowledge of droplet growth thus requires understanding of mass transport in both of these regimes. Present study aims to understand the dynamics of the Microthermofluidic sensor which has been developed, based on above mentioned fundamentals. Using continuum approach, numerical modeling was carried to understand the effect of various system parameters for improving the device performance to produce conditions which can lead to conditions abetting condensational growth. The study reveals that the minimum size of nanoparticle which can be detected is critically dependent upon controlling wall geometry and size, wall temperature, flow rate and relative humidity of nanoparticle laden air stream. Droplet growths rates and sizes have been predicted based on different models. The efficacy of the device under various conditions has been measured in terms of its ability to activate nanoparticles of different sizes. Since the condensation mechanism is dependent upon the Knudsen regime in which droplets are growing via condensation, special consideration was made to understand their behavior in large Knudsen number conditions. For this purpose, ESEM was used to study condensation on a bare surface. Droplet growth obtained as a function of time reveals that the rate of growth decreases as the droplet increases in size. The experimental results obtained from these experiments were matched with theoretical description provided by a model based on framework of kinetic theory. Evidence was also found which establishes the presence of submicroscopic droplets nucleating and growing in between microscopic droplets for partially wetting case.

Analytical electron microscopy of fine-grained phases in primitive interplanetary dust particles and carbonaceous chondrites

NASA Technical Reports Server (NTRS)

Mackinnon, Ian D. R.; Rietmeijer, Frans J. M.; Mckay, David S.

1987-01-01

In order to describe the total mineralogical diversity within primitive extraterrestrial materials, individual interplanetary dust particles (IDPs) collected from the stratosphere as part of the JSC Cosmic Dust Curatorial Program were analyzed using a variety of AEM techniques. Identification of over 250 individual grains within one chondritic porous (CP) IDP shows that most phases could be formed by low temperature processes and that heating of the IDP during atmospheric entry is minimal and less than 600 C. In a review of the mineralogy of IDPs, it was suggested that the occurrence of other silicates such as enstatite whiskers is consistent with the formation in an early turbulent period of the solar nebula. Experimental confirmation of fundamental chemical and physical processes in a stellar environment, such as vapor phase condensation, nucleation, and growth by annealing, is an important aspect of astrophysical models for the evolution of the Solar System. A detailed comparison of chondritic IDP and carbonaceous chondrite mineralogies shows significant differences between the types of silicate minerals as well as the predominant oxides.

Dense crystalline packings of ellipsoids

NASA Astrophysics Data System (ADS)

Jin, Weiwei; Jiao, Yang; Liu, Lufeng; Yuan, Ye; Li, Shuixiang

2017-03-01

An ellipsoid, the simplest nonspherical shape, has been extensively used as a model for elongated building blocks for a wide spectrum of molecular, colloidal, and granular systems. Yet the densest packing of congruent hard ellipsoids, which is intimately related to the high-density phase of many condensed matter systems, is still an open problem. We discover an unusual family of dense crystalline packings of self-dual ellipsoids (ratios of the semiaxes α : √{α }:1 ), containing 24 particles with a quasi-square-triangular (SQ-TR) tiling arrangement in the fundamental cell. The associated packing density ϕ exceeds that of the densest known SM2 crystal [ A. Donev et al., Phys. Rev. Lett. 92, 255506 (2004), 10.1103/PhysRevLett.92.255506] for aspect ratios α in (1.365, 1.5625), attaining a maximal ϕ ≈0.758 06 ... at α = 93 /64 . We show that the SQ-TR phase derived from these dense packings is thermodynamically stable at high densities over the aforementioned α range and report a phase diagram for self-dual ellipsoids. The discovery of the SQ-TR crystal suggests organizing principles for nonspherical particles and self-assembly of colloidal systems.

Novel Quantum Criticality in Two Dimensional Topological Phase transitions

PubMed Central

Cho, Gil Young; Moon, Eun-Gook

2016-01-01

Topological quantum phase transitions intrinsically intertwine self-similarity and topology of many-electron wave-functions, and divining them is one of the most significant ways to advance understanding in condensed matter physics. Our focus is to investigate an unconventional class of the transitions between insulators and Dirac semimetals whose description is beyond conventional pseudo relativistic Dirac Hamiltonian. At the transition without the long-range Coulomb interaction, the electronic energy dispersion along one direction behaves like a relativistic particle, linear in momentum, but along the other direction it behaves like a non-relativistic particle, quadratic in momentum. Various physical systems ranging from TiO2-VO2 heterostructure to organic material α-(BEDT-TTF)2I3 under pressure have been proposed to have such anisotropic dispersion relation. Here, we discover a novel quantum criticality at the phase transition by incorporating the long range Coulomb interaction. Unique interplay between the Coulomb interaction and electronic critical modes enforces not only the anisotropic renormalization of the Coulomb interaction but also marginally modified electronic excitation. In connection with experiments, we investigate several striking effects in physical observables of our novel criticality. PMID:26791803

Mineralogy, textures and mode of formation of a hibonite-bearing Allende inclusion

NASA Technical Reports Server (NTRS)

Allen, J. M.; Grossman, L.; Davis, A. M.; Hutcheon, I. D.

1978-01-01

The origin of a Type A, hibonite-rich, coarse-grained inclusion is investigated with the electron microprobe and petrographic and scanning electron microscopes. The primary phases are hibonite, rhonite, Ti-Al-pyroxene, spinel, perovskite and melilite. Evidence for the crystallization of the bulk of the primary phases, hibonite and melilite, from a melt is lacking, suggesting that they may have condensed directly from a solar nebular gas instead. Primary phases were intensely altered during a later condensation event which deposited grossular, anorthite, nepheline and wollastonite in veins and cavities. Four or five condensate rims were deposited as successive layers on the outside of the inclusion. From inside to outside, they consist of perovskite + spinel, nepheline + anorthite, Ti-Al-pyroxene + diopside, hedenbergite + or - wollastonite + or - andradite and, finally, prisms of diopside and hedenbergite with wollastonite and andradite. Reverse zoning in melilite; alteration phases and rim phases, which are not stable condensates from a gas of solar composition; and details of the sequence of rim condensates all suggest that the entire condensation history of this inclusion was interrupted by changes in pressure and/or temperature and/or gas phase composition.

Evaluation and modelling of the size fractionated aerosol particle number concentration measurements nearby a major road in Helsinki - Part I: Modelling results within the LIPIKA project

NASA Astrophysics Data System (ADS)

Pohjola, M. A.; Pirjola, L.; Karppinen, A.; Härkönen, J.; Korhonen, H.; Hussein, T.; Ketzel, M.; Kukkonen, J.

2007-08-01

A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17-20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm-10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3-50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. For model comparison purposes, one of the cases was additionally computed using the aerosol process model UHMA, combined with the CAR-FMI model. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible on this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm-3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the concentration of condensable organic vapour of 109-1010 molecules cm-3 resulted in particle sizes that were closest to the measured values.

Sulfur and Sulfuric Acid Microphysics in the Venus Atmosphere: Implications for the Unknown UV Absorber

NASA Astrophysics Data System (ADS)

Gao, P.; Carlson, R. W.; Robinson, T. D.; Crisp, D.; Lyons, J. R.; Yung, Y. L.

2016-12-01

A mystery that has continued to plague our sister planet, Venus, for nearly a century is the nature of the brightness contrasts observed crisscrossing its disk in near-ultraviolet wavelength images. These contrasts - specifically the dark regions - have been attributed to the actions of an unknown UV absorber, knowing the identity of which is integral to understanding the Venus atmosphere due to the high rates of mesospheric heating attributed to the absorption of solar UV. One possible candidate for the UV absorber is polysulfur, which form from polymerization of elemental sulfur arising from SO2 photolysis at the Venus cloud tops under low O2 conditions. In this work we investigate the microphysics of condensed polysulfur and its interaction with the sulfuric acid clouds. We consider the "gumdrop model", where sulfur is allowed to condense onto sulfuric acid cloud particles. We explore the possibility that S2 vapor may condense faster than its loss to gas phase reactions that produce higher allotropes, leading to solid state polymerization to S8. This process may explain the ephemeral and variable nature of the UV absorption.

Accelerating activity coefficient calculations using multicore platforms, and profiling the energy use resulting from such calculations.

NASA Astrophysics Data System (ADS)

Topping, David; Alibay, Irfan; Bane, Michael

2017-04-01

To predict the evolving concentration, chemical composition and ability of aerosol particles to act as cloud droplets, we rely on numerical modeling. Mechanistic models attempt to account for the movement of compounds between the gaseous and condensed phases at a molecular level. This 'bottom up' approach is designed to increase our fundamental understanding. However, such models rely on predicting the properties of molecules and subsequent mixtures. For partitioning between the gaseous and condensed phases this includes: saturation vapour pressures; Henrys law coefficients; activity coefficients; diffusion coefficients and reaction rates. Current gas phase chemical mechanisms predict the existence of potentially millions of individual species. Within a dynamic ensemble model, this can often be used as justification for neglecting computationally expensive process descriptions. Indeed, on whether we can quantify the true sensitivity to uncertainties in molecular properties, even at the single aerosol particle level it has been impossible to embed fully coupled representations of process level knowledge with all possible compounds, typically relying on heavily parameterised descriptions. Relying on emerging numerical frameworks, and designed for the changing landscape of high-performance computing (HPC), in this study we focus specifically on the ability to capture activity coefficients in liquid solutions using the UNIFAC method. Activity coefficients are often neglected with the largely untested hypothesis that they are simply too computationally expensive to include in dynamic frameworks. We present results demonstrating increased computational efficiency for a range of typical scenarios, including a profiling of the energy use resulting from reliance on such computations. As the landscape of HPC changes, the latter aspect is important to consider in future applications.

In-Flight Annealing of Magnetic Nanoparticles, Produced by the Particle Gun Technique

NASA Astrophysics Data System (ADS)

Stoyanov, S.; Skumryev, V.; Zhang, Y.; Huang, Y.; Hadjipanayis, G. C.

2003-03-01

The need of post annealing of nanocomposite structures aimed to form nanoparticles or to obtain a desired crystal structure often results in particles growth and/or a harmful alloying with the matrix material. In this study, we present a new technique to perform an in situ phase transformation of particles produced by the gas condensation process in a Particle Gun (PG). Particles are heat treated during their flight from the PG to the substrate, by absorption of light in a specially designed Heating Stage (HS), placed on the top of the PG. The total power of the light sources used is 2 kWatt. A simple model for the thermodynamic conditions in a single particle during the annealing process is developed. It is shown that the temperature of the particle depends on the light power and the size of the particle and can easily reach the required annealing values of 400 to 900^oC in a millisecond time scale. The versatility of this technique is demonstrated on the fabrication of high anisotropy FePt and SmCo particles, embedded in a carbon matrix. Work supported by NSF DMR9972035

Examining Model Atmospheric Particles Inside and Out

NASA Astrophysics Data System (ADS)

Wingen, L. M.; Zhao, Y.; Fairhurst, M. C.; Perraud, V. M.; Ezell, M. J.; Finlayson-Pitts, B. J.

2017-12-01

Atmospheric particles scatter incoming solar radiation and act as cloud condensation nuclei (CCN), thereby directly and indirectly affecting the earth's radiative balance and reducing visibility. These atmospheric particles may not be uniform in composition. Differences in the composition of a particle's outer surface from its core can arise during particle growth, (photo)chemical aging, and exchange of species with the gas phase. The nature of the surface on a molecular level is expected to impact growth mechanisms as well as their ability to act as CCN. Model laboratory particle systems are explored using direct analysis in real time-mass spectrometry (DART-MS), which is sensitive to surface composition, and contrasted with average composition measurements using high resolution, time-of-flight aerosol mass spectrometry (HR-ToF-AMS). Results include studies of the heterogeneous reactions of amines with solid dicarboxylic acid particles, which are shown to generate aminium dicarboxylate salts at the particle surface, leaving an unreacted core. Combination of both mass spectrometric techniques reveals a trend in reactivity of C3-C7 dicarboxylic acids with amines and allows calculation of the DART probe depth into the particles. The results of studies on additional model systems that are currently being explored will also be reported.

Analysis of flame spread over multicomponent combustibles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohtani, H.; Sato, J.

1985-01-01

A theoretical model of volatile component diffusion in the condensed phase is carried out in order to form a basis for predicting the flame spread rate in thermally thick multicomponent combustibles in a non-fluid condensed phase. The fuels could be, e.g., crude oil, heavy oil, or light oil. Mass transfer occurs only by diffusion so the gas phase volatile concentration at the surface is estimated from the condensed phase volatile concentration and the surface temperature, which increases close to the leading flame edge. The flame spread rate is assumed steady. The velocity of the flame spread is shown to bemore » a function of the initial condensed phase temperature and the temperature at the leading flame edge.« less

ON THE ORIGIN AND PHYSICS OF GAMMA FLARES IN CRAB NEBULA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Machabeli, George; Rogava, Andria; Shapakidze, David, E-mail: andria.rogava@iliauni.edu.ge

We consider parametric generation of electrostatic waves in the magnetosphere of the pulsar PSR0531. The suggested mechanism allows us to convert the pulsar rotational energy into the energy of Langmuir waves. The maximum growth rate is achieved in the “superluminal” area, where the phase velocity of perturbations exceeds the speed of light. Therefore, electromagnetic waves do not damp on particles. Instead, they create plasmon condensate, which is carried out outside of the pulsar magnetosphere and reaches the Crab Nebula. It is shown that the transfer of the energy of the plasmon condensate from the light cylinder to the active regionmore » of the nebula happens practically without losses. Unlike the plasma of the magnetosphere, the one of the nebula contains ions, i.e., it may sustain modulation instability, that leads to the collapse of the Langmuir condensate. Langmuir wave collapse, in turn, leads to the acceleration of the distribution function particles. Furthermore, the processes that lead to self-trapping of the synchrotron radiation are discussed. The self-trapping results in the growth of the radiation intensity, which manifests itself observationally as a flare. The condition for the self-trapping onset is derived, showing that if the phenomenon takes place at 100 MeV, then it does not happen at lower (or higher) energies. This specific kind of higher-/lower-energy cutoff could explain why when we observe the flare at 100 MeV that no enhanced emission is observed at lower/higher energies!.« less

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

NASA Technical Reports Server (NTRS)

Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

1980-01-01

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Measuring Uptake Coefficients and Henry's Law Constants of Gas-Phase Species with Models for Secondary Organic Aerosol

NASA Astrophysics Data System (ADS)

Fairhurst, M. C.; Waring-Kidd, C.; Ezell, M. J.; Finlayson-Pitts, B. J.

2014-12-01

Volatile organic compounds (VOC) are oxidized in the atmosphere and their products contribute to secondary organic aerosol (SOA) formation. These particles have been shown to have effects on visibility, climate, and human health. Current models typically under-predict SOA concentrations from field measurements. Underestimation of these concentrations could be a result of how models treat particle growth. It is often assumed that particles grow via instantaneous thermal equilibrium partitioning between liquid particles and gas-phase species. Recent work has shown that growth may be better represented by irreversible, kinetically limited uptake of gas-phase species onto more viscous, tar-like SOA. However, uptake coefficients for these processes are not known. The goal of this project is to measure uptake coefficients and solubilities for different gases onto models serving as proxies for SOA and determine how they vary based on the chemical composition of the gas and the condensed phase. Experiments were conducted using two approaches: attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy and a flow system coupled to a mass spectrometer. The ATR crystal was coated with the SOA proxy and the gas-phase species introduced via a custom flow system. Uptake of the gas-phase species was characterized by measuring the intensity of characteristic IR bands as a function of time, from which a Henry's law constant and initial estimate of uptake coefficients could be obtained. Uptake coefficients were also measured in a flow system where the walls of the flow tube were coated with the SOA proxy and gas-phase species introduced via a moveable inlet. Uptake coefficients were derived from the decay in gas-phase species measured by mass spectrometry. The results of this work will establish a structure-interaction relationship for uptake of gases into SOA that can be implemented into regional and global models.

Compressible Heating in the Condense Phase due to Pore Collapse in HMX

NASA Astrophysics Data System (ADS)

Zhang, Ju; Jackson, Thomas

Axisymmetric pore collapse in HMX is studied numerically by solving multi-phase reactive Euler equations. The generation of hot spots in the condense phase due to compressible heating is examined. The motivation is to improve the understanding of the role of embedded cavities in the initiation of reaction in explosives, and to investigate the effect of hot spots in the condense phase due to compressible heating alone, complementing previous study on hot spots due to the reaction in the gas phase and at the interface. It is found that the shock-cavity interaction results in pressures and thus temperatures that are substantially higher than the post-shock values in the condense phase. However, these hot spots in the condense phase due to compressible heating alone do not seem to be sufficiently hot to lead to ignition at shock pressures of 1-3 GPa. Thus, compressible heating in the condense phase may be excluded as a mechanism for initiation of explosives. It should be pointed out that the ignition threshold for the temperature, the so-called ``switch-on'' temperature, of hot spots depend on chemistry kinetics parameters. Switch-on temperature is lower for faster reaction rate. The current chemistry kinetics parameters are based on previous experimental work. This work was supported in part by the Defense Threat Reduction Agency and by the U.S. Department of Energy.

Type-II Weyl semimetals.

PubMed

Soluyanov, Alexey A; Gresch, Dominik; Wang, Zhijun; Wu, QuanSheng; Troyer, Matthias; Dai, Xi; Bernevig, B Andrei

2015-11-26

Fermions--elementary particles such as electrons--are classified as Dirac, Majorana or Weyl. Majorana and Weyl fermions had not been observed experimentally until the recent discovery of condensed matter systems such as topological superconductors and semimetals, in which they arise as low-energy excitations. Here we propose the existence of a previously overlooked type of Weyl fermion that emerges at the boundary between electron and hole pockets in a new phase of matter. This particle was missed by Weyl because it breaks the stringent Lorentz symmetry in high-energy physics. Lorentz invariance, however, is not present in condensed matter physics, and by generalizing the Dirac equation, we find the new type of Weyl fermion. In particular, whereas Weyl semimetals--materials hosting Weyl fermions--were previously thought to have standard Weyl points with a point-like Fermi surface (which we refer to as type-I), we discover a type-II Weyl point, which is still a protected crossing, but appears at the contact of electron and hole pockets in type-II Weyl semimetals. We predict that WTe2 is an example of a topological semimetal hosting the new particle as a low-energy excitation around such a type-II Weyl point. The existence of type-II Weyl points in WTe2 means that many of its physical properties are very different to those of standard Weyl semimetals with point-like Fermi surfaces.

In Situ Visualization of the Growth and Fluctuations of Nanoparticle Superlattice in Liquids

NASA Astrophysics Data System (ADS)

Ou, Zihao; Shen, Bonan; Chen, Qian

We use liquid phase transmission electron microscopy to image and understand the crystal growth front and interfacial fluctuation of a nanoparticle superlattice. With single particle resolution and hundreds of nanoscale building blocks in view, we are able to identify the interface between ordered lattice and disordered structure and visualize the kinetics of single building block attachment at the lattice growth front. The spatial interfacial fluctuation profiles support the capillary wave theory, from which we derive a surface stiffness value consistent with scaling analysis. Our experiments demonstrate the potential of extending model study on collective systems to nanoscale with single particle resolution and testing fundamental theories of condensed matter at a length scale linking atoms and micron-sized colloids.

Pulmonary aerosol delivery and the importance of growth dynamics.

PubMed

Haddrell, Allen E; Lewis, David; Church, Tanya; Vehring, Reinhard; Murnane, Darragh; Reid, Jonathan P

2017-12-01

Aerosols are dynamic systems, responding to variations in the surrounding environmental conditions by changing in size, composition and phase. Although, widely used in inhalation therapies, details of the processes occurring on aerosol generation and during inhalation have received little attention. Instead, research has focused on improvements to the formulation of the drug prior to aerosolization and the resulting clinical efficacy of the treatment. Here, we highlight the processes that occur during aerosol generation and inhalation, affecting aerosol disposition when deposited and, potentially, impacting total and regional doses. In particular, we examine the response of aerosol particles to the humid environment of the respiratory tract, considering both the capacity of particles to grow by absorbing moisture and the timescale for condensation to occur. [Formula: see text].

Preparing ultrafine PbS powders from the scrap lead-acid battery by sulfurization and inert gas condensation

NASA Astrophysics Data System (ADS)

Xia, Huipeng; Zhan, Lu; Xie, Bing

2017-02-01

A novel method for preparing ultrafine PbS powders involving sulfurization combined with inert gas condensation is developed in this paper, which is applicable to recycle Pb from lead paste of spent lead-acid batteries. Initially, the effects of the evaporation and condensation temperature, the inert gas pressure, the condensation distance and substrate on the morphology of as-obtained PbS ultrafine particles are intensively investigated using sulfur powders and lead particles as reagents. Highly dispersed and homogeneous PbS nanoparticles can be prepared under the optimized conditions which are 1223 K heating temperature, 573 K condensation temperature, 100 Pa inert gas pressure and 60 cm condensation distance. Furthermore, this method is successfully applied to recycle Pb from the lead paste of spent lead acid battery to prepare PbS ultrafine powders. This work does not only provide the theoretical fundamental for PbS preparation, but also provides a novel and efficient method for recycling spent lead-acid battery with high added-value products.

Stratospheric aircraft exhaust plume and wake chemistry studies

NASA Technical Reports Server (NTRS)

Miake-Lye, R. C.; Martinez-Sanchez, M.; Brown, R. C.; Kolb, C. E.; Worsnop, D. R.; Zahniser, M. S.; Robinson, G. N.; Rodriguez, J. M.; Ko, M. K. W.; Shia, R-L.

1992-01-01

This report documents progress to date in an ongoing study to analyze and model emissions leaving a proposed High Speed Civil Transport (HSCT) from when the exhaust gases leave the engine until they are deposited at atmospheric scales in the stratosphere. Estimates are given for the emissions, summarizing relevant earlier work (CIAP) and reviewing current propulsion research efforts. The chemical evolution and the mixing and vortical motion of the exhaust are analyzed to track the exhaust and its speciation as the emissions are mixed to atmospheric scales. The species tracked include those that could be heterogeneously reactive on the surfaces of the condensed solid water (ice) particles and on exhaust soot particle surfaces. Dispersion and reaction of chemical constituents in the far wake are studied with a Lagrangian air parcel model, in conjunction with a radiation code to calculate the net heating/cooling. Laboratory measurements of heterogeneous chemistry of aqueous sulfuric acid and nitric acid hydrates are also described. Results include the solubility of HCl in sulfuric acid which is a key parameter for modeling stratospheric processing. We also report initial results for condensation of nitric acid trihydrate from gas phase H2O and HNO3.

New Approach for Gas Phase Synthesis and Growth Mechanism of MoS2 Fullerene-like Nanoparticles

NASA Astrophysics Data System (ADS)

Zak, Alla; Feldman, Yishay; Alperovich, Vladimir; Rosentsveig, Rita; Tenne, Reshef

2002-10-01

Inorganic fullerene-like (hollow onion-like) nanoparticles (IF) and nanotubes are of significant interest over the past few years due to their unusual crystallographic morphology and their interesting physical properties. The synthesis of inorganic fullerene-like spherical MoS2 nanoparticles (IF-MoS2) of 5-300nm in diameter was studied in the present work. This process is based on the previous formation of suboxide (MoO3-x) 5-300nm nanoparticles and their subsequent sulfidization. During the sulfidization process the overall geometrical parameters of the suboxide nanoparticles are preserved. The oxide nanoparticles were obtained in-situ by the condensation of the evaporated MoO3 powder precursor. The condensation was provoked not by cooling (conventional method for nano-size particle formation), but by a chemical reaction (partial reduction of the MoO3 vapor by hydrogen). In this case the vapor pressure of the product (MoO2) was much lower than that of the precursor (MoO3). Based on the comprehensive understanding of the IF-MoS2 growth mechanism from MoO3 powder, a gas phase reactor, which allowed reproducible preparation of a pure IF-MoS2 phase (up to 100mg/batch) with controllable sizes, is demonstrated. Further scale-up of this production is underway.

Thermal infrared properties of Titan's stratospheric aerosol

NASA Technical Reports Server (NTRS)

Samuelson, Robert E.; Mayo, Louis A.

1991-01-01

The monotonic increase with wavenumber of stratospheric IR opacities in the north polar neighborhood of Titan, in the 250-600/cm bandpass, becomes more extreme with decreasing altitude, consistent with an opacity that is primarily dependent on a high altitude photochemical aerosol, on the one hand, but which is moderated by condensed organics at lower altitudes. Because condensates exhibit a wavenumber dependence for opacity which is the opposite of that required, it is suggested that condensed nitriles may be prominent; either of these condensates may be acceptable for sufficiently large particles. While comparisons with low-latitude data indicate no clear dependence of vertically-integrated opacity on latitude above 80 km, indications of a particle size and/or composition gradient with latitude in the lower stratosphere are noted.

Aerosol processing of materials: Aerosol dynamics and microstructure evolution

NASA Astrophysics Data System (ADS)

Gurav, Abhijit Shankar

Spray pyrolysis is an aerosol process commonly used to synthesize a wide variety of materials in powder or film forms including metals, metal oxides and non-oxide ceramics. It is capable of producing high purity, unagglomerated, and micrometer to submicron-size powders, and scale-up has been demonstrated. This dissertation deals with the study of aerosol dynamics during spray pyrolysis of multicomponent systems involving volatile phases/components, and aspects involved with using fuel additives during spray processes to break apart droplets and particles in order to produce powders with smaller sizes. The gas-phase aerosol dynamics and composition size distributions were measured during spray pyrolysis of (Bi, Pb)-Sr-Ca-Cu-O, and Sr-Ru-O and Bi-Ru-O at different temperatures. A differential mobility analyzer (DMA) was used in conjunction with a condensation particle counter (CPC) to monitor the gas-phase particle size distributions, and a Berner-type low-pressure impactor was used to obtain mass size distributions and size-classified samples for chemical analysis. (Bi, Pb)-Sr-Ca-Cu-O powders made at temperatures up to 700sp°C maintained their initial stoichiometry over the whole range of particle sizes monitored, however, those made at 800sp°C and above were heavily depleted in lead in the size range 0.5-5.0 mum. When the reactor temperature was raised from 700 and 800sp°C to 900sp°C, a large number ({˜}10sp7\\ #/cmsp3) of new ultrafine particles were formed from PbO vapor released from the particles and the reactor walls at the beginning of high temperature runs (at 900sp°C). The metal ruthenate systems showed generation of ultrafine particles (<40-50 nm) at the beginning of runs at 800-900sp°C and also as a steady state process at a reactor temperature of 1000sp°C. The methods of aerosol dynamics measurements were also used to monitor the gas-phase particle size distributions during the generation of fullerene (Csb{60}) nano-particles (30 to 50 nm size) via vapor condensation at 400-650sp°C using Nsb2 carrier gas. In general, during laboratory-scale aerosol processing of materials containing a volatile component, significant evaporative losses and formation of new ultrafine particles were observed at synthesis temperatures at which the saturation vapor pressure of the volatile species exceeded about 0.1-0.5 mTorr. Spray calcination synthesis of pigment-size titania from titanium hydrolysate (TiOsb{x}(SOsb4)sb{y}(OH)sb{z}) using fuel additives such as ethyl alcohol, sugar and urea was also investigated. When pure water was used as a medium of suspension, agglomerates of 0.5 to 1.5 mum were produced by spray calcination. Use of pure ethanol as a solvent as well as small amounts (5-10 wt.%) urea additions to the suspension of Ti-hydrolysate in water were successful in producing predominantly unagglomerated, single crystalline titania particles of 0.1 to 0.3 mum size. Such additions of fuels such as alcohols, sugar and urea to suspensions and solutions used in spray processes are promising for making powders having smaller sizes and unagglomerated, denser morphologies.

Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine oxide particles in the coastal marine boundary layer

NASA Astrophysics Data System (ADS)

Murray, B. J.; Haddrell, A. E.; Peppe, S.; Davies, J. F.; Reid, J. P.; O'Sullivan, D.; Price, H. C.; Kumar, R.; Saunders, R. W.; Plane, J. M. C.; Umo, N. S.; Wilson, T. W.

2012-03-01

Iodine oxide particles are known to nucleate in the marine boundary layer where gas phase molecular iodine and organoiodine species are produced by macroalgae. There has been some debate over the chemical identity of these particles. Hygroscopic measurements have been used to infer that they are composed of insoluble I2O4, while elemental analysis of laboratory generated particles suggests soluble I2O5 or its hydrated form iodic acid, HIO3 (I2O5 · H2O). In this paper we explore the response of super-micron sized aqueous iodic acid solution droplets to varying humidity using both Raman microscopy and single particle electrodynamic traps. These measurements reveal that the propensity of an iodic acid solution droplet to crystallise is negligible on drying to ~0% relative humidity (RH). On applying mechanical pressure to these droplets they shatter in a manner consistent with an ultra-viscous liquid or a brittle glass, but subsequent water uptake between 10 and 20% RH causes their viscosity to reduce sufficiently that the cracked droplets flow and merge. The persistence of iodic acid solution in an amorphous state, rather than a crystalline state, suggests they will more readily accommodate other condensable material and are therefore more likely to grow to sizes where they may serve as cloud condensation nuclei. On increasing the humidity to ~90% the mass of the droplets only increases by ~20% with a corresponding increase in radius of only ~6 %, which is remarkably small for a highly soluble material. We suggest that the small growth factor of aqueous iodic acid solution droplets is consistent with the small aerosol growth factors observed in field experiments.

Structural and phase transformations in zinc and brass wires under heating with high-density current pulse

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pervikov, A. V.

The work is focused on revealing the mechanism of structure and phase transformations in the metal wires under heating with a high-density current pulse (the electric explosion of wires, EEWs). It has been demonstrated on the example of brass and zinc wires that the transition of a current pulse with the density of j ≈ 3.3 × 10{sup 7} A/cm{sup 2} results in homogeneous heating of the crystalline structure of the metal/alloy. It has been determined that under heating with a pulse of high-density current pulse, the electric resistance of the liquid phases of zinc and brass decreases as the temperature increases. The results obtainedmore » allow for a conclusion that the presence of the particles of the condensed phase in the expanding products of EEW is the result of overheating instabilities in the liquid metal.« less

Experiments With Trapped Neutral Atoms

DTIC Science & Technology

2010-01-05

number of condensate atoms in the trap [11]. (a) i solitons (b) £ 10 \\QT>J — \\^y Darks -WW . ’ VrV Ground state A(|>=0 <* -^ Mr...interacting condensates leading to soliton formation for a relative phase of Pi. (b) The relative phase of two split condensates was monitored for various

A hydroxyapatite coating covalently linked onto a silicone implant material.

PubMed

Furuzono, T; Sonoda, K; Tanaka, J

2001-07-01

A novel composite consisting of hydroxyapatite (HAp) microparticles covalently coupled onto a silicone sheet was developed. Initially, an acrylic acid (AAc) -grafted silicone sheet with a 16.7 microg/cm(2) surface graft density was prepared by corona-discharge treatment. The surface of sintered, spherical, carbonated HAp particles with an average diameter of 2.0 microm was subsequently modified with amino groups. The amino group surface density of the HAp particles was calculated to be approximately one amino molecule per 1.0 nm(2) of particle surface area. These samples were characterized with Fourier transform infrared spectrometry and X-ray photoelectron spectroscopy. After the formation of ammonium ionic bonds between both samples under aqueous conditions, they were reacted at 180 degrees C for 6 h in vacuo to form covalent bonds through a solid-phase condensation. The HAp particles were coupled to the AAc-grafted silicone surface by a covalent linkage. Further improvements in the adhesive and bioactive properties of the HAp-coated silicone material are expected.

Online single particle measurement of fireworks pollution during Chinese New Year in Nanning.

PubMed

Li, Jingyan; Xu, Tingting; Lu, Xiaohui; Chen, Hong; Nizkorodov, Sergey A; Chen, Jianmin; Yang, Xin; Mo, Zhaoyu; Chen, Zhiming; Liu, Huilin; Mao, Jingying; Liang, Guiyun

2017-03-01

Time-resolved single-particle measurements were conducted during Chinese New Year in Nanning, China. Firework displays resulted in a burst of SO 2 , coarse mode, and accumulation mode (100-500nm) particles. Through single particle mass spectrometry analysis, five different types of particles (fireworks-metal, ash, dust, organic carbon-sulfate (OC-sulfate), biomass burning) with different size distributions were identified as primary emissions from firework displays. The fireworks-related particles accounted for more than 70% of the total analyzed particles during severe firework detonations. The formation of secondary particulate sulfate and nitrate during firework events was investigated on single particle level. An increase of sulfite peak (80SO 3 - ) followed by an increase of sulfate peaks (97HSO 4 - +96SO 4 - ) in the mass spectra during firework displays indicated the aqueous uptake and oxidation of SO 2 on particles. High concentration of gaseous SO 2 , high relative humidity and high particle loading likely promoted SO 2 oxidation. Secondary nitrate formed through gas-phase oxidation of NO 2 to nitric acid, followed by the condensation into particles as ammonium nitrate. This study shows that under worm, humid conditions, both primary and secondary aerosols contribute to the particulate air pollution during firework displays. Copyright © 2016. Published by Elsevier B.V.

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

NASA Astrophysics Data System (ADS)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. Decreases in NOx emissions without simultaneous decreases in SO2 emissions increase new-particle formation and growth due to increased oxidation of SO2. The parameterization we describe here should allow for more accurate predictions of aerosol size distributions and a greater confidence in the effects of aerosols in climate and health studies.

Self-cleaning of superhydrophobic surfaces by spontaneously jumping condensate drops

NASA Astrophysics Data System (ADS)

Wisdom, Katrina; Watson, Jolanta; Watson, Gregory; Chen, Chuan-Hua

2012-11-01

The self-cleaning function of superhydrophobic surfaces is conventionally attributed to the removal of contaminating particles by impacting or rolling water droplets, which implies the action of external forces such as gravity. Here, we demonstrate a new self-cleaning mechanism, whereby condensate drops spontaneously jump upon coalescence on a superhydrophobic surface, and the merged drop self-propels away from the surface along with the contaminants. The jumping-condensate mechanism is shown to autonomously clean superhydrophobic cicada wings, where the contaminating particles cannot be removed by external wind flow. Our findings offer new insights for the development of self-cleaning materials.

Direct Measurements of Gas/Particle Partitioning and Mass Accommodation Coefficients in Environmental Chambers.

PubMed

Krechmer, Jordan E; Day, Douglas A; Ziemann, Paul J; Jimenez, Jose L

2017-10-17

Secondary organic aerosols (SOA) are a major contributor to fine particulate mass and wield substantial influences on the Earth's climate and human health. Despite extensive research in recent years, many of the fundamental processes of SOA formation and evolution remain poorly understood. Most atmospheric aerosol models use gas/particle equilibrium partitioning theory as a default treatment of gas-aerosol transfer, despite questions about potentially large kinetic effects. We have conducted fundamental SOA formation experiments in a Teflon environmental chamber using a novel method. A simple chemical system produces a very fast burst of low-volatility gas-phase products, which are competitively taken up by liquid organic seed particles and Teflon chamber walls. Clear changes in the species time evolution with differing amounts of seed allow us to quantify the particle uptake processes. We reproduce gas- and aerosol-phase observations using a kinetic box model, from which we quantify the aerosol mass accommodation coefficient (α) as 0.7 on average, with values near unity especially for low volatility species. α appears to decrease as volatility increases. α has historically been a very difficult parameter to measure with reported values varying over 3 orders of magnitude. We use the experimentally constrained model to evaluate the correction factor (Φ) needed for chamber SOA mass yields due to losses of vapors to walls as a function of species volatility and particle condensational sink. Φ ranges from 1-4.

Critical fermion density for restoring spontaneously broken symmetry

NASA Astrophysics Data System (ADS)

Kleinert, Hagen; Xue, She-Sheng

2015-07-01

We show how the phenomenon of spontaneous symmetry breakdown is affected by the presence of a sea of fermions in the system. When its density exceeds a critical value, the broken symmetry can be restored. We calculate the critical value and discuss the consequences for three different physical systems: First, for the Standard Model (SM) of particle physics, where the spontaneous symmetry breakdown leads to nonzero masses of intermediate gauge bosons and fermions. The symmetry restoration will greatly enhance various processes with dramatic consequences for the early universe. Second, for the Gell-Mann-Lévy σ-model of nuclear physics, where the symmetry breakdown gives rise to the nucleon and meson masses. The symmetry restoration may have important consequences for formation or collapse of stellar cores. Third, for the superconductive phase of condensed-matter, where the BCS condensate at low-temperature may be destroyed by a too large electron density.

Substantial Seasonal Contribution of Observed Biogenic Sulfate Particles to Cloud Condensation Nuclei.

PubMed

Sanchez, Kevin J; Chen, Chia-Li; Russell, Lynn M; Betha, Raghu; Liu, Jun; Price, Derek J; Massoli, Paola; Ziemba, Luke D; Crosbie, Ewan C; Moore, Richard H; Müller, Markus; Schiller, Sven A; Wisthaler, Armin; Lee, Alex K Y; Quinn, Patricia K; Bates, Timothy S; Porter, Jack; Bell, Thomas G; Saltzman, Eric S; Vaillancourt, Robert D; Behrenfeld, Mike J

2018-02-19

Biogenic sources contribute to cloud condensation nuclei (CCN) in the clean marine atmosphere, but few measurements exist to constrain climate model simulations of their importance. The chemical composition of individual atmospheric aerosol particles showed two types of sulfate-containing particles in clean marine air masses in addition to mass-based Estimated Salt particles. Both types of sulfate particles lack combustion tracers and correlate, for some conditions, to atmospheric or seawater dimethyl sulfide (DMS) concentrations, which means their source was largely biogenic. The first type is identified as New Sulfate because their large sulfate mass fraction (63% sulfate) and association with entrainment conditions means they could have formed by nucleation in the free troposphere. The second type is Added Sulfate particles (38% sulfate), because they are preexisting particles onto which additional sulfate condensed. New Sulfate particles accounted for 31% (7 cm -3 ) and 33% (36 cm -3 ) CCN at 0.1% supersaturation in late-autumn and late-spring, respectively, whereas sea spray provided 55% (13 cm -3 ) in late-autumn but only 4% (4 cm -3 ) in late-spring. Our results show a clear seasonal difference in the marine CCN budget, which illustrates how important phytoplankton-produced DMS emissions are for CCN in the North Atlantic.

Element Mapping in Anhydrous IDPs: Identification of the Host Phases of Major/Minor Elements as a Test of Nebula Condensation Models

NASA Technical Reports Server (NTRS)

Flynn, G. J.; Keller, L. P.; Wirick, S.; Jacobsen, C.

2004-01-01

Many anhydrous interplanetary dust particles (IDPs) are the most pristine samples of primitive solar system dust currently available for laboratory analysis. Their primitive nature is demonstrated by: 1) the high content of moderately volatile elements, indicating they have not been heated significantly since formation, 2) the absence of hydrated material, indicating they never experienced aqueous processing, 3) the presence of unequilibrated mineral assemblages, 4) the presence of large isotopic anomalies (e.g., D and 15N enrichment), in these IDPs.

Equilibrium and disequilibrium chemistry of adiabatic, solar-composition planetary atmospheres

NASA Technical Reports Server (NTRS)

Lewis, J. S.

1976-01-01

The impact of atmospheric and cloud-structure models on the nonequilibrium chemical behavior of the atmospheres of the Jovian planets is discussed. Quantitative constraints on photochemical, lightning, and charged-particle production of organic matter and chromophores are emphasized whenever available. These considerations imply that inorganic chromophore production is far more important than that of organic chromophores, and that lightning is probably a negligibly significant process relative to photochemistry on Jupiter. Production of complex molecules by gas-phase disequilibrium processes on Saturn, Uranus, and Neptune is severely limited by condensation of even simple intermediates.

Two-phase flow pressure drop and heat transfer during condensation in microchannels with uniform and converging cross-sections

NASA Astrophysics Data System (ADS)

Kuo, Ching Yi; Pan, Chin

2010-09-01

This study experimentally investigates steam condensation in rectangular microchannels with uniform and converging cross-sections and a mean hydraulic diameter of 135 µm. The steam flow in the microchannels was cooled by water cross-flowing along its bottom surface, which is different from other methods reported in the literature. The flow patterns, two-phase flow pressure drop and condensation heat transfer coefficient are determined. The microchannels with the uniform cross-section design have a higher heat transfer coefficient than those with the converging cross-section under condensation in the mist/annular flow regimes, although the latter work best for draining two-phase fluids composed of uncondensed steam and liquid water, which is consistent with the result of our previous study. From the experimental results, dimensionless correlations of condensation heat transfer for the mist and annular flow regions and a two-phase frictional multiplier are developed for the microchannels with both types of cross-section designs. The experimental data agree well with the obtained correlations, with the maximum mean absolute errors of 6.4% for the two-phase frictional multiplier and 6.0% for the condensation heat transfer.

A Local Condensation Analysis Representing Two-phase Annular Flow in Condenser/radiator Capillary Tubes

NASA Technical Reports Server (NTRS)

Karimi, Amir

1991-01-01

NASA's effort for the thermal environmental control of the Space Station Freedom is directed towards the design, analysis, and development of an Active Thermal Control System (ATCS). A two phase, flow through condenser/radiator concept was baselined, as a part of the ATCS, for the radiation of space station thermal load into space. The proposed condenser rejects heat through direct condensation of ATCS working fluid (ammonia) in the small diameter radiator tubes. Analysis of the condensation process and design of condenser tubes are based on the available two phase flow models for the prediction of flow regimes, heat transfer, and pressure drops. The prediction formulas use the existing empirical relationships of friction factor at gas-liquid interface. An attempt is made to study the stability of interfacial waves in two phase annular flow. The formulation is presented of a stability problem in cylindrical coordinates. The contribution of fluid viscosity, surface tension, and transverse radius of curvature to the interfacial surface is included. A solution is obtained for Kelvin-Helmholtz instability problem which can be used to determine the critical and most dangerous wavelengths for interfacial waves.

ATom observations of new particle formation in the tropical upper troposphere. The role of convection and nucleation mechanisms

NASA Astrophysics Data System (ADS)

Kupc, A.; Williamson, C.; Hodshire, A. L.; Pierce, J. R.; Ray, E. A.; Froyd, K. D.; Richardson, M.; Weinzierl, B.; Dollner, M.; Erdesz, F.; Bui, T. V.; Diskin, G. S.; Brock, C. A.

2017-12-01

Measurements of size distributions during the Atmospheric Tomography Mission (ATom) reveal high number concentrations (>>1000 cm-3) of nucleation mode particles at high altitudes in the tropics and subtropics under low condensation sink conditions and are associated with upwelling in convective clouds. The broad spatial extent of these newly formed particles shows that the upper free troposphere (FT) of the tropics and subtropics is a globally significant source. In this study, we investigate the link between convection and new particle formation (NPF) by exploring the processes that govern NPF and growth in the tropical and subtropical FT of the Pacific and Atlantic Oceans. We use measurements of the size distributions made with a suite of fast-response instruments on board of a NASA DC-8 aircraft during ATom mission. ATom maps the remote atmosphere over the Pacific and Atlantic basins ( 80 °N and 65 °S) in continuous ascents and descents (0.2 and 13 km), providing the latitudinal and vertical information on the greenhouse gases, reactive and tracer species and aerosol properties and their seasonal variability. We couple measurements of size distributions between 0.003 and 4.8 µm and potential aerosol precursor vapors measured on ATom (August 2016 and February 2017) with calculated air mass back trajectories and the TwO-Moment Aerosol Sectional (TOMAS) box model. The back trajectories identify air masses potentially influenced by recent convection. We then use TOMAS to model particle nucleation, condensation and coagulation along that trajectory to investigate the link between convection and NPF. Through TOMAS, we explore the influence of different nucleation mechanisms (such as binary, ternary or the one with organics) and gas-phase aerosol precursors (such as sulfur dioxide) on observed particle size distributions. We discuss similarities and differences in NPF over the Pacific and Atlantic Oceans and their relationship to convection, examine particle composition and volatility from in situ measurements, and examine which nucleation schemes are most consistent with the observations.

GoAmazon 2014/15 Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS) Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, JN

2016-04-01

The Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS) deployment to the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility T3 site in Manacapuru, Brazil, was motivated by two main scientific objectives of the Green Ocean Amazon (GoAmazon) 2014/15 field campaign. 1) Study the interactions between anthropogenic and biogenic emissions by determining important molecular species in ambient nanoparticles. To address this, TDCIMS data will be combined with coincident measurements such as gas-phase sulfuric acid to determine the contribution of sulfuric acid condensation to nucleation and growth. We can then compare that result to TDCIMS-derived nanoparticle composition tomore » determine the fraction of growth that can be attributed to the uptake of organic compounds. The molecular composition of sampled particles will also be used to attribute specific chemical species and mechanisms to growth, such as the condensation of low-volatility species or the oligomerization of α-dicarbonyl compounds. 2) Determine the source of new ambient nanoparticles in the Amazon. The hypothesis prior to measurements was that potassium salts formed from the evaporation of primary particles emitted by fungal spores can provide a unique and important pathway for new particle production in the Amazon basin. To explore this hypothesis, the TDCIMS recorded the mass spectra of sampled ambient particles using a protonated water cluster Chemical Ionization Mass Spectrometer (CIMS). Laboratory tests performed using potassium salts show that the TDCIMS can detect potassium with high sensitivity with this technique.« less

Atmospheric new particle formation at the research station Melpitz, Germany: connection with gaseous precursors and meteorological parameters

NASA Astrophysics Data System (ADS)

Größ, Johannes; Hamed, Amar; Sonntag, André; Spindler, Gerald; Elina Manninen, Hanna; Nieminen, Tuomo; Kulmala, Markku; Hõrrak, Urmas; Plass-Dülmer, Christian; Wiedensohler, Alfred; Birmili, Wolfram

2018-02-01

This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2-20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.

Uncertainty in aerosol hygroscopicity resulting from semi-volatile organic compounds

NASA Astrophysics Data System (ADS)

Goulden, Olivia; Crooks, Matthew; Connolly, Paul

2018-01-01

We present a novel method of exploring the effect of uncertainties in aerosol properties on cloud droplet number using existing cloud droplet activation parameterisations. Aerosol properties of a single involatile particle mode are randomly sampled within an uncertainty range and resulting maximum supersaturations and critical diameters calculated using the cloud droplet activation scheme. Hygroscopicity parameters are subsequently derived and the values of the mean and uncertainty are found to be comparable to experimental observations. A recently proposed cloud droplet activation scheme that includes the effects of co-condensation of semi-volatile organic compounds (SVOCs) onto a single lognormal mode of involatile particles is also considered. In addition to the uncertainties associated with the involatile particles, concentrations, volatility distributions and chemical composition of the SVOCs are randomly sampled and hygroscopicity parameters are derived using the cloud droplet activation scheme. The inclusion of SVOCs is found to have a significant effect on the hygroscopicity and contributes a large uncertainty. For non-volatile particles that are effective cloud condensation nuclei, the co-condensation of SVOCs reduces their actual hygroscopicity by approximately 25 %. A new concept of an effective hygroscopicity parameter is introduced that can computationally efficiently simulate the effect of SVOCs on cloud droplet number concentration without direct modelling of the organic compounds. These effective hygroscopicities can be as much as a factor of 2 higher than those of the non-volatile particles onto which the volatile organic compounds condense.

Condensation of Forced Convection Two-Phase Flow in a Miniature Tube

NASA Technical Reports Server (NTRS)

Begg, E.; Faghri, A.; Krustalev, D.

1999-01-01

A physical/mathematical model of annular film condensation at the inlet of a miniature tube has been developed. In the model, the liquid flow is coupled with the vapor flow along the liquid-vapor interface through the interfacial temperature, heat flux, shear stress, and pressure jump conditions due to surface tension effects. The model predicts the shape of the liquid-vapor interface along the condenser and leads to the conclusion that there is complete condensation at a certain distance from the condenser inlet. The numerical results show that complete condensation of the incoming vapor is possible at comparatively low heat loads and that this is a special case of a more general condensation regime with two-phase bubbly flow downstream of the initial annular film condensation region. Observations from the flow visualization experiment confirm the existence and qualitative features of annular film condensation leading to the complete condensation phenomenon in a small diameter (3.25 mm) circular tube condenser.

Organic Nitrate Contribution to New Particle Formation and Growth in Secondary Organic Aerosols from α-Pinene Ozonolysis.

PubMed

Berkemeier, Thomas; Ammann, Markus; Mentel, Thomas F; Pöschl, Ulrich; Shiraiwa, Manabu

2016-06-21

The chemical kinetics of organic nitrate production during new particle formation and growth of secondary organic aerosols (SOA) were investigated using the short-lived radioactive tracer (13)N in flow-reactor studies of α-pinene oxidation with ozone. Direct and quantitative measurements of the nitrogen content indicate that organic nitrates accounted for ∼40% of SOA mass during initial particle formation, decreasing to ∼15% upon particle growth to the accumulation-mode size range (>100 nm). Experiments with OH scavengers and kinetic model results suggest that organic peroxy radicals formed by α-pinene reacting with secondary OH from ozonolysis are key intermediates in the organic nitrate formation process. The direct reaction of α-pinene with NO3 was found to be less important for particle-phase organic nitrate formation. The nitrogen content of SOA particles decreased slightly upon increase of relative humidity up to 80%. The experiments show a tight correlation between organic nitrate content and SOA particle-number concentrations, implying that the condensing organic nitrates are among the extremely low volatility organic compounds (ELVOC) that may play an important role in the nucleation and growth of atmospheric nanoparticles.

Dimethylamine as a major alkyl amine species in particles and cloud water: Observations in semi-arid and coastal regions.

PubMed

Youn, J-S; Crosbie, E; Maudlin, L C; Wang, Z; Sorooshian, A

2015-12-01

Aerosol and cloud water measurements of dimethylamine (DMA), the most abundant amine in this study, were conducted in semi-arid (Tucson, Arizona) and marine (Nucleation in California Experiment, NiCE; central coast of California) areas. In both regions, DMA exhibits a unimodal aerosol mass size distribution with a dominant peak between 0.18 and 0.56 μm. Particulate DMA concentrations increase as a function of marine biogenic emissions, sulfate, BVOC emissions, and aerosol-phase water. Such data supports biogenic sources of DMA, aminium salt formation, and partitioning of DMA to condensed phases. DMA concentrations exhibit positive correlations with various trace elements and most especially vanadium, which warrants additional investigation. Cloud water DMA levels are enhanced significantly during wildfire periods unlike particulate DMA levels, including in droplet residual particles, due to effective dissolution of DMA into cloud water and probably DMA volatilization after drop evaporation. DMA:NH + 4 molar ratios peak between 0.18 and 1.0 μm depending on the site and time of year, suggesting that DMA competes better with NH 3 in those sizes in terms of reactive uptake by particles.

Influence of different propellant systems on ablation of EPDM insulators in overload state

NASA Astrophysics Data System (ADS)

Guan, Yiwen; Li, Jiang; Liu, Yang; Xu, Tuanwei

2018-04-01

This study examines the propellants used in full-scale solid rocket motors (SRM) and investigates how insulator ablation is affected by two propellant formulations (A and B) during flight overload conditions. An experimental study, theoretical analysis, and numerical simulations were performed to discover the intrinsic causes of insulator ablation rates from the perspective of lab-scaled ground-firing tests, the decoupling of thermochemical ablation, and particle erosion. In addition, the difference in propellant composition, and the insulator charring layer microstructure were analyzed. Results reveal that the degree of insulator ablation is positively correlated with the propellant burn rate, particle velocity, and aggregate concentrations during the condensed phase. A lower ratio of energetic additive material in the AP oxidizer of the propellant is promising for the reduction in particle size and increase in the burn rate and pressure index. However, the overall higher velocity of a two-phase flow causes severe erosion of the insulation material. While the higher ratio of energetic additive to the AP oxidizer imparts a smaller ablation rate to the insulator (under lab-scale test conditions), the slag deposition problem in the combustion chamber may cause catastrophic consequences for future large full-scale SRM flight experiments.

Non-Gaussian precision metrology via driving through quantum phase transitions

NASA Astrophysics Data System (ADS)

Huang, Jiahao; Zhuang, Min; Lee, Chaohong

2018-03-01

We propose a scheme to realize high-precision quantum interferometry with entangled non-Gaussian states by driving the system through quantum phase transitions. The beam splitting, in which an initial nondegenerate ground state evolves into a highly entangled state, is achieved by adiabatically driving the system from a nondegenerate regime to a degenerate one. Inversely, the beam recombination, in which the output state after interrogation becomes gradually disentangled, is accomplished by adiabatically driving the system from the degenerate regime to the nondegenerate one. The phase shift, which is accumulated in the interrogation process, can then be easily inferred via population measurement. We apply our scheme to Bose condensed atoms and trapped ions and find that Heisenberg-limited precision scalings can be approached. Our proposed scheme does not require single-particle resolved detection and is within the reach of current experiment techniques.

An investigation of the microstructure and mechanical properties of electrochemically coated Ag(4)Sn dental alloy particles condensed in vitro

NASA Astrophysics Data System (ADS)

Marquez, Jose Antonio

As part of the ongoing scientific effort to develop a new amalgam-like material without mercury, a team of metallurgists and electrochemists at the National Institute of Standards and Technology (NIST) in Gaithersburg, Maryland, announced in 1993 the development of a new Ag-Sn dental alloy system without mercury that sought to replace conventional dental amalgams. They used spherical Ag3Sn and Ag4Sn intermetallic dental alloy particles, commonly used in conventional dental alloys, and coated them with electrodeposited silver with newly-developed electrolytic and immersion techniques. The particles had relatively pure silver coatings that were closely adherent to the intermetalfic cores. These silver-coated particles, due to silver's plasticity at room temperature, were condensed into PlexiglasRTM molds with the aid of an acidic surface activating solution (HBF4) and a mechanical condensing device, producing a metal-matrix composite with Ag3,4Sn filler particles surrounded by a cold-welded silver matrix. Since silver strain hardens rather easily, the layers had to be condensed in less than 0.5 mm increments to obtain a dense structure. Mechanical testing at NIST produced compressive strength values equal to or greater than those of conventional dental amalgams. Because of its potential for eliminating mercury as a constituent in dental amalgam, this material created a stir in dental circles when first developed and conceivably could prove to be a major breakthrough in the field of dental restoratives. To date, the chief impediments to its approval for human clinical applications by the Food and Drug Administration are the potentially-toxic surface activating solution used for oxide reduction, and the high condensation pressures needed for cold welding because of the tendency for silver to strain harden. In this related study, the author, who has practiced general dentistry for 25 years, evaluates some of the mechanical and microstructural properties of these electrochemically coated particles when they are amalgamated with mercury. Because of patent restrictions for the coated particles that protect the cold-welding work being done at NIST, these particles necessarily had to include mercury as a constituent for this investigation. (Abstract shortened by UMI.)

Modeling the Hydrological Cycle in the Atmosphere of Mars: Influence of a Bimodal Size Distribution of Aerosol Nucleation Particles

NASA Astrophysics Data System (ADS)

Shaposhnikov, Dmitry S.; Rodin, Alexander V.; Medvedev, Alexander S.; Fedorova, Anna A.; Kuroda, Takeshi; Hartogh, Paul

2018-02-01

We present a new implementation of the hydrological cycle scheme into a general circulation model of the Martian atmosphere. The model includes a semi-Lagrangian transport scheme for water vapor and ice and accounts for microphysics of phase transitions between them. The hydrological scheme includes processes of saturation, nucleation, particle growth, sublimation, and sedimentation under the assumption of a variable size distribution. The scheme has been implemented into the Max Planck Institute Martian general circulation model and tested assuming monomodal and bimodal lognormal distributions of ice condensation nuclei. We present a comparison of the simulated annual variations, horizontal and vertical distributions of water vapor, and ice clouds with the available observations from instruments on board Mars orbiters. The accounting for bimodality of aerosol particle distribution improves the simulations of the annual hydrological cycle, including predicted ice clouds mass, opacity, number density, and particle radii. The increased number density and lower nucleation rates bring the simulated cloud opacities closer to observations. Simulations show a weak effect of the excess of small aerosol particles on the simulated water vapor distributions.

In-Situ Imaging of Particles during Rapid Thermite Deflagrations

NASA Astrophysics Data System (ADS)

Grapes, Michael; Sullivan, Kyle; Reeves, Robert; Densmore, John; Willey, Trevor; van Buuren, Tony; Fezaa, Kamel

The dynamic behavior of rapidly deflagrating thermites is a highly complex process involving rapid decomposition, melting, and outgassing of intermediate and/or product gases. Few experimental techniques are capable of probing these phenomena in situ due to the small length and time scales associated with the reaction. Here we use a recently developed extended burn tube test, where we initiate a small pile of thermite on the closed end of a clear acrylic tube. The length of the tube is sufficient to fully contain the reaction as it proceeds and flows entrained particles down the tube. This experiment was brought to the Advanced Photon Source, and the particle formation was X-ray imaged at various positions down the tube. Several formulations, as well as formulation parameters were varied to investigate the size and morphology of the particles, as well as to look for dynamic behavior attributed to the reaction. In all cases, we see evidence of particle coalescence and condensed-phase interfacial reactions. The results improve our understanding of the procession of reactants to products in these systems. Funding provided by the LLNL LDRD program (PLS-16FS-028).

Planetary astronomy

NASA Technical Reports Server (NTRS)

1976-01-01

Color and spectral data from spectrometer observations and computerized analyses of asteroid spectra are discussed. Potential occultations of bright asteroids by the moon are summarized. Analysis of anisotropic scattering within Saturn's rings indicates that mineral contamination of the 120 particles cannot exceed 5 percent by weight, and that the rings formed from particle breakup rather than from particle condensation. Raman probe applications to Jupiter and Uranus atmospheres indicate the presence of aerosol particles. A review of Mariner 9 Mars cloud topography data establishes that most blue clouds are orographic uplift clouds composed of condensates, and that sporadic red clouds are associated with blue clouds or volcanoes and thus probably do not represent dust storm phenomena.

Comparison of aerosol effects on simulated spring and summer hailstorm clouds

NASA Astrophysics Data System (ADS)

Yang, Huiling; Xiao, Hui; Guo, Chunwei; Wen, Guang; Tang, Qi; Sun, Yue

2017-07-01

Numerical simulations are carried out to investigate the effect of cloud condensation nuclei (CCN) concentrations on microphysical processes and precipitation characteristics of hailstorms. Two hailstorm cases are simulated, a spring case and a summer case, in a semiarid region of northern China, with the Regional Atmospheric Modeling System. The results are used to investigate the differences and similarities of the CCN effects between spring and summer hailstorms. The similarities are: (1) The total hydrometeor mixing ratio decreases, while the total ice-phase mixing ratio enhances, with increasing CCN concentration; (2) Enhancement of the CCN concentration results in the production of a greater amount of small-sized hydrometeor particles, but a lessening of large-sized hydrometeor particles; (3) As the CCN concentration increases, the supercooled cloud water and rainwater make a lesser contribution to hail, while the ice-phase hydrometeors take on active roles in the growth of hail; (4) When the CCN concentration increases, the amount of total precipitation lessens, while the role played by liquid-phase rainfall in the amount of total precipitation reduces, relatively, compared to that of ice-phase precipitation. The differences between the two storms include: (1) An increase in the CCN concentration tends to reduce pristine ice mixing ratios in the spring case but enhance them in the summer case; (2) Ice-phase hydrometeor particles contribute more to hail growth in the spring case, while liquid water contributes more in the summer case; (3) An increase in the CCN concentration has different effects on surface hail precipitation in different seasons.

A Condensation-coalescence Cloud Model for Exoplanetary Atmospheres: Formulation and Test Applications to Terrestrial and Jovian Clouds

NASA Astrophysics Data System (ADS)

Ohno, Kazumasa; Okuzumi, Satoshi

2017-02-01

A number of transiting exoplanets have featureless transmission spectra that might suggest the presence of clouds at high altitudes. A realistic cloud model is necessary to understand the atmospheric conditions under which such high-altitude clouds can form. In this study, we present a new cloud model that takes into account the microphysics of both condensation and coalescence. Our model provides the vertical profiles of the size and density of cloud and rain particles in an updraft for a given set of physical parameters, including the updraft velocity and the number density of cloud condensation nuclei (CCNs). We test our model by comparing with observations of trade-wind cumuli on Earth and ammonia ice clouds in Jupiter. For trade-wind cumuli, the model including both condensation and coalescence gives predictions that are consistent with observations, while the model including only condensation overestimates the mass density of cloud droplets by up to an order of magnitude. For Jovian ammonia clouds, the condensation-coalescence model simultaneously reproduces the effective particle radius, cloud optical thickness, and cloud geometric thickness inferred from Voyager observations if the updraft velocity and CCN number density are taken to be consistent with the results of moist convection simulations and Galileo probe measurements, respectively. These results suggest that the coalescence of condensate particles is important not only in terrestrial water clouds but also in Jovian ice clouds. Our model will be useful to understand how the dynamics, compositions, and nucleation processes in exoplanetary atmospheres affect the vertical extent and optical thickness of exoplanetary clouds via cloud microphysics.

Dynamics of inhomogeneous chiral condensates

NASA Astrophysics Data System (ADS)

Carlomagno, Juan Pablo; Krein, Gastão; Kroff, Daniel; Peixoto, Thiago

2018-01-01

We study the dynamics of the formation of inhomogeneous chirally broken phases in the final stages of a heavy-ion collision, with particular interest on the time scales involved in the formation process. The study is conducted within the framework of a Ginzburg-Landau time evolution, driven by a free energy functional motivated by the Nambu-Jona-Lasinio model. Expansion of the medium is modeled by one-dimensional Bjorken flow and its effect on the formation of inhomogeneous condensates is investigated. We also use a free energy functional from a nonlocal Nambu-Jona-Lasinio model which predicts metastable phases that lead to long-lived inhomogeneous condensates before reaching an equilibrium phase with homogeneous condensates.

Anomalous mobility of highly charged particles in pores

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qiu, Yinghua; Yang, Crystal; Hinkle, Preston

2015-07-16

Single micropores in resistive-pulse technique were used to understand a complex dependence of particle mobility on its surface charge density. We show that the mobility of highly charged carboxylated particles decreases with the increase of the solution pH due to an interplay of three effects: (i) ion condensation, (ii) formation of an asymmetric electrical double layer around the particle, and (iii) electroosmotic flow induced by the charges on the pore walls and the particle surfaces. The results are important for applying resistive-pulse technique to determine surface charge density and zeta potential of the particles. As a result, the experiments alsomore » indicate the presence of condensed ions, which contribute to the measured current if a sufficiently high electric field is applied across the pore.« less

Dynamics of Electronically Excited Species in Gaseous and Condensed Phase

DTIC Science & Technology

1989-12-01

heatbath models of condensed phase helium, (3) development of models of condensed phase hydrogen and (4) development of simulation procedures for solution... Modelling and Computer Experiments 93 Introduction 93 Monte Carlo Simulations of Helium Bubble States 94 Heatbath Models f6r Helium Bubble States 114...ILLUSTRATIONS 1 He-He* potential energy curves and couplings for two-state model . 40 2 Cross section for He(1P) quenching to He( 3S) 42 3 Opacity

Comparison of the solid-phase fragment condensation and phase-change approaches in the synthesis of salmon I calcitonin.

PubMed

Gatos, D; Tzavara, C

2001-02-01

Salmon I calcitonin was synthesized using both phase-change and conventional solid-phase fragment condensation (SPFC) approaches, utilizing the Rink amide linker (Fmoc-amido-2,4-dimethoxybenzyl-4-phenoxyacetic acid) combined with 2-chlorotrityl resin and the Fmoc/tBu(Trt)-based protection scheme. Phase-change synthesis, performed by the selective detachment of the fully protected C-terminal 22-mer peptide-linker from the resin and subsequent condensation in solution with the N-terminal 1-10 fragment, gave a product of slightly less purity (85 vs. 92%) than the corresponding synthesis on the solid-phase. In both cases salmon I calcitonin was easily obtained in high purity.

Space shuttle orbiter mechanical refrigeration system

NASA Technical Reports Server (NTRS)

Williams, J. L.

1974-01-01

A radiator/condenser was designed which is efficient in both condensation (refrigeration) and liquid phase (radiator) operating modes, including switchover from the refrigeration mode to the radiator mode and vice versa. A method for predicting the pressure drop of a condensing two-phase flow in zero-gravity was developed along with a method for predicting the flow regime which would prevail along the condensation path. The hybrid refrigeration system was assembled with the two radiator/condenser panels installed in a space environment simulator. The system was tested under both atmospheric and vacuum conditions. Results of the tests are presented.

Development of a Charge-Implicit ReaxFF Potential for Hydrocarbon Systems.

PubMed

Kański, Michał; Maciążek, Dawid; Postawa, Zbigniew; Ashraf, Chowdhury M; van Duin, Adri C T; Garrison, Barbara J

2018-01-18

Molecular dynamics (MD) simulations continue to make important contributions to understanding chemical and physical processes. Concomitant with the growth of MD simulations is the need to have interaction potentials that both represent the chemistry of the system and are computationally efficient. We propose a modification to the ReaxFF potential for carbon and hydrogen that eliminates the time-consuming charge equilibration, eliminates the acknowledged flaws of the electronegativity equalization method, includes an expanded training set for condensed phases, has a repulsive wall for simulations of energetic particle bombardment, and is compatible with the LAMMPS code. This charge-implicit ReaxFF potential is five times faster than the conventional ReaxFF potential for a simulation of keV particle bombardment with a sample size of over 800 000 atoms.

Reactivity of chlorine radical with submicron palmitic acid particles: kinetic measurements and products identification

NASA Astrophysics Data System (ADS)

Mendez, M.; Ciuraru, R.; Gosselin, S.; Batut, S.; Visez, N.; Petitprez, D.

2013-06-01

The heterogeneous reaction of Cl. radicals with sub-micron palmitic acid (PA) particles was studied in an aerosol flow tube in the presence or in the absence of O2. Fine particles were generated by homogeneous condensation of PA vapors and introduced in the reactor where chlorine atoms are produced by photolysis of Cl2 using UV lamps surrounding the reactor. The effective reactive uptake coefficient (γ) has been determined from the rate loss of PA measured by GC/MS analysis of reacted particles as a function of the chlorine exposure. In the absence of O2, γ = 14 ± 5 indicates efficient secondary chemistry involving Cl2. GC/MS analyses have shown the formation of monochlorinated and polychlorinated compounds in the oxidized particles. Although, the PA particles are solid, the complete mass can be consumed. In the presence of oxygen, the reaction is still dominated by secondary chemistry but the propagation chain length is smaller than in the absence of O2 which leads to an uptake coefficient γ = 3 ± 1. In the particulate phase, oxocarboxylic acids and dicarboxylic acids are identified by GC/MS. Formation of alcohols and monocarboxylic acids are also suspected. All these results show that solid organic particles could be efficiently oxidized by gas-phase radicals not only on their surface, but also in bulk by mechanisms which are still unclear. Furthermore the identified reaction products are explained by a chemical mechanism showing the pathway of the formation of more functionalized products. They help to understand the aging of primary tropospheric aerosol containing fatty acids.

Reactivity of chlorine radical with submicron palmitic acid particles: kinetic measurements and product identification

NASA Astrophysics Data System (ADS)

Mendez, M.; Ciuraru, R.; Gosselin, S.; Batut, S.; Visez, N.; Petitprez, D.

2013-12-01

The heterogeneous reaction of Cl• radicals with submicron palmitic acid (PA) particles was studied in an aerosol flow tube in the presence or in the absence of O2. Fine particles were generated by homogeneous condensation of PA vapours and introduced into the reactor, where chlorine atoms were produced by photolysis of Cl2 using UV lamps surrounding the reactor. The effective reactive uptake coefficient (γ) has been determined from the rate loss of PA measured by gas chromatography-mass spectrometer (GC/MS) analysis of reacted particles as a function of the chlorine exposure. In the absence of O2, γ = 14 ± 5 indicates efficient secondary chemistry involving Cl2. GC/MS analysis has shown the formation of monochlorinated and polychlorinated compounds in the oxidized particles. Although the PA particles are solid, the complete mass can be consumed. In the presence of oxygen, the reaction is still dominated by secondary chemistry but the propagation chain length is smaller than in the absence of O2, which leads to an uptake coefficient γ = 3 ± 1. In the particulate phase, oxocarboxylic acids and dicarboxylic acids were identified by GC/MS. The formation of alcohols and monocarboxylic acids is also suspected. A reaction pathway for the main products and more functionalized species is proposed. All these results show that solid organic particles could be efficiently oxidized by gas-phase radicals not only on their surface but also in bulk by mechanisms which are still unclear. They help to understand the aging of primary tropospheric aerosol containing fatty acids.

Sub-micron particle sampler apparatus and method for sampling sub-micron particles

DOEpatents

Gay, D.D.; McMillan, W.G.

1984-04-12

Apparatus and method steps for collecting sub-micron sized particles include a collection chamber and cryogenic cooling. The cooling is accomplished by coil tubing carrying nitrogen in liquid form, with the liquid nitrogen changing to the gas phase before exiting from the collection chamber in the tubing. Standard filters are used to filter out particles of diameter greater than or equal to 0.3 microns; however, the present invention is used to trap particles of less than 0.3 micron in diameter. A blower draws air to said collection chamber through a filter which filters particles with diameters greater than or equal to 0.3 micron. The air is then cryogenically cooled so that moisture and sub-micron sized particles in the air condense into ice on the coil. The coil is then heated so that the ice melts, and the liquid is then drawn off and passed through a Buchner funnel where the liquid is passed through a Nuclepore membrane. A vacuum draws the liquid through the Nuclepore membrane, with the Nuclepore membrane trapping sub-micron sized particles therein. The Nuclepore membrane is then covered on its top and bottom surfaces with sheets of Mylar and the assembly is then crushed into a pellet. This effectively traps the sub-micron sized particles for later analysis. 6 figures.

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

NASA Astrophysics Data System (ADS)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

Mars atmospheric CO2 condensation above the north and south poles as revealed by radio occultation, climate sounder, and laser ranging observations

NASA Astrophysics Data System (ADS)

Hu, Renyu; Cahoy, Kerri; Zuber, Maria T.

2012-07-01

We study the condensation of CO2 in Mars' atmosphere using temperature profiles retrieved from radio occultation measurements from Mars Global Surveyor (MGS) as well as the climate sounding instrument onboard the Mars Reconnaissance Orbiter (MRO), and detection of reflective clouds by the MGS Mars Orbiter Laser Altimeter (MOLA). We find 11 events in 1999 where MGS temperature profiles indicate CO2 condensation and MOLA simultaneously detects reflective clouds. We thus provide causal evidence that MOLA non-ground returns are associated with CO2 condensation, which strongly indicates their nature being CO2 clouds. The MGS and MRO temperature profiles together reveal the seasonal expansion and shrinking of the area and the vertical extent of atmospheric saturation. The occurrence rate of atmospheric saturation is maximized at high latitudes in the middle of winter. The atmospheric saturation in the northern polar region exhibits more intense seasonal variation than in the southern polar region. In particular, a shrinking of saturation area and thickness from LS ˜ 270° to ˜300° in 2007 is found; this is probably related to a planet-encircling dust storm. Furthermore, we integrate the condensation area and the condensation occurrence rate to estimate cumulative masses of CO2 condensates deposited onto the northern and southern seasonal polar caps. The precipitation flux is approximated by the particle settling flux which is estimated using the impulse responses of MOLA filter channels. With our approach, the total atmospheric condensation mass can be estimated from these observational data sets with average particle size as the only free parameter. By comparison with the seasonal polar cap masses inferred from the time-varying gravity of Mars, our estimates indicate that the average condensate particle radius is 8-22 μm in the northern hemisphere and 4-13 μm in the southern hemisphere. Our multi-instrument data analysis provides new constraints on modeling the global climate of Mars.

Dirty bosons in a three-dimensional harmonic trap

NASA Astrophysics Data System (ADS)

Khellil, Tama; Pelster, Axel

2017-09-01

We study a three-dimensional Bose-Einstein condensate in an isotropic harmonic trapping potential with an additional delta-correlated disorder potential and investigate the emergence of a Bose-glass phase for increasing disorder strength. At zero temperature a first-order quantum phase transition from the superfluid phase to the Bose-glass phase is detected at a critical disorder strength, which agrees with the findings in the literature. Afterwards, we study the interplay between temperature and disorder fluctuations on the respective components of the particle density. In particular, we find for smaller disorder strengths that a superfluid region, a Bose-glass region, and a thermal region coexist. Furthermore, depending on the respective system parameters, three phase transitions are detected, namely, one from the superfluid to the Bose-glass phase, another one from the Bose-glass to the thermal phase, and finally one from the superfluid to the thermal phase. All these results are obtained by extending a quite recent Hartree-Fock mean-field theory for the dirty boson problem, which is based on the replica method, from the homogeneous case to a harmonic confinement.

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

NASA Technical Reports Server (NTRS)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Impact of new particle formation on the concentrations of aerosol number and cloud condensation nuclei around Beijing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsui, H.; Koike, Makoto; Kondo, Yutaka

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosol number (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduced a new aerosol model representation with 20 size bins between 1 nm and 10 {mu}m and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the CARE-Beijing 2006 campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurementsmore » (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20-30% of CN concentrations (> 10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of pre-existing particles through the competition of condensable gases between new particles and pre-existing particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.« less

Impact of new particle formation on the concentrations of aerosols and cloud condensation nuclei around Beijing

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Wiedensohler, A.; Fast, J. D.; Zaveri, R. A.

2011-10-01

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosols (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduce a new aerosol model representation with 20 size bins between 1 nm and 10 μm and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the Campaign of Air Quality Research in Beijing and Surrounding Region 2006 (CARE-Beijing 2006) campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurements (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens of nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20%-30% of the CN concentrations (>10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of preexisting particles through the competition of condensable gases between new particles and preexisting particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.

Cluster growth mechanisms in Lennard-Jones fluids: A comparison between molecular dynamics and Brownian dynamics simulations

NASA Astrophysics Data System (ADS)

Jung, Jiyun; Lee, Jumin; Kim, Jun Soo

2015-03-01

We present a simulation study on the mechanisms of a phase separation in dilute fluids of Lennard-Jones (LJ) particles as a model of self-interacting molecules. Molecular dynamics (MD) and Brownian dynamics (BD) simulations of the LJ fluids are employed to model the condensation of a liquid droplet in the vapor phase and the mesoscopic aggregation in the solution phase, respectively. With emphasis on the cluster growth at late times well beyond the nucleation stage, we find that the growth mechanisms can be qualitatively different: cluster diffusion and coalescence in the MD simulations and Ostwald ripening in the BD simulations. We also show that the rates of the cluster growth have distinct scaling behaviors during cluster growth. This work suggests that in the solution phase the random Brownian nature of the solute dynamics may lead to the Ostwald ripening that is qualitatively different from the cluster coalescence in the vapor phase.

interThermalPhaseChangeFoam-A framework for two-phase flow simulations with thermally driven phase change

NASA Astrophysics Data System (ADS)

Nabil, Mahdi; Rattner, Alexander S.

The volume-of-fluid (VOF) approach is a mature technique for simulating two-phase flows. However, VOF simulation of phase-change heat transfer is still in its infancy. Multiple closure formulations have been proposed in the literature, each suited to different applications. While these have enabled significant research advances, few implementations are publicly available, actively maintained, or inter-operable. Here, a VOF solver is presented (interThermalPhaseChangeFoam), which incorporates an extensible framework for phase-change heat transfer modeling, enabling simulation of diverse phenomena in a single environment. The solver employs object oriented OpenFOAM library features, including Run-Time-Type-Identification to enable rapid implementation and run-time selection of phase change and surface tension force models. The solver is packaged with multiple phase change and surface tension closure models, adapted and refined from earlier studies. This code has previously been applied to study wavy film condensation, Taylor flow evaporation, nucleate boiling, and dropwise condensation. Tutorial cases are provided for simulation of horizontal film condensation, smooth and wavy falling film condensation, nucleate boiling, and bubble condensation. Validation and grid sensitivity studies, interfacial transport models, effects of spurious currents from surface tension models, effects of artificial heat transfer due to numerical factors, and parallel scaling performance are described in detail in the Supplemental Material (see Appendix A). By incorporating the framework and demonstration cases into a single environment, users can rapidly apply the solver to study phase-change processes of interest.

Particle Number Concentrations for HI-SCALE Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hering, Susanne V

In support of the Holistic Interactions of Shallow Clouds, Aerosols, and Ecosystems (HI-SCALE) project to study new particle formation in the atmosphere, a pair of custom water condensation particle counters were provided to the second intensive field campaign, from mid-August through mid-September 2017, at the U.S. Department of Energy Southern Great Plains Atmospheric Radiation Measurement (ARM) Climate Research Facility observatory. These custom instruments were developed by Aerosol Dynamics, Inc. (Hering et al. 2017) to detect particles into the nanometer size range. Referred to as “versatile water condensation particle counter (vWCPC)”, they are water-based, laminar-flow condensational growth instruments whose lower particlemore » size threshold can be set based on user-selected operating temperatures. For HI-SCALE, the vWCPCs were configured to measure airborne particle number concentrations in the size range from approximately 2nm to 2μm. Both were installed in the particle sizing system operated by Chongai Kuang of Brookhaven National Laboratory (BNL). One of these was operated in parallel to a TSI Model 3776, upstream of the mobility particle sizing system, to measure total ambient particle concentrations. The airborne particle concentration data from this “total particle number vWCPC” (Ntot-vWCPC) system has been reported to the ARM database. The data are reported with one-second resolution. The second vWCPC was operated in parallel with the BNL diethylene glycol instrument to count particles downstream of a separate differential mobility size analyzer. Data from this “DMA-vWCPC” system was logged by BNL, and will eventually be provided by that laboratory.« less

Tachyon condensation due to domain-wall annihilation in Bose-Einstein condensates.

PubMed

Takeuchi, Hiromitsu; Kasamatsu, Kenichi; Tsubota, Makoto; Nitta, Muneto

2012-12-14

We show theoretically that a domain-wall annihilation in two-component Bose-Einstein condensates causes tachyon condensation accompanied by spontaneous symmetry breaking in a two-dimensional subspace. Three-dimensional vortex formation from domain-wall annihilations is considered a kink formation in subspace. Numerical experiments reveal that the subspatial dynamics obey the dynamic scaling law of phase-ordering kinetics. This model is experimentally feasible and provides insights into how the extra dimensions influence subspatial phase transition in higher-dimensional space.

Cavitation During Superplastic Forming

PubMed Central

Campbell, John

2011-01-01

Cavitation is the opening of pores during superplastic forming, typically at grain boundary triple points or on second phase grain boundary particles during slip of grain boundaries. Theories for the initiation of cavitation are reviewed. It seems that cavitation is unlikely to occur by processes intrinsic to metals such as dislocation mechanisms or point defect condensation. It is proposed that cavitation can only occur at non-bonded interfaces such as those introduced extrinsically (i.e., from the outside) during the original casting of the metal. These defects, known as oxide bifilms, are naturally introduced during pouring of the liquid metal, and are frozen into the solid, often pushed by dendritic growth into grain boundaries where they are difficult to detect because of their extreme thinness, often measured in nanometres. Their unbonded central interface acts as a crack and can initiate cavitation. Second phase precipitates probably do not nucleate and grow on grain boundaries but grow on bifilms in the boundaries, explaining the apparent association between boundaries, second phase particles and failure initiation. Improved melting and casting techniques can provide metal with reduced or zero bifilm population for which cavitation would not be possible, promising significant improvements in superplastic behaviour. PMID:28824142

Cavitation During Superplastic Forming.

PubMed

Campbell, John

2011-07-08

Cavitation is the opening of pores during superplastic forming, typically at grain boundary triple points or on second phase grain boundary particles during slip of grain boundaries. Theories for the initiation of cavitation are reviewed. It seems that cavitation is unlikely to occur by processes intrinsic to metals such as dislocation mechanisms or point defect condensation. It is proposed that cavitation can only occur at non-bonded interfaces such as those introduced extrinsically (i.e., from the outside) during the original casting of the metal. These defects, known as oxide bifilms, are naturally introduced during pouring of the liquid metal, and are frozen into the solid, often pushed by dendritic growth into grain boundaries where they are difficult to detect because of their extreme thinness, often measured in nanometres. Their unbonded central interface acts as a crack and can initiate cavitation. Second phase precipitates probably do not nucleate and grow on grain boundaries but grow on bifilms in the boundaries, explaining the apparent association between boundaries, second phase particles and failure initiation. Improved melting and casting techniques can provide metal with reduced or zero bifilm population for which cavitation would not be possible, promising significant improvements in superplastic behaviour.

Heat transfer in a liquid helium cooled vacuum tube following sudden vacuum loss

NASA Astrophysics Data System (ADS)

Dhuley, R. C.; Van Sciver, S. W.

2015-12-01

Condensation of nitrogen gas rapidly flowing into a liquid helium (LHe) cooled vacuum tube is studied. This study aims to examine the heat transfer in geometries such as the superconducting RF cavity string of a particle accelerator following a sudden loss of vacuum to atmosphere. In a simplified experiment, the flow is generated by quickly venting a large reservoir of nitrogen gas to a straight long vacuum tube immersed in LHe. Normal LHe (LHe I) and superfluid He II are used in separate experiments. The rate of condensation heat transfer is determined from the temperature of the tube measured at several locations along the gas flow. Instantaneous heat deposition rates in excess of 200 kW/m2 result from condensation of the flowing gas. The gas flow is then arrested in its path to pressurize the tube to atmosphere and estimate the heat transfer rate to LHe. A steady LHe I heat load of ≈25 kW/m2 is obtained in this scenario. Observations from the He II experiment are briefly discussed. An upper bound for the LHe I heat load is derived based on the thermodynamics of phase change of nitrogen.

Production of higher quality bio-oils by in-line esterification of pyrolysis vapor

DOEpatents

Hilten, Roger Norris; Das, Keshav; Kastner, James R; Bibens, Brian P

2014-12-02

The disclosure encompasses in-line reactive condensation processes via vapor phase esterification of bio-oil to decease reactive species concentration and water content in the oily phase of a two-phase oil, thereby increasing storage stability and heating value. Esterification of the bio-oil vapor occurs via the vapor phase contact and subsequent reaction of organic acids with ethanol during condensation results in the production of water and esters. The pyrolysis oil product can have an increased ester content and an increased stability when compared to a condensed pyrolysis oil product not treated with an atomized alcohol.

Assessment of the temporal relationship between daily summertime ultra-fine particulate count concentration with PM2.5 and black carbon soot in Washington, DC

DOE Office of Scientific and Technical Information (OSTI.GOV)

Allen, G.; Abt, E.; Koutrakis, P.

Several recent epidemiological studies have shown a significant relationship between ambient daily particulate mass concentrations and human health effects as measured by cardio-pulmonary morbidity and mortality. Much of the current research aimed at determining causal agents of these PM health effects focuses on fine mass (PM2.5), which is primarily the combustion-related component of PM10. Some studies have suggested that ultra-fine aerosols (typically defined as those particles that are less than 0.1 or 0.15 micrometers in diameter) may be an important category of particulate matter to consider, as opposed to or in addition to other measures of fine particle mass. Onemore » of the postulated toxicological mechanisms for ultra-fine particles is that it is the number of particles which is most important, and not necessarily their composition or mass. Some studies suggest that the count concentration could be important by overwhelming macrophages. Another possible particle metric that could be important in health-effect outcomes is particle surface area, which may serve as a condensation surface for gas phase components that are then deposited deep in the lung.« less

Convective heat transfer measurements in a vapour-liquid-liquid three-phase direct contact heat exchanger

NASA Astrophysics Data System (ADS)

Mahood, Hameed B.; Campbell, A. N.; Baqir, Ali Sh.; Sharif, A. O.; Thorpe, R. B.

2018-06-01

Energy usage is increasing around the world due to the continued development of technology, and population growth. Solar energy is a promising low-grade energy resource that can be harvested and utilised in different applications, such solar heater systems, which are used in both domestic and industrial settings. However, the implementation of an efficient energy conversion system or heat exchanger would enhance such low-grade energy processes. The direct contact heat exchanger could be the right choice due to its ability to efficiently transfer significant amounts of heat, simple design, and low cost. In this work, the heat transfer associated with the direct contact condensation of pentane vapour bubbles in a three-phase direct contact condenser is investigated experimentally. Such a condenser could be used in a cycle with a solar water heater and heat recovery systems. The experiments on the steady state operation of the three-phase direct contact condenser were carried out using a short Perspex tube of 70 cm in total height and an internal diameter of 4 cm. Only a height of 48 cm was active as the direct contact condenser. Pentane vapour, (the dispersed phase) with three different initial temperatures (40° C, 43.5° C and 47.5° C) was directly contacted with water (the continuous phase) at 19° C. The experimental results showed that the total heat transfer rate per unit volume along the direct contact condenser gradually decreased upon moving higher up the condenser. Additionally, the heat transfer rate increases with increasing mass flow rate ratio, but no significant effect on the heat transfer rate of varying the initial temperature of the dispersed phase was seen. Furthermore, both the outlet temperature of the continuous phase and the void fraction were positively correlated with the total heat transfer rate per unit volume, with no considerable effect of the initial temperature difference between the dispersed and continuous phases.

Convective heat transfer measurements in a vapour-liquid-liquid three-phase direct contact heat exchanger

NASA Astrophysics Data System (ADS)

Mahood, Hameed B.; Campbell, A. N.; Baqir, Ali Sh.; Sharif, A. O.; Thorpe, R. B.

2017-12-01

Energy usage is increasing around the world due to the continued development of technology, and population growth. Solar energy is a promising low-grade energy resource that can be harvested and utilised in different applications, such solar heater systems, which are used in both domestic and industrial settings. However, the implementation of an efficient energy conversion system or heat exchanger would enhance such low-grade energy processes. The direct contact heat exchanger could be the right choice due to its ability to efficiently transfer significant amounts of heat, simple design, and low cost. In this work, the heat transfer associated with the direct contact condensation of pentane vapour bubbles in a three-phase direct contact condenser is investigated experimentally. Such a condenser could be used in a cycle with a solar water heater and heat recovery systems. The experiments on the steady state operation of the three-phase direct contact condenser were carried out using a short Perspex tube of 70 cm in total height and an internal diameter of 4 cm. Only a height of 48 cm was active as the direct contact condenser. Pentane vapour, (the dispersed phase) with three different initial temperatures (40° C, 43.5° C and 47.5° C) was directly contacted with water (the continuous phase) at 19° C. The experimental results showed that the total heat transfer rate per unit volume along the direct contact condenser gradually decreased upon moving higher up the condenser. Additionally, the heat transfer rate increases with increasing mass flow rate ratio, but no significant effect on the heat transfer rate of varying the initial temperature of the dispersed phase was seen. Furthermore, both the outlet temperature of the continuous phase and the void fraction were positively correlated with the total heat transfer rate per unit volume, with no considerable effect of the initial temperature difference between the dispersed and continuous phases.

Interaction of evaporating and condensing particles in the free-molecular regime

NASA Astrophysics Data System (ADS)

Kogan, M. N.; Bobrov, I. N.; Cercignani, C.; Frezzotti, A.

1995-07-01

In a previous paper it was shown that repulsive/attractive forces arise between evaporating/ condensing particles in the free-molecular regime. Here we obtain explicit expressions for these forces in the case of spherical particles with equal temperatures. The temperature of the surrounding vapor is, generally speaking, different from that of the particles. Numerical results are obtained for different values of the ratios between particle and vapor temperatures and pressures, of the particles radii and of the evaporation coefficients. In the case when the evaporation coefficient equals unity, an exact expression is obtained for the force between particles of different radii. A simple model describing coagulation processes and taking the above-mentioned forces into account is proposed. It is shown that for large values of the vapor supersaturation, the influence of these forces on the coagulation rate may be very pronounced.

Structure of dental gallium alloys.

PubMed

Herø, H; Simensen, C J; Jørgensen, R B

1996-07-01

The interest in gallium alloys as a replacement for amalgam has increased in recent years due to the risk of environmental pollution from amalgam. Alloy powders with compositions close to those for alloys of amalgam are mixed with a liquid gallium alloy. The mix is condensed into a prepared cavity in much the same way as for amalgam. The aim of the present work was to study the structure of: (1) two commercial alloy powders containing mainly silver, tin and copper, and (2) the phases formed by mixing these powders with a liquid alloy of gallium, indium and tin. One of the alloy powders contained 9 wt% palladium. Cross-sections of cylindrical specimens made by these gallium mixes were investigated by scanning electron microscopy, energy dispersive spectroscopy and X-ray diffraction. Discrete grains of the following phases were found to be present in both gallium alloys: hexagonal Ag2Ga, tetragonal Cu(Pd)Ga2, cubic Ag9In4 and tetragonal beta-Sn. Indications of hexagonal or orthorhombic Ag2Sn were found in the remaining, unreacted alloy particles. In the palladium-containing alloy the X-ray reflections indicate a minor fraction of cubic Cu9Ga4 in addition to the Cu(Pd)Ga2 phase. Particles of beta-Sn are probably precipitated because Sn-Ga phases cannot be formed according to the binary phase diagram.

Sub-micron particle sampler apparatus

DOEpatents

Gay, Don D.; McMillan, William G.

1987-01-01

Apparatus and method steps for collecting sub-micron sized particles include a collection chamber and cryogenic cooling. The cooling is accomplished by coil tubing carrying nitrogen in liquid form, with the liquid nitrogen changing to the gas phase before exiting from the collection chamber in the tubing. Standard filters are used to filter out particles of diameter greater than or equal to 0.3 microns; however the present invention is used to trap particles of less than 0.3 micron in diameter. A blower draws air to said collection chamber through a filter which filters particles with diameters greater than or equal to 0.3 micron. The air is then cryogenically cooled so that moisture and sub-micron sized particles in the air condense into ice on the coil. The coil is then heated so that the ice melts, and the liquid is then drawn off and passed through a Buchner funnel where the liquid is passed through a Nuclepore membrane. A vacuum draws the liquid through the Nuclepore membrane, with the Nuclepore membrane trapping sub-micron sized particles therein. The Nuclepore membrane is then covered on its top and bottom surfaces with sheets of Mylar.RTM. and the assembly is then crushed into a pellet. This effectively traps the sub-micron sized particles for later analysis.

Method for sampling sub-micron particles

DOEpatents

Gay, Don D.; McMillan, William G.

1985-01-01

Apparatus and method steps for collecting sub-micron sized particles include a collection chamber and cryogenic cooling. The cooling is accomplished by coil tubing carrying nitrogen in liquid form, with the liquid nitrogen changing to the gas phase before exiting from the collection chamber in the tubing. Standard filters are used to filter out particles of diameter greater than or equal to 0.3 microns; however the present invention is used to trap particles of less than 0.3 micron in diameter. A blower draws air to said collection chamber through a filter which filters particles with diameters greater than or equal to 0.3 micron. The air is then cryogenically cooled so that moisture and sub-micron sized particles in the air condense into ice on the coil. The coil is then heated so that the ice melts, and the liquid is then drawn off and passed through a Buchner funnel where the liquid is passed through a Nuclepore membrane. A vacuum draws the liquid through the Nuclepore membrane, with the Nuclepore membrane trapping sub-micron sized particles therein. The Nuclepore membrane is then covered on its top and bottom surfaces with sheets of Mylar.RTM. and the assembly is then crushed into a pellet. This effectively traps the sub-micron sized particles for later analysis.

Acid-catalyzed condensed-phase reactions of limonene and terpineol and their impacts on gas-to-particle partitioning in the formation of organic aerosols.

PubMed

Li, Yong Jie; Cheong, Gema Y L; Lau, Arthur P S; Chan, Chak K

2010-07-15

We investigated the condensed-phase reactions of biogenic VOCs with C double bond C bonds (limonene, C(10)H(16), and terpineol, C(10)H(18)O) catalyzed by sulfuric acid by both bulk solution (BS) experiments and gas-particle (GP) experiments using a flow cell reactor. Product analysis by gas chromatography-mass spectrometry (GC-MS) showed that cationic polymerization led to dimeric and trimeric product formation under conditions of relative humidity (RH) <20% (in the GP experiments) and a sulfuric acid concentration of 57.8 wt % (in the BS experiments), while hydration occurred under conditions of RH > 20% (in the GP experiments) and sulfuric acid concentrations of 46.3 wt % or lower (in the BS experiments). Apparent partitioning coefficients (K(p,rxn)) were estimated from the GP experiments by including the reaction products. Only under extremely low RH conditions (RH < 5%) did the values of K(p,rxn) ( approximately 5 x 10(-6) m(3)/microg for limonene and approximately 2 x 10(-5) m(3)/microg for terpineol) substantially exceed the physical partitioning coefficients (K(p) = 6.5 x 10(-8) m(3)/microg for limonene and =2.3 x 10(-6) m(3)/microg for terpineol) derived from the absorptive partitioning theory. At RH higher than 5%, the apparent partitioning coefficients (K(p,rxn)) of both limonene and terpineol were in the same order of magnitude as the K(p) values derived from the absorptive partitioning theory. Compared with other conditions including VOC concentration and degree of neutralization (by ammonium) of acidic particles, RH is a critical parameter that influences both the reaction mechanisms and the uptake ability (K(p,rxn) values) of these processes. The finding suggests that RH needs to be considered when taking the effects of acid-catalyzed reactions into account in estimating organic aerosol formation from C double bond C containing VOCs.

NMOC, ozone, and organic aerosol in the southeastern United States, 1999-2007: 3. Origins of organic aerosol in Atlanta, Georgia, and surrounding areas

NASA Astrophysics Data System (ADS)

Blanchard, C. L.; Hidy, G. M.; Tanenbaum, S.; Edgerton, E. S.

2011-02-01

Carbonaceous compounds constitute a major fraction of the fine particle mass at locations throughout North America; much of the condensed-phase organic carbon (OC) is produced in the atmosphere from NMOC reactions as "secondary" OC (SOC). Ten years of particulate carbon and speciated non-methane organic compound (NMOC) data combined with other measurements from Southeastern Aerosol Research and Characterization (SEARCH) and other sites provide insight into the association between elemental carbon (EC), OC and NMOCs. Data are analyzed to characterize the OC and SOC contrasts between urban Atlanta, Georgia, and nearby non-urban conditions in the Southeast. Analysis of the monitoring record indicates that the mean Atlanta urban excess of total carbon (TC) is 2.1-2.8 μg m -3. The OC/EC ratio of the Atlanta urban excess is in the range 1.3 to 1.8, consistent with OC/EC ratios observed in motor vehicle emissions and a fossil carbon source of urban excess TC. Carbon isotope analysis of a subset of particle samples demonstrates that the urban excess is mainly fossil in origin, even though the majority of the TC is modern at both urban and non-urban sites. Temperature-dependent partitioning of OC between gas and condensed phases cannot explain the observed diurnal and seasonal variations of OC/CO, EC/CO, and OC/EC ratios. Alternatively, a hypothesis involving vertical mixing of OC-enriched air from aloft is supported by the seasonal and diurnal OC, isopentane, aromatic and isoprene observations at the ground. A statistical model is applied to indicate the relative significance of aerometric factors affecting OC and EC concentrations, including meteorological and pollutant associations. The model results demonstrate strong linkages between fine particle carbon and pollutant indicators of source emissions compared with meteorological factors; the model results show weaker dependence of OC on meteorological factors than is the case for ozone (O 3) concentrations.

Ionic Liquid Fuels for Chemical Propulsion

DTIC Science & Technology

2016-10-31

nucleophilicity in the ionic liquid is critical. Both gas -phase and condensed-phase (CPCM-GIL) density functional theory calculations support the...stability trends in dialkylimidazolium ionic liquids and could be used as a higher accuracy method than the gas -phase DFT approach for predicting thermal...stabilities of ionic liquids in general. One important finding from the comparison of the gas -phase basicities relative to the GIL condensed- phase

The Origin of Inertia and Matter as a Superradiant Phase Transition of Quantum Vacuum

NASA Astrophysics Data System (ADS)

Maxmilian Caligiuri, Luigi

Mass is one of the most important concepts in physics and its real understanding represents the key for the formulation of any consistent physical theory. During the past years, a very interesting model of inertial and gravitational mass as the result of the reaction interaction between the charged particles (electrons and quarks) contained in a given body and a suitable "fraction" of QED Zero Point Fields confined within an ideal resonant cavity, associated to the same body, has been proposed by Haish, Rueda and Puthoff. More recently, the author showed that this interpretation is consistent with a picture of mass (both inertial and gravitational) as the seat of ZPF standing waves whose presence reduces quantum vacuum energy density inside the resonant cavity ideally associated to the body volume. Nevertheless so far, the ultimate physical origin of such resonant cavity as well as the mechanism able to "select" the fraction of ZPF electromagnetic modes interacting within it, remained unrevealed. In this paper, basing on the framework of QED coherence in condensed matter, we'll show mass can be viewed as the result of a spontaneous superradiant phase transition of quantum vacuum giving rise to a more stable, energetically favored, oscopic quantum state characterized by an ensemble of coherence domains, "trapping" the coherent ZPF fluctuations inside a given volume just acting as a resonant cavity. Our model is then able to explain the "natural" emergence of the ideal resonant cavity speculated by Haish, Rueda and Puthoff and its defining parameters as well as the physical mechanism selecting the fraction of ZPF interacting with the body particles. Finally, a generalization of the model to explain the origin of mass of elementary particles is proposed also suggesting a new understanding of Compton's frequency and De Broglie's wavelength. Our results indicates both inertia and matter could truly originate from coherent interaction between quantum matter-wave and radiation fields condensed from quantum vacuum and also give novel and interesting insights into fundamental physical questions as, for example, the structure of elementary particles and matter stability.

Characterization of Reaerosolization From Impingers in an Effort to Improve Airborne Virus Sampling

DTIC Science & Technology

2009-04-01

Koutrakis, P. (1996) Inertial separation of ultrafine particles using a condensational growth/ virtual impaction system. Aerosol Sci. Tech. 25, 424–436...Environ. 42, 828–832. Demokritou, P., Gupta, T., and and Koutrakis, P. (2002) A high volume apparatus for the condensational growth of ultrafine ... particles for inhalation toxicological studies. Aerosol Sci. Tech. 36, 1061–1072. Floyd, R., and Sharp, D. G. (1978) Viral aggregation: Effects of salts

Alpha particle condensation in {sup 12}C and nuclear rainbow scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohkubo, S.; Hirabayashi, Y.

2008-05-12

It is shown that the large radius of the Hoyle state of {sup 12}C with a dilute density distribution in an {alpha} particle condensate can be clearly seen in the shift of the rainbow angle (therefore the Airy minimum) to a larger angle in {alpha}+{sup 12}C rainbow scattering at the high energy region and prerainbow oscillations in {sup 3}He+{sup 12}C scattering at the lower energy region.

Microcanonical fluctuations of the condensate in weakly interacting Bose gases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Idziaszek, Zbigniew

2005-05-15

We study fluctuations of the number of Bose condensed atoms in a weakly interacting homogeneous and trapped gases. For a homogeneous system we apply the particle-number-conserving formulation of the Bogoliubov theory and calculate the condensate fluctuations within the canonical and the microcanonical ensembles. We demonstrate that, at least in the low-temperature regime, predictions of the particle-number-conserving and traditional, nonconserving theory are identical, and lead to the anomalous scaling of fluctuations. Furthermore, the microcanonical fluctuations differ from the canonical ones by a quantity which scales normally in the number of particles, thus predictions of both ensembles are equivalent in the thermodynamicmore » limit. We observe a similar behavior for a weakly interacting gas in a harmonic trap. This is in contrast to the trapped, ideal gas, where microcanonical and canonical fluctuations are different in the thermodynamic limit.« less

The N-terminus of histone H2B, but not that of histone H3 or its phosphorylation, is essential for chromosome condensation

PubMed Central

de la Barre, Anne-Elisabeth; Angelov, Dimitri; Molla, Annie; Dimitrov, Stefan

2001-01-01

We have studied the role of individual histone N-termini and the phosphorylation of histone H3 in chromosome condensation. Nucleosomes, reconstituted with histone octamers containing different combinations of recombinant full-length and tailless histones, were used as competitors for chromosome assembly in Xenopus egg extracts. Nucleosomes reconstituted with intact octamers inhibited chromosome condensation as efficiently as the native ones, while tailless nucleosomes were unable to affect this process. Importantly, the addition to the extract of particles containing only intact histone H2B strongly interfered with chromosome formation while such an effect was not observed with particles lacking the N-terminal tail of H2B. This demonstrates that the inhibition effect observed in the presence of competitor nucleosomes is mainly due to the N-terminus of this histone, which, therefore, is essential for chromosome condensation. Nucleosomes in which all histones but H3 were tailless did not impede chromosome formation. In addition, when competitor nucleosome particles were reconstituted with full-length H2A, H2B and H4 and histone H3 mutated at the phosphorylable serine 10 or serine 28, their inhibiting efficiency was identical to that of the native particles. Hence, the tail of H3, whether intact or phosphorylated, is not important for chromosome condensation. A novel hypothesis, termed ‘the ready production label’ was suggested to explain the role of histone H3 phosphorylation during cell division. PMID:11707409

Hidden multiparticle excitation in a weakly interacting Bose-Einstein condensate

NASA Astrophysics Data System (ADS)

Watabe, Shohei

2018-03-01

We investigate multiparticle excitation effect on a collective density excitation as well as a single-particle excitation in a weakly interacting Bose-Einstein condensate (BEC). We find that although the weakly interacting BEC offers weak multiparticle excitation spectrum at low temperatures, this multiparticle excitation effect may not remain hidden, but emerges as bimodality in the density response function through the single-particle excitation. Identification of spectra in the BEC between the single-particle excitation and the density excitation is also assessed at nonzero temperatures, which has been known to be unique nature in the BEC at absolute zero temperature.

Competition for water vapour results in suppression of ice formation in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Simpson, Emma L.; Connolly, Paul J.; McFiggans, Gordon

2018-05-01

The formation of ice in clouds can initiate precipitation and influence a cloud's reflectivity and lifetime, affecting climate to a highly uncertain degree. Nucleation of ice at elevated temperatures requires an ice nucleating particle (INP), which results in so-called heterogeneous freezing. Previously reported measurements for the ability of a particle to nucleate ice have been made in the absence of other aerosol which will act as cloud condensation nuclei (CCN) and are ubiquitous in the atmosphere. Here we show that CCN can outcompete INPs for available water vapour thus suppressing ice formation, which has the potential to significantly affect the Earth's radiation budget. The magnitude of this suppression is shown to be dependent on the mass of condensed water required for freezing. Here we show that ice formation in a state-of-the-art cloud parcel model is strongly dependent on the criteria for heterogeneous freezing selected from those previously hypothesised. We have developed an alternative criteria which agrees well with observations from cloud chamber experiments. This study demonstrates the dominant role that competition for water vapour can play in ice formation, highlighting both a need for clarity in the requirements for heterogeneous freezing and for measurements under atmospherically appropriate conditions.

A hybrid formulation for the numerical simulation of condensed phase explosives

NASA Astrophysics Data System (ADS)

Michael, L.; Nikiforakis, N.

2016-07-01

In this article we present a new formulation and an associated numerical algorithm, for the simulation of combustion and transition to detonation of condensed-phase commercial- and military-grade explosives, which are confined by (or in general interacting with one or more) compliant inert materials. Examples include confined rate-stick problems and interaction of shock waves with gas cavities or solid particles in explosives. This formulation is based on an augmented Euler approach to account for the mixture of the explosive and its products, and a multi-phase diffuse interface approach to solve for the immiscible interaction between the mixture and the inert materials, so it is in essence a hybrid (augmented Euler and multi-phase) model. As such, it has many of the desirable features of the two approaches and, critically for our applications of interest, it provides the accurate recovery of temperature fields across all components. Moreover, it conveys a lot more physical information than augmented Euler, without the complexity of full multi-phase Baer-Nunziato-type models or the lack of robustness of augmented Euler models in the presence of more than two components. The model can sustain large density differences across material interfaces without the presence of spurious oscillations in velocity and pressure, and it can accommodate realistic equations of state and arbitrary (pressure- or temperature-based) reaction-rate laws. Under certain conditions, we show that the formulation reduces to well-known augmented Euler or multi-phase models, which have been extensively validated and used in practice. The full hybrid model and its reduced forms are validated against problems with exact (or independently-verified numerical) solutions and evaluated for robustness for rate-stick and shock-induced cavity collapse case-studies.

Characterization of Organic Nitrate Formation in Limonene Secondary Organic Aerosol using High-Resolution Chemical Ionization Mass Spectrometry

NASA Astrophysics Data System (ADS)

Faxon, Cameron; Hammes, Julia; Peng, Jianfei; Hallquist, Mattias; Pathak, Ravi

2016-04-01

Previous work has shown that organic nitrates (RONO2) are prevalent in the boundary layer, and can contribute significantly to secondary organic aerosol formation. Monoterpenes, including limonene, have been shown to be precursors for the formation of these organic nitrates. Limonene has two double bonds, either of which may be oxidized by NO3 or O3. This leads to the generation of products that can subsequently condense or partition into the particle phase, producing secondary organic aerosol. In order to further elucidate the particle and gas phase product distribution of organic nitrates forming from the reactions of limonene and the nitrate radical (NO3), a series of experiments were performed in the Gothenburg Flow Reactor for Oxidation Studies at Low Temperatures (G-FROST), described by previous work. N2O5 was used as the source for NO3 and NO2, and a characterized diffusion source was used to introduce limonene into the flow reactor. All experiments were conducted in the absence of light, and the concentration of limonene was increased step-wise throughout each experiment to modify the ratio of N2O5to limonene. The experiments were conducted such that both limonene- and N2O5-limited regimes were present. Gas and particle phase products were measured using an iodide High-Resolution Time-of-Flight Mass Spectrometer (HR-ToF-CIMS) coupled to a Filter Inlet for Gases and AEROsols (FIGAERO, and particle size and SOA mass concentrations were derived using a Scanning Mobility Particle Sizer (SMPS). CIMS measurement techniques have previously been employed for the measurement of organic nitrate products of such compounds using multiple reagent ions. The use of this instrumentation allowed for the identification of chemical formulas for gas and particle phase species. The findings from the experiments will be presented in terms of the relative gas-particle partitioning of major products and the effects of N2O5/limonene ratios on product distributions. Additionally, a comparison of the distribution of the most prevalent reaction products relative to the expected distribution derived using chemical kinetics simulations based on the Master Chemical Mechanism (MCM) limonene mechanism will be discussed.

Measurements of Gas and Particle Phase Emissions From Munitions Detonation in a Field Environment

NASA Astrophysics Data System (ADS)

Fortner, E. C.; Knighton, W. B.; Timko, M.; Wood, E.; Onasch, T. B.; Kolb, C. E.; Beardsley, H. M.

2007-12-01

During the Point of Fire (POF) field campaign conducted at Fort Sill Oklahoma U.S.A. in March 2007 a suite of real- time trace gas and fine (submicron) particulate matter (PM) instrumentation characterized the point of fire emission plumes from large, medium and small caliber weapons systems. Muzzle emission plumes were measured and where appropriate, breach plumes and gun crew breathing zone measurements were also conducted. Aerosol measurements were conducted with an aerosol mass spectrometer (Aerodyne CTOF-AMS) for particle composition, condensation particle counter (CPC) for particle number density and DUSTRAK aerosol monitor for particle mass. Gas phase measurements included CO, CO2, NOx and a variety of trace gas species measured by proton transfer reaction mass spectrometry (PTR-MS) including hydrogen cyanide (HCN), acetonitrile, acrylonitrile, benzene, toluene, benzonitrile and styrene. In the majority of the plume measurements, HCN was the most prominent compound measured by PTR-MS. Quantification of HCN by PTR-MS is difficult due to its proton affinity being close enough to that of water to allow a significant backward reaction of protonated HCN with water, reducing the detection sensitivity and making the response dependent on humidity. We have developed a quantification procedure for HCN based on laboratory measurements of a calibration gas standard of HCN, which allows the humidity dependence to be extracted directly from the proton hydrate ion intensities. The correction factors for HCN are quite significant varying between 10 and 30 depending on sample humidity.

Field and Laboratory Studies of Atmospheric Organic Aerosol

NASA Astrophysics Data System (ADS)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of these conditions to all measurements conducted during E-PEACE demonstrated that a large fraction of cloud droplet (72%) and dry aerosol mass (12%) sampled in the California coastal study region was heavily or moderately influenced by ship emissions. Another study investigated the chemical and physical evolution of a controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed of oxidized organic compounds contributed nearly an order of magnitude more cloud condensation nuclei (CCN) than less oxidized particles formed under cloudy conditions. The processing time necessary for particles to become CCN active was short ( 4 hr). Laboratory chamber experiments were also conducted to evaluate particle-phase processes influencing aerosol phase and composition. In one study, ammonium sulfate seed was coated with a layer of secondary organic aerosol (SOA) from toluene oxidation followed by a layer of SOA from α-pinene oxidation. The system exhibited different evaporative properties than ammonium sulfate seed initially coated with α-pinene SOA followed by a layer of toluene SOA. This behavior is consistent with a shell-and-core model and suggests limited mixing among different SOA types. Another study investigated the reactive uptake of isoprene epoxy diols (IEPOX) onto non-acidified aerosol. It was demonstrated that particle acidity has limited influence on organic aerosol formation onto ammonium sulfate seed, and that the chemical system is limited by the availability of nucleophiles such as sulfate. Flow tube experiments were conducted to examine the role of iron in the reactive uptake and chemical oxidation of glycolaldehyde. Aerosol particles doped with iron and hydrogen peroxide were mixed with gas-phase glycolaldehyde and photochemically aged in a custom-built flow reactor. Compared to particles free of iron, iron-doped aerosols significantly enhanced the oxygen to carbon (O/C) ratio of accumulated organic mass. The primary oxidation mechanism is suggested to be a combination of Fenton and photo-Fenton reactions which enhance particle-phase OH radical concentrations.

Thermally induced phase transformation in multi-phase iron oxide nanoparticles on vacuum annealing

NASA Astrophysics Data System (ADS)

Anupama, A. V.; Keune, W.; Sahoo, B.

2017-10-01

The evolution of magnetic phases in multi-phase iron oxide nanoparticles, synthesized via the transferred arc plasma induced gas phase condensation method, was investigated by X-ray diffraction, vibrating sample magnetometry and 57Fe Mössbauer spectroscopy. The particles are proposed to be consisting of three different iron oxide phases: α-Fe2O3, γ-Fe2O3 and Fe3O4. These nanoparticles were exposed to high temperature (∼935 K) under vacuum (10-3 mbar He pressure), and the thermally induced phase transformations were investigated. The Rietveld refinement of the X-ray diffraction data corroborates the least-squares fitting of the transmission Mössbauer spectra in confirming the presence of Fe3O4, γ-Fe2O3 and α-Fe2O3 phases before the thermal treatment, while only Fe3O4 and α-Fe2O3 phases exist after thermal treatment. On thermal annealing in vacuum, conversion from γ-Fe2O3 to Fe3O4 and α-Fe2O3 was observed. Interestingly, we have observed a phase transformation occurring in the temperature range ∼498 K-538 K, which is strikingly lower than the phase transformation temperature of γ-Fe2O3 to α-Fe2O3 (573-623 K) in air. Combining the results of Rietveld refinement of X-ray diffraction patterns and Mössbauer spectroscopy, we have attributed this phase transformation to the phase conversion of a metastable "defected and strained" d-Fe3O4 phase, present in the as-prepared sample, to the α-Fe2O3 phase. Stabilization of the phases by controlling the phase transformations during the use of different iron-oxide nanoparticles is the key factor to select them for a particular application. Our investigation provides insight into the effect of temperature and chemical nature of the environment, which are the primary factors governing the phase stability, suitability and longevity of the iron oxide nanomaterials prepared by the gas-phase condensation method for various applications.

Deep Metastable Eutectic Nanometer-Scale Particles in the MgO-Al2O3-SiO2 System

NASA Technical Reports Server (NTRS)

Reitmeijer, Frans J. M.; Nash, J. A., III

2011-01-01

Laboratory vapor phase condensation experiments systematically yield amorphous, homogeneous, nanoparticles with unique deep metastable eutectic compositions. They formed during the nucleation stage in rapidly cooling vapor systems. These nanoparticles evidence the complexity of the nucleation stage. Similar complex behavior may occur during the nucleation stage in quenched-melt laboratory experiments. Because of the bulk size of the quenched system many of such deep metastable eutectic nanodomains will anneal and adjust to local equilibrium but some will persist metastably depending on the time-temperature regime and melt/glass transformation.

Recent Progress in the Study of Topological Semimetals

NASA Astrophysics Data System (ADS)

Bernevig, Andrei; Weng, Hongming; Fang, Zhong; Dai, Xi

2018-04-01

The topological semimetal is a new, theoretically predicted and experimentally discovered, topological state of matter. In one of its several realizations, the topological semimetal hosts Weyl fermions, elusive particles predicted more than 85 years ago, sought after in high-energy experiments, but only recently found in a condensed-matter setting. In the present review, we catalogue the most recent progress in this fast-developing research field. We give special attention to topological invariants and the material realization of three different types of topological semimetal. We also discuss various photo emission, transport and optical experimental observables that characterize the appearance of topological semimetal phases.

Emissions of Volatile Particulate Components from Turboshaft Engines running JP-8 and Fischer-Tropsch Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng, Mengdawn; Corporan, E.; DeWitt, M.

2009-01-01

Rotating-wing aircraft or helicopters are heavily used by the US military and also a wide range of commercial applications around the world, but emissions data for this class of engines are limited. In this study, we focus on emissions from T700-GE-700 and T700-GE-701C engines; T700 engine was run with military JP-8 and T701C run with both JP-8 and Fischer-Tropsch (FT) fuels. Each engine was run at three engine power settings from the idle to maximum power in sequence. Exhaust particles measured at the engine exhaust plane (EEP) have a peak mobility diameter less than 50nm in all engine power settings.more » At a 4-m downstream location, sulfate/sulfur measurements indicate all particulate sulfur exists practically as sulfate, and the particulate sulfur and sulfate contents increased as the engine power increased. The conversion of sulfur to sulfate was found not to be dependent on engine power setting. Analysis also showed that conversion of sulfur to sulfate was not by the adsorption of sulfur dioxide gas on the soot particles and then subsequently oxidized to form sulfate, but by gas-phase conversion of SO2 via OH or O then subsequently forming H2SO4 and condensing on soot particles. Without the sulfur and aromatic components, use of the FT fuel led to significant reduction of soot emissions as compared to that of the JP-8 fuel producing less number of particles than that of the JP-8 fuel; however, the FT fuel produced much higher number concentrations of particles smaller than 7nm than that of JP-8 in all engine power settings. This indicates non-aromatics components in the FT fuel could have contributed to the enhancement of emissions of particles smaller than 7nm. These small particles are volatile, not observed at the EEP, and may be important in playing a role for the formation of secondary particles in the atmosphere or serving as a site for effective cloud nuclei condensation to occur.« less

BOOK REVIEW: Soft Condensed Matter

NASA Astrophysics Data System (ADS)

Jones, Richard A. L.

2002-11-01

The author states in the preface of the book that the aim is '...to give a unified overview of the various aspects of the physics of soft condensed matter'. The book succeeds in fulfilling this aim in many respects. i) The style is fluent and concise and gives the necessary explanations to make its content understandable to people with some knowledge of the basic principles of physics. ii) The content of the book is complete enough to give a panoramic view of the landscape of soft condensed matter. The first two chapters give, respectively, a short introduction and a presentation of forces, energies and timescales, giving a general overview and pointing out the particular importance of different aspects such as timescales, which are much more important in soft condensed matter than in traditional or 'hard' condensed matter. The next chapter, devoted to phase transition, recalls that the equilibrium between two phases is controlled by free energy considerations. Spinodal decomposition is presented as a counterpart of nucleation and growth. Again, characteristic length scales are considered and applied to a phase separation mixture of polymers in a common solvent. The following three chapters are devoted respectively to specific topics: colloidal dispersion, polymers and gelation. The stability and phase behaviour of colloids are related to the interaction between colloidal particles. Properties of colloidal crystals as well as colloidal dispersion are depicted in terms of stabilization of crystalline colloids. The flow properties of colloidal dispersion are presented in terms of free energy minimization and the structure of the dispersion. After a brief introduction to polymer chemistry and architecture, the coil-globule transition is discussed. Viscoelasticity of polymers is described and discussed by introducing the notion of entanglement. This leads to the introduction of the tube model and the theory of reptation. The sol-gel transition is presented phenomenologically and formulated through the current percolation model and the Flory-Stockmayer model. The next two chapters consider the molecular order in soft condensed matter. The rich complexity of liquid crystals is emphasized and the Frederiks transition is described in relation to liquid crystal displays. The crystallinity in polymers is discussed and its usual semi-crystallinity presented as a consequence of entanglement and timescales. The next chapter describes the self-assembly of phases and the great importance of the self-assembly phenomenon in solutions of amphiphilic molecules is largely discussed in several specific phenomena. The book ends with a chapter devoted to the description of soft matter realizations in nature. Special attention is paid to the components and structure of life: nucleic acids, proteins, polysaccharides and membranes. There are two appendixes recalling the basic concepts of thermodynamics and statistical mechanics. In each chapter, several problems are included, and solutions to a selection of them are given. The bibliography proposed is pertinent and each chapter gives details of further reading, mostly addressed to known books on the topic. iii) The presentation of the book is good. Throughout the book, the relevant, basic or new concepts of each topic are typed in bold characters and succinctly defined. The figures are abundant and adequately illustrate the text either by plots of experimental data or by computed predictions from models. Many schematic representations of structures, molecular distributions or arrangements are also included. In summary, the author has succeeded in producing a scientifically rigorous book of affordable size (around 200 pages) that is well illustrated (about 120 figures) and written in a fluent style that describes the many different physical phenomena involved in soft condensed matter. N Clavaguera

Condensate statistics and thermodynamics of weakly interacting Bose gas: Recursion relation approach

NASA Astrophysics Data System (ADS)

Dorfman, K. E.; Kim, M.; Svidzinsky, A. A.

2011-03-01

We study condensate statistics and thermodynamics of weakly interacting Bose gas with a fixed total number N of particles in a cubic box. We find the exact recursion relation for the canonical ensemble partition function. Using this relation, we calculate the distribution function of condensate particles for N=200. We also calculate the distribution function based on multinomial expansion of the characteristic function. Similar to the ideal gas, both approaches give exact statistical moments for all temperatures in the framework of Bogoliubov model. We compare them with the results of unconstraint canonical ensemble quasiparticle formalism and the hybrid master equation approach. The present recursion relation can be used for any external potential and boundary conditions. We investigate the temperature dependence of the first few statistical moments of condensate fluctuations as well as thermodynamic potentials and heat capacity analytically and numerically in the whole temperature range.

Freeze-Tolerant Condensers

NASA Technical Reports Server (NTRS)

Crowley, Christopher J.; Elkouhk, Nabil

2004-01-01

Two condensers designed for use in dissipating heat carried by working fluids feature two-phase, self-adjusting configurations such that their working lengths automatically vary to suit their input power levels and/or heat-sink temperatures. A key advantage of these condensers is that they can function even if the temperatures of their heat sinks fall below the freezing temperatures of their working fluids and the fluids freeze. The condensers can even be restarted from the frozen condition. The top part of the figure depicts the layout of the first condenser. A two-phase (liquid and vapor) condenser/vapor tube is thermally connected to a heat sink typically, a radiatively or convectively cooled metal panel. A single-phase (liquid) condensate-return tube (return artery) is also thermally connected to the heat sink. At intervals along their lengths, the condenser/vapor tube and the return artery are interconnected through porous plugs. This condenser configuration affords tolerance of freezing, variable effective thermal conductance (such that the return temperature remains nearly constant, independently of the ultimate sink temperature), and overall pressure drop smaller than it would be without the porous interconnections. An additional benefit of this configuration is that the condenser can be made to recover from the completely frozen condition either without using heaters, or else with the help of heaters much smaller than would otherwise be needed. The second condenser affords the same advantages and is based on a similar principle, but it has a different configuration that affords improved flow of working fluid, simplified construction, reduced weight, and faster recovery from a frozen condition.

Stepwise Bose-Einstein Condensation in a Spinor Gas.

PubMed

Frapolli, C; Zibold, T; Invernizzi, A; Jiménez-García, K; Dalibard, J; Gerbier, F

2017-08-04

We observe multistep condensation of sodium atoms with spin F=1, where the different Zeeman components m_{F}=0,±1 condense sequentially as the temperature decreases. The precise sequence changes drastically depending on the magnetization m_{z} and on the quadratic Zeeman energy q (QZE) in an applied magnetic field. For large QZE, the overall structure of the phase diagram is the same as for an ideal spin-1 gas, although the precise locations of the phase boundaries are significantly shifted by interactions. For small QZE, antiferromagnetic interactions qualitatively change the phase diagram with respect to the ideal case, leading, for instance, to condensation in m_{F}=±1, a phenomenon that cannot occur for an ideal gas with q>0.

Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

NASA Astrophysics Data System (ADS)

Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

2015-12-01

The German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new particle formation has not been observed.

Drying of pulverized material with heated condensible vapor

DOEpatents

Carlson, Larry W.

1986-01-01

Apparatus for drying pulverized material utilizes a high enthalpy condensable vapor such as steam for removing moisture from the individual particles of the pulverized material. The initially wet particulate material is tangentially delivered by a carrier vapor flow to an upper portion of a generally vertical cylindrical separation drum. The lateral wall of the separation drum is provided with a plurality of flow guides for directing the vapor tangentially therein in the direction of particulate material flow. Positioned concentrically within the separation drum and along the longitudinal axis thereof is a water-cooled condensation cylinder which is provided with a plurality of collection plates, or fins, on the outer lateral surface thereof. The cooled collection fins are aligned counter to the flow of the pulverized material and high enthalpy vapor mixture to maximize water vapor condensation thereon. The condensed liquid which includes moisture removed from the pulverized material then flows downward along the outer surface of the coolant cylinder and is collected and removed. The particles travel in a shallow helix due to respective centrifugal and vertical acceleration forces applied thereto. The individual particles of the pulverized material are directed outwardly by the vortex flow where they contact the inner cylindrical surface of the separation drum and are then deposited at the bottom thereof for easy collection and removal. The pulverized material drying apparatus is particularly adapted for drying coal fines and facilitates the recovery of the pulverized coal.

Magnetic Assisted Colloidal Pattern Formation

NASA Astrophysics Data System (ADS)

Yang, Ye

Pattern formation is a mysterious phenomenon occurring at all scales in nature. The beauty of the resulting structures and myriad of resulting properties occurring in naturally forming patterns have attracted great interest from scientists and engineers. One of the most convenient experimental models for studying pattern formation are colloidal particle suspensions, which can be used both to explore condensed matter phenomena and as a powerful fabrication technique for forming advanced materials. In my thesis, I have focused on the study of colloidal patterns, which can be conveniently tracked in an optical microscope yet can also be thermally equilibrated on experimentally relevant time scales, allowing for ground states and transitions between them to be studied with optical tracking algorithms. In particular, I have focused on systems that spontaneously organize due to particle-surface and particle-particle interactions, paying close attention to systems that can be dynamically adjusted with an externally applied magnetic or acoustic field. In the early stages of my doctoral studies, I developed a magnetic field manipulation technique to quantify the adhesion force between particles and surfaces. This manipulation technique is based on the magnetic dipolar interactions between colloidal particles and their "image dipoles" that appear within planar substrate. Since the particles interact with their own images, this system enables massively parallel surface force measurements (>100 measurements) in a single experiment, and allows statistical properties of particle-surface adhesion energies to be extracted as a function of loading rate. With this approach, I was able to probe sub-picoNewton surface interactions between colloidal particles and several substrates at the lowest force loading rates ever achieved. In the later stages of my doctoral studies, I focused on studying patterns formed from particle-particle interaction, which serve as an experimental model of phase transitions in condensed matter systems that can be tracked with single particle resolution. Compared with other research on colloidal crystal formation, my research has focused on multi-component colloidal systems of magnetic and non-magnetic colloids immersed in a ferrofluid. Initially, I studied the types of patterns that form as a function of the concentrations of the different particles and ferrofluid, and I discovered a wide variety of chains, rings and crystals forming in bi-component and tri-component systems. Based on these results, I narrowed my focus to one specific crystal structure (checkerboard lattice) as a model of phase transformations in alloy. Liquid/solid phase transitions were studied by slowly adjusting the magnetic field strength, which serves to control particle-particle interactions in a manner similar to controlling the physical temperature of the fluid. These studies were used to determine the optimal conditions for forming large single crystal structures, and paved the way for my later work on solid/solid phase transitions when the angle of the external field was shifted away from the normal direction. The magnetostriction coefficient of these crystals was measured in low tilt angle of the applied field. At high tilt angles, I observed a variety of martensitic transformations, which followed different pathways depending on the crystal direction relative to the in-plane field. In the last part of my doctoral studies, I investigated colloidal patterns formed in a superimposed acoustic and magnetic field. In this approach, the magnetic field mimics "temperature", while the acoustic field mimics "pressure". The ability to simultaneously tune both temperature and pressure allows for more efficient exploration of phase space. With this technique I demonstrated a large class of particle structures ranging from discrete molecule-like clusters to well ordered crystal phases. Additionally, I demonstrated a crosslinking strategy based on photoacids, which stabilized the structures after the external field was removed. This approach has potential applications in the fabrication of advanced materials. My thesis is arranged as follows. In Chapter 1, I present a brief background of general pattern formation and why I chose to investigate patterns formed in colloidal systems. I also provide a brief review of field-assisted manipulation techniques in order to motivate why I selected magnetic and acoustic field to study colloidal patterns. In chapter 2, I present the theoretical background of magnetic manipulation, which is the main technique used in my research. In this chapter, I will introduce the basic knowledge on magnetic materials and theories behind magnetic manipulation. The underlining thermodynamic mechanisms and theoretical/computational approaches in colloidal pattern formation are also briefly reviewed. In Chapter 3, I focus on using these concepts to study adhesion forces between particle and surfaces. In Chapter 4, I focus on exploring the ground states of colloidal patterns formed from the anti-ferromagnetic interactions of mixtures of particles, as a function of the particle volume fractions. In Chapter 5, I discuss my research on phase transformations of the well-ordered checkerboard phase formed from the equimolar mixture of magnetic and non-magnetic beads in ferrofluid, and I focus mainly on phase transformations in a slowly varying magnetic field. In Chapter 6, I discuss my work on the superimposed magnetic and acoustic field to study patterns formed from monocomponent colloidal suspensions under vertical confinement. Finally, I conclude my thesis in Chapter 7 and discuss future directions and open questions that can be explored in magnetic field directed self-organization in colloidal systems.

High-Harmonic Generation in Solids with and without Topological Edge States

NASA Astrophysics Data System (ADS)

Bauer, Dieter; Hansen, Kenneth K.

2018-04-01

High-harmonic generation in the two topological phases of a finite, one-dimensional, periodic structure is investigated using a self-consistent time-dependent density functional theory approach. For harmonic photon energies smaller than the band gap, the harmonic yield is found to differ by up to 14 orders of magnitude for the two topological phases. This giant topological effect is explained by the degree of destructive interference in the harmonic emission of all valence-band (and edge-state) electrons, which strongly depends on whether or not topological edge states are present. The combination of strong-field laser physics with topological condensed matter opens up new possibilities to electronically control strong-field-based light or particle sources or—conversely—to steer by all optical means topological electronics.

Flying Cages in Traveling Wave Ion Mobility: Influence of the Instrumental Parameters on the Topology of the Host-Guest Complexes

NASA Astrophysics Data System (ADS)

Carroy, Glenn; Lemaur, Vincent; Henoumont, Céline; Laurent, Sophie; De Winter, Julien; De Pauw, Edwin; Cornil, Jérôme; Gerbaux, Pascal

2018-01-01

Supramolecular mass spectrometry has emerged in the last decade as an orthogonal method to access, at the molecular level, the structures of noncovalent complexes extracted from the condensed phase to the rarefied gas phase using electrospray ionization. It is often considered that the soft nature of the ESI source confers to the method the capability to generate structural data comparable to those in the condensed phase. In the present paper, using the ammonium ion/cucurbituril combination as a model system, we investigate using ion mobility and computational chemistry the influence of the instrumental parameters on the topology, i.e., internal versus external association, of gaseous host/guest complex ions. MS and theoretical data are confronted to condensed phase data derived from nuclear magnetic resonance spectroscopy to assess whether the instrumental parameters can play an insidious role when trying to derive condensed phase data from mass spectrometry results. [Figure not available: see fulltext.

Thermodynamic properties of gas-condensate system with abnormally high content of heavy hydrocarbons

NASA Astrophysics Data System (ADS)

Zanochuev, S. A.; Shabarov, A. B.; Podorozhnikov, S. Yu; Zakharov, A. A.

2018-05-01

Gas-condensate systems (GCS) with an abnormally high content of heavy hydrocarbons are characterized by a sharp change in both phase and component compositions with an insignificant decrease in pressure below the start pressure of the phase transitions (the beginning of condensation). Calculation methods for describing the phase behavior of such systems are very sensitive to the quality of the initial information. The uncertainty of the input data leads not only to significant errors in the forecast of phase compositions, but also to an incorrect phase state estimation of the whole system. The research presents the experimental thermodynamic parameters of the GCS of the BT reservoirs on the Beregovoye field, obtained at the phase equilibrium facility. The data contribute to the adaptation of the calculated models of the phase behavior of the GCS with a change in pressure.

Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations

DOE PAGES

Yang, Huan; Goudeli, Eirini; Hogan, Christopher J.

2018-04-24

In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-Molecular Dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients; we use this approach to examine atomic condensation onto 6-56 atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity ( v) between atom and cluster andmore » the initial impact parameter ( b). In all cases there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms, and for 14 atom and 28 atom Mg clusters, as cluster equilibration temperature increases the condensation rate coefficient drops to values below the hard sphere rate coefficient. Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (> 1000 m s -1) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). In conclusion, the presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.« less

Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations.

PubMed

Yang, Huan; Goudeli, Eirini; Hogan, Christopher J

2018-04-28

In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard-sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-molecular dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients. We use this approach to examine atomic condensation onto 6-56-atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity (v) between atom and cluster and the initial impact parameter (b). In all cases, there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard-sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms and for 14- and 28-atom Mg clusters, as cluster equilibration temperature increases, the condensation rate coefficient drops to values below the hard-sphere rate coefficient. Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (>1000 m s -1 ) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). The presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.

Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Huan; Goudeli, Eirini; Hogan, Christopher J.

In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-Molecular Dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients; we use this approach to examine atomic condensation onto 6-56 atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity ( v) between atom and cluster andmore » the initial impact parameter ( b). In all cases there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms, and for 14 atom and 28 atom Mg clusters, as cluster equilibration temperature increases the condensation rate coefficient drops to values below the hard sphere rate coefficient. Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (> 1000 m s -1) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). In conclusion, the presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.« less

Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations

NASA Astrophysics Data System (ADS)

Yang, Huan; Goudeli, Eirini; Hogan, Christopher J.

2018-04-01

In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard-sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-molecular dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients. We use this approach to examine atomic condensation onto 6-56-atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity (v) between atom and cluster and the initial impact parameter (b). In all cases, there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard-sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms and for 14- and 28-atom Mg clusters, as cluster equilibration temperature increases, the condensation rate coefficient drops to values below the hard-sphere rate coefficient. Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (>1000 m s-1) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). The presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.

Selective condensation of aminoacyl adenylates by nucleoproteinoid microparticles.

NASA Technical Reports Server (NTRS)

Nakashima, T.; Fox, S. W.

1972-01-01

Microparticles composed of each of four enzymically synthesized homopolynucleotides and the same lysine-rich proteinoid have been found to influence the condensation of the AMP-anhydrides of each of four amino acids. The conditions of preparation of the particles and other variables of the experiments control the types of reaction. When a period set of conditions was identified empirically, the incorporation favored the amino acids whose present-day codons are related to the homopolynucleotide in the particle.

Heat-transfer characteristics of the R113 annular two-phase closed thermosyphon - Heat transfer in the condenser

NASA Astrophysics Data System (ADS)

Maezawa, Saburo; Tsuchida, Akira; Takuma, Masao

1988-08-01

Visual observation of flow patterns in the condenser and heat transfer measurements were conducted for heat transfer rate ranges of 18-800 W using a vertical annular device with various quantities of R113 as a working fluid. As a result of visual observations, it was shown that ripples (interfacial waves) were generated on the condensate film surface when the condensate film Reynolds number exceeded approximately 20, and the condensation heat transfer was prompted. A simple theoretical analysis was presented in which the effects of interfacial waves and vapor drag were both considered. This analysis agreed very well with experimental results when the working fluid quantity was small enough so that the two-phase mixture generated by boiling the working fluid did not reach the condenser. The effects of interfacial waves and vapor drag on condensation heat transfer were also investigated theoretically.

Aerosol Processing in Mixed-Phase Clouds in ECHAM5-HAM: Comparison of Single-Column Model Simulations to Observations

NASA Astrophysics Data System (ADS)

Hoose, C.; Lohmann, U.; Stier, P.; Verheggen, B.; Weingartner, E.; Herich, H.

2007-12-01

The global aerosol-climate model ECHAM5-HAM (Stier et al., 2005) has been extended by an explicit treatment of cloud-borne particles. Two additional modes for in-droplet and in-crystal particles are introduced, which are coupled to the number of cloud droplet and ice crystal concentrations simulated by the ECHAM5 double-moment cloud microphysics scheme (Lohmann et al., 2007). Transfer, production and removal of cloud-borne aerosol number and mass by cloud droplet activation, collision scavenging, aqueous-phase sulfate production, freezing, melting, evaporation, sublimation and precipitation formation are taken into account. The model performance is demonstrated and validated with observations of the evolution of total and interstitial aerosol concentrations and size distributions during three different mixed-phase cloud events at the alpine high-altitude research station Jungfraujoch (Switzerland) (Verheggen et al, 2007). Although the single-column simulations can not be compared one-to-one with the observations, the governing processes in the evolution of the cloud and aerosol parameters are captured qualitatively well. High scavenged fractions are found during the presence of liquid water, while the release of particles during the Bergeron-Findeisen process results in low scavenged fractions after cloud glaciation. The observed coexistence of liquid and ice, which might be related to cloud heterogeneity at subgrid scales, can only be simulated in the model when forcing non-equilibrium conditions. References: U. Lohmann et al., Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM, Atmos. Chem. Phys. 7, 3425-3446 (2007) P. Stier et al., The aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys. 5, 1125-1156 (2005) B. Verheggen et al., Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds, Accepted for publication in J. Geophys. Res. (2007)

Infrared spectroscopy and Mie scattering of acetylene aerosols formed in a low temperature diffusion cell

NASA Technical Reports Server (NTRS)

Dunder, T.; Miller, R. E.

1990-01-01

A method is described for forming and spectroscopically characterizing cryogenic aerosols formed in a low temperature gas cell. By adjusting the cell pressure, gas composition and flow rate, the size distribution of aerosol particles can be varied over a wide range. The combination of pressure and flow rate determine the residence time of the aerosols in the cell and hence the time available for the particles to grow. FTIR spectroscopy, over the range from 600/cm to 6000/cm, is used to characterize the aerosols. The particle size distribution can be varied so that, at one extreme, the spectra show only absorption features associated with the infrared active vibrational bands and, at the other, they display both absorption and Mie scattering. In the latter case, Mie scattering theory is used to obtain semiquantitative aerosol size distributions, which can be understood in terms of the interplay between nucleation and condensation. In the case of acetylene aerosols, the infrared spectra suggest that the particles exist in the high temperature cubic phase of the solid.

Middle atmosphere electrical structure, dynamics and coupling

NASA Technical Reports Server (NTRS)

Hale, L. C.

1984-01-01

The ram current to ion traps and the insensitivity of ion conductivity to compressibility provide the basis of robust techniques for middle atmosphere measurements. Gerdien condensers are more difficult to implement but provide more information. Mesospheric electrical conductivity shows many orders of magnitude variability, with depressions below gas phase model values indicating dominance by aerosol particles. The mobility of these ions has been directly measured and indicates particles of thousands of AMU. Large mesospheric fields have come into question, and diagnostic measurements show that many such measurements may be artifacts. However, some measurements of V/m fields with symmetrical and redundant sensors appear to be real. These fields complicate the 'mapping' picture of electrical coupling and may also modulate the transport of aerosol particles. They are probably related to neutral atmospheric dynamics and/or the aerosol particles. Lightning couples much more energy to the middle atmosphere and above than previously suspected, primarily in the ELF-UHF range. There are many important unanswered questions in this relatively unexplored frontier area which may be answered with low cost balloon and sounding rocket experiments.

[Separation of PM2.5 from coal combustion with phase change].

PubMed

Yan, Jin-pei; Yang, Lin-jun; Zhang, Xia; Sun, Lu-juan; Zhang, Yu; Shen, Xiang-lin

2008-12-01

The influence of two methods of gas moisture conditioning on removal efficiency of PM2.5 from coal combustion with addition of atomized droplets and steam was investigated. The particles size distribution and number concentration were measured in real time by electrical low pressure impactor (ELPI). The results show that collection efficiency of PM2.5 from coal combustion can be highly improved with steam condensational enlargement. Particle stage collection efficiency increases with the particles, especially for those smaller than 0.3 microm. The separation efficiency can be improved by 60% with the size of particles increasing from 0.03 microm to 0.3 microm for 0.1 kg/m3 of steam addition. The removal efficiency is independent of the gas temperature at the inlet of conditioning chamber for steam addition. But it increases with the gas temperature obviously for atomized droplets addition, which can be improved by 30% with increasing gas temperature from 136 degrees C to 256 degrees C. High removal efficiency of PM2.5 from coal combustion can be obtained with atomized droplets evaporation in hot flue gas except for steam addition.

Using satellite-based measurements to explore spatiotemporal scales and variability of drivers of new particle formation

EPA Science Inventory

New particle formation (NPF) can potentially alter regional climate by increasing aerosol particle (hereafter particle) number concentrations and ultimately cloud condensation nuclei. The large scales on which NPF is manifest indicate potential to use satellite-based (inherently ...

Kinetic modeling of the formation and growth of inorganic nano-particles during pulverized coal char combustion in O 2/N 2 and O 2/CO 2 atmospheres

DOE PAGES

Shaddix, Christopher R.; Niu, Yanqing; Hui, Shi'en; ...

2016-08-01

In this formation of nano-particles during coal char combustion, the vaporization of inorganic components in char and the subsequent homogeneous particle nucleation, heterogeneous condensation, coagulation, and coalescence play decisive roles. Furthermore, conventional measurements cannot provide detailed information on the dynamics of nano-particle formation and evolution, In this study, a sophisticated intrinsic char kinetics model that considers ash effects (including ash film formation, ash dilution, and ash vaporization acting in tandem), both oxidation and gasification by CO 2 and H 2O, homogeneous particle nucleation, heterogeneous vapor condensation, coagulation, and and coalescence mechanisms is developed and used to compare the temporal evolutionmore » of the number and size of nano-particles during coal char particle combustion as a function of char particle size, ash content, and oxygen content in O 2/N 2 and O 2/CO 2 atmospheres .« less

Kinetic modeling of the formation and growth of inorganic nano-particles during pulverized coal char combustion in O 2/N 2 and O 2/CO 2 atmospheres

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shaddix, Christopher R.; Niu, Yanqing; Hui, Shi'en

In this formation of nano-particles during coal char combustion, the vaporization of inorganic components in char and the subsequent homogeneous particle nucleation, heterogeneous condensation, coagulation, and coalescence play decisive roles. Furthermore, conventional measurements cannot provide detailed information on the dynamics of nano-particle formation and evolution, In this study, a sophisticated intrinsic char kinetics model that considers ash effects (including ash film formation, ash dilution, and ash vaporization acting in tandem), both oxidation and gasification by CO 2 and H 2O, homogeneous particle nucleation, heterogeneous vapor condensation, coagulation, and and coalescence mechanisms is developed and used to compare the temporal evolutionmore » of the number and size of nano-particles during coal char particle combustion as a function of char particle size, ash content, and oxygen content in O 2/N 2 and O 2/CO 2 atmospheres .« less

Thermodynamics and Dynamics of Bose condensation in a quasi-homogeneous gas

NASA Astrophysics Data System (ADS)

Navon, Nir; Schmidutz, Tobias; Gotlibovych, Igor; Gaunt, Alexander; Robert-de-Saint-Vincent, Martin; Smith, Robert; Hadzibabic, Zoran

2014-05-01

We present an experimental study of the thermodynamics and dynamics of Bose-Einstein condensation (BEC) in an optical-box trap. We first characterize the critical point for BEC, and observe saturation of the thermal component in a partially condensed cloud, in agreement with Einstein's textbook picture of a purely statistical phase transition. We also observed the quantum Joule-Thomson effect, namely isoenthalpic cooling of a non-interacting gas. We then investigate the dynamics of Bose condensation in the box potential following a rapid temperature quench through the phase transition, and focus on the time-evolution of the condensed fraction, the coherence length and the mean-field shift, that we probe via Bragg spectroscopy.

Interfacial condensation induced by sub-cooled liquid jet

NASA Astrophysics Data System (ADS)

Rame, Enrique; Balasubramaniam, R.

2016-11-01

When a sub-cooled liquid jet impinges on the free surface between a liquid and its vapor, vapor will condense at a rate dependent on the sub-cooling, the jet strength and fluid properties. In 1966 and during the examination of a different type of condensation flow, Shekriladeze found an approximate result, valid at large condensation rates, that decouples the flow in the liquid phase from that of the vapor, without putting it in the context of a formal asymptotic approximation. In this talk we will develop an asymptotic approximation that contains Shekriladze's result, and extend the calculations to the case when a non-condensable gas is present in the vapor phase.

Phase transition for the system of finite volume in the ϕ4 theory in the Tsallis nonextensive statistics

NASA Astrophysics Data System (ADS)

Ishihara, Masamichi

2018-04-01

We studied the effects of nonextensivity on the phase transition for the system of finite volume V in the ϕ4 theory in the Tsallis nonextensive statistics of entropic parameter q and temperature T, when the deviation from the Boltzmann-Gibbs (BG) statistics, |q ‑ 1|, is small. We calculated the condensate and the effective mass to the order q ‑ 1 with the normalized q-expectation value under the free particle approximation with zero bare mass. The following facts were found. The condensate Φ divided by v, Φ/v, at q (v is the value of the condensate at T = 0) is smaller than that at q‧ for q > q‧ as a function of Tph/v which is the physical temperature Tph divided by v. The physical temperature Tph is related to the variation of the Tsallis entropy and the variation of the internal energies, and Tph at q = 1 coincides with T. The effective mass decreases, reaches minimum, and increases after that, as Tph increases. The effective mass at q > 1 is lighter than the effective mass at q = 1 at low physical temperature and heavier than the effective mass at q = 1 at high physical temperature. The effects of the nonextensivity on the physical quantity as a function of Tph become strong as |q ‑ 1| increases. The results indicate the significance of the definition of the expectation value, the definition of the physical temperature, and the constraints for the density operator, when the terms including the volume of the system are not negligible.

Nanocellulose Fragmentation Mechanisms and Inversion of Chirality from the Single Particle to the Cholesteric Phase.

PubMed

Nyström, Gustav; Arcari, Mario; Adamcik, Jozef; Usov, Ivan; Mezzenga, Raffaele

2018-05-22

Understanding how nanostructure and nanomechanics influence physical material properties on the micro- and macroscale is an essential goal in soft condensed matter research. Mechanisms governing fragmentation and chirality inversion of filamentous colloids are of specific interest because of their critical role in load-bearing and self-organizing functionalities of soft nanomaterials. Here we provide a fundamental insight into the self-organization across several length scales of nanocellulose, an important biocolloid system with wide-ranging applications as structural, insulating, and functional material. Through a combined microscopic and statistical analysis of nanocellulose fibrils at the single particle level, we show how mechanically and chemically induced fragmentations proceed in this system. Moreover, by studying the bottom-up self-assembly of fragmented carboxylated cellulose nanofibrils into cholesteric liquid crystals, we show via direct microscopic observations that the chirality is inverted from right-handed at the nanofibril level to left-handed at the level of the liquid crystal phase. These results improve our fundamental understanding of nanocellulose and provide an important rationale for its application in colloidal systems, liquid crystals, and nanomaterials.

Organic condensation - a vital link connecting aerosol formation to climate forcing

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-01-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Microfluidic techniques for the study of self-assembly of soft materials

NASA Astrophysics Data System (ADS)

Aguade Cabanas, Rafael

This research is an approach to the study of soft condensed matter where the use of new microfluidic technology plays a central role. Often, in the study of soft matter, the sample volumes are very small, of the order of nanoliters. Therefore to quantitatively measure the equilibrium or non-equilibrium phase behavior requires microfluidics. Presented here are (1) a new way of producing aqueous drops of order 1 nl volume, in oil, (2) a new fabrication protocol to make microfluidic devices out of epoxy glue, and (3) a new microfluidic flow cell to study colloidal self-assembly. Also presented here is a new kind of colloidal particle, consisting of single strands of DNA linked to the surface of fd virus. This new particle may serve as a liquid crystalline colloid with a temperature dependent tunable potential. The fabrication process is the first step in the study of the self-assembly of rod-like particles with a temperature dependent potential.

Uptake of Alkylamines on Dicarboxylic Acids Relevant to Secondary Organic Aerosol Formation

NASA Astrophysics Data System (ADS)

Marrero-Ortiz, W.; Secrest, J.; Zhang, R.

2017-12-01

Aerosols play a critical role in climate directly by scattering and absorbing solar radiation, and indirectly by functioning as cloud condensation nuclei (CCN); both represent the largest uncertainties in climate predictions. New particle formation contributes significantly to CCN production; however, the mechanisms related to particle nucleation and growth processes are not well understood. Organic acids are atmospherically abundant, and their neutralization by low molecular weight amines may result in the formation of stable low volatility aminium salt products contributing to the growth of secondary organic aerosols and even the alteration of the aerosol properties. The acid-base neutralization of particle phase succinic acid and tartaric acid by low molecular weight aliphatic amines, i.e. methylamine, dimethylamine, and trimethylamine, has been investigated by employing a low-pressure fast flow reactor at 298K with an ion drift - chemical ionization mass spectrometer (ID-CIMS). The heterogeneous uptake is time dependent and influenced by organic acids functionality, alkylamines basicity, and steric effect. The implications of our results to atmospheric nanoparticle growth will be discussed.

Yield of reversible colloidal gels during flow start-up: release from kinetic arrest.

PubMed

Johnson, Lilian C; Landrum, Benjamin J; Zia, Roseanna N

2018-06-05

Yield of colloidal gels during start-up of shear flow is characterized by an overshoot in shear stress that accompanies changes in network structure. Prior studies of yield of reversible colloidal gels undergoing strong flow model the overshoot as the point at which network rupture permits fluidization. However, yield under weak flow, which is of interest in many biological and industrial fluids shows no such disintegration. The mechanics of reversible gels are influenced by bond strength and durability, where ongoing rupture and re-formation impart aging that deepens kinetic arrest [Zia et al., J. Rheol., 2014, 58, 1121], suggesting that yield be viewed as release from kinetic arrest. To explore this idea, we study reversible colloidal gels during start-up of shear flow via dynamic simulation, connecting rheological yield to detailed measurements of structure, bond dynamics, and potential energy. We find that pre-yield stress grows temporally with the changing roles of microscopic transport processes: early time behavior is set by Brownian diffusion; later, advective displacements permit relative particle motion that stretches bonds and stores energy. Stress accumulates in stretched, oriented bonds until yield, which is a tipping point to energy release, and is passed with a fully intact network, where the loss of very few bonds enables relaxation of many, easing glassy arrest. This is immediately followed by a reversal to growth in potential energy during bulk plastic deformation and condensation into larger particle domains, supporting the view that yield is an activated release from kinetic arrest. The continued condensation of dense domains and shrinkage of network surfaces, along with a decrease in the potential energy, permit the gel to evolve toward more complete phase separation, supporting our view that yield of weakly sheared gels is a 'non-equilibrium phase transition'. Our findings may be particularly useful for industrial or other coatings, where weak, slow application via shear may lead to phase separation, inhibiting smooth distribution.

Water Capture Device Signal Integration Board

NASA Technical Reports Server (NTRS)

Chamberlin, Kathryn J.; Hartnett, Andrew J.

2018-01-01

I am a junior in electrical engineering at Arizona State University, and this is my second internship at Johnson Space Center. I am an intern in the Command and Data Handling Branch of Avionics Division (EV2), my previous internship was also in EV2. During my previous internship I was assigned to the Water Capture Device payload, where I designed a prototype circuit board for the electronics system of the payload. For this internship, I have come back to the Water Capture Device project to further the work on the electronics design I completed previously. The Water Capture Device is an experimental payload to test the functionality of two different phase separators aboard the International Space Station (ISS). A phase separator sits downstream of a condensing heat exchanger (CHX) and separates the water from the air particles for environmental control on the ISS. With changing CHX technology, new phase separators are required. The goal of the project is to develop a test bed for the two phase separators to determine the best solution.

Generating a Multiphase Equation of State with Swarm Intelligence

NASA Astrophysics Data System (ADS)

Cox, Geoffrey

2017-06-01

Hydrocode calculations require knowledge of the variation of pressure of a material with density and temperature, which is given by the equation of state. An accurate model needs to account for discontinuities in energy, density and properties of a material across a phase boundary. When generating a multiphase equation of state the modeller attempts to balance the agreement between the available data for compression, expansion and phase boundary location. However, this can prove difficult because minor adjustments in the equation of state for a single phase can have a large impact on the overall phase diagram. Recently, Cox and Christie described a method for combining statistical-mechanics-based condensed matter physics models with a stochastic analysis technique called particle swarm optimisation. The models produced show good agreement with experiment over a wide range of pressure-temperature space. This talk details the general implementation of this technique, shows example results, and describes the types of analysis that can be performed with this method.

Separation and recycling of nanoparticles using cloud point extraction with non-ionic surfactant mixtures.

PubMed

Nazar, Muhammad Faizan; Shah, Syed Sakhawat; Eastoe, Julian; Khan, Asad Muhammad; Shah, Afzal

2011-11-15

A viable cost-effective approach employing mixtures of non-ionic surfactants Triton X-114/Triton X-100 (TX-114/TX-100), and subsequent cloud point extraction (CPE), has been utilized to concentrate and recycle inorganic nanoparticles (NPs) in aqueous media. Gold Au- and palladium Pd-NPs have been pre-synthesized in aqueous phases and stabilized by sodium 2-mercaptoethanesulfonate (MES) ligands, then dispersed in aqueous non-ionic surfactant mixtures. Heating the NP-micellar systems induced cloud point phase separations, resulting in concentration of the NPs in lower phases after the transition. For the Au-NPs UV/vis absorption has been used to quantify the recovery and recycle efficiency after five repeated CPE cycles. Transmission electron microscopy (TEM) was used to investigate NP size, shape, and stability. The results showed that NPs are preserved after the recovery processes, but highlight a potential limitation, in that further particle growth can occur in the condensed phases. Copyright © 2011 Elsevier Inc. All rights reserved.

Triply degenerate nodal points and topological phase transitions in NaCu3Te2

NASA Astrophysics Data System (ADS)

Xia, Yunyouyou; Li, Gang

2017-12-01

Quasiparticle excitations of free electrons in condensed-matter physics, characterized by the dimensionality of the band crossing, can find their elementary-particle analogs in high-energy physics, such as Majorana, Weyl, and Dirac fermions, while crystalline symmetry allows more quasiparticle excitations and exotic fermions to emerge. Using symmetry analysis and ab initio calculations, we propose that the three-dimensional honeycomb crystal NaCu3Te2 hosts triply degenerate nodal points (TDNPs) residing at the Fermi level. Furthermore, in this system we find a tunable phase transition between a trivial insulator, a TDNP phase, and a weak topological insulator (TI), triggered by a symmetry-allowed perturbation and the spin-orbital coupling (SOC). Such a topological nontrivial ternary compound not only serves as a perfect candidate for studying three-component fermions, but also provides an excellent playground for understanding the topological phase transitions between TDNPs, TIs, and trivial insulators, which distinguishes this system from other TDNP candidates.

Higgs amplitude mode in a two-dimensional quantum antiferromagnet near the quantum critical point

NASA Astrophysics Data System (ADS)

Hong, Tao; Matsumoto, Masashige; Qiu, Yiming; Chen, Wangchun; Gentile, Thomas R.; Watson, Shannon; Awwadi, Firas F.; Turnbull, Mark M.; Dissanayake, Sachith E.; Agrawal, Harish; Toft-Petersen, Rasmus; Klemke, Bastian; Coester, Kris; Schmidt, Kai P.; Tennant, David A.

2017-07-01

Spontaneous symmetry-breaking quantum phase transitions play an essential role in condensed-matter physics. The collective excitations in the broken-symmetry phase near the quantum critical point can be characterized by fluctuations of phase and amplitude of the order parameter. The phase oscillations correspond to the massless Nambu-Goldstone modes whereas the massive amplitude mode, analogous to the Higgs boson in particle physics, is prone to decay into a pair of low-energy Nambu-Goldstone modes in low dimensions. Especially, observation of a Higgs amplitude mode in two dimensions is an outstanding experimental challenge. Here, using inelastic neutron scattering and applying the bond-operator theory, we directly and unambiguously identify the Higgs amplitude mode in a two-dimensional S = 1/2 quantum antiferromagnet C9H18N2CuBr4 near a quantum critical point in two dimensions. Owing to an anisotropic energy gap, it kinematically prevents such decay and the Higgs amplitude mode acquires an infinite lifetime.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ackerman, P. J.; van de Lagemaat, J.; Smalyukh, I. I.

Some of the most exotic condensed matter phases, such as twist grain boundary and blue phases in liquid crystals and Abrikosov phases in superconductors, contain arrays of topological defects in their ground state. Comprised of a triangular lattice of double-twist tubes of magnetization, the so-called ‘A-phase’ in chiral magnets is an example of a thermodynamically stable phase with topologically nontrivial solitonic field configurations referred to as two-dimensional skyrmions, or baby-skyrmions. Here we report that three-dimensional skyrmions in the form of double-twist tori called ‘hopfions’, or ‘torons’ when accompanied by additional self-compensating defects, self-assemble into periodic arrays and linear chains thatmore » exhibit electrostriction. In confined chiral nematic liquid crystals, this self-assembly is similar to that of liquid crystal colloids and originates from long-range elastic interactions between particle-like skyrmionic torus knots of molecular alignment field, which can be tuned from isotropic repulsive to weakly or highly anisotropic attractive by low-voltage electric fields.« less

Effect of photochemical aging on the ice nucleation properties of diesel and wood burning particles

NASA Astrophysics Data System (ADS)

Chou, C.; Stetzer, O.; Tritscher, T.; Chirico, R.; Heringa, M. F.; Kanji, Z. A.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.; Lohmann, U.

2012-06-01

A measurement campaign (IMBALANCE) was conducted in 2009 and aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro with no emission after-treatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, -30 °C, -35 °C and -40 °C. Freshly emitted diesel particles showed ice formation only at -40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical aging did not play a role in modifying their ice nucleation behavior. Only one diesel experiment where α-pinene was added, showed an ice nucleation enhancement after the aging at -35 °C. Wood burning particles also act as ice nuclei (IN) at -40 °C in the deposition mode at the same conditions as for diesel particles and photochemical aging did also not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at -35 °C with no ice nucleation observed at -30 °C for wood burning particles. Photochemical aging did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below -30 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical aging on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

Characterization of three new condensation particle counters for sub-3 nm particle detection during the Helsinki CPC workshop: the ADI versatile water CPC, TSI 3777 nano enhancer and boosted TSI 3010

NASA Astrophysics Data System (ADS)

Kangasluoma, Juha; Hering, Susanne; Picard, David; Lewis, Gregory; Enroth, Joonas; Korhonen, Frans; Kulmala, Markku; Sellegri, Karine; Attoui, Michel; Petäjä, Tuukka

2017-06-01

In this study we characterized the performance of three new particle counters able to detect particles smaller than 3 nm during the Helsinki condensation particle counter (CPC) workshop in summer 2016: the Aerosol Dynamics Inc. (ADI; Berkeley, USA) versatile water condensation particle counter (vWCPC), TSI 3777 nano enhancer (TSI Inc., Shoreview, USA) and modified and boosted TSI 3010-type CPC from Université Blaise Pascal called a B3010. The performance of all CPCs was first measured with charged tungsten oxide test particles at temperature settings which resulted in supersaturation low enough to not detect any ions produced by a radioactive source. Due to similar measured detection efficiencies, additional comparison between the 3777 and vWCPC were conducted using electrically neutral tungsten oxide test particles and with positively charged tetradodecylammonium bromide. Furthermore, the detection efficiencies of the 3777 and vWCPC were measured with boosted temperature settings yielding supersaturation which was at the onset of homogeneous nucleation for the 3777 or confined within the range of liquid water for the ADI vWCPC. Finally, CPC-specific tests were conducted to probe the response of the 3777 to various inlet flow relative humidities, of the B3010 to various inlet flow rates and of the vWCPC to various particle concentrations. For the 3777 and vWCPC the measured 50 % detection diameters (d50s) were in the range of 1.3-2.4 nm for the tungsten oxide particles, depending on the particle charging state and CPC temperature settings, between 2.5 and 3.3 nm for the organic test aerosol, and in the range of 3.2-3.4 nm for tungsten oxide for the B3010.

Flow Boiling and Condensation Experiment (FBCE) for the International Space Station

NASA Technical Reports Server (NTRS)

Mudawar, Issam; Hasan, Mohammad M.; Kharangate, Chirag; O'Neill, Lucas; Konishi, Chris; Nahra, Henry; Hall, Nancy; Balasubramaniam, R.; Mackey, Jeffrey

2015-01-01

The proposed research aims to develop an integrated two-phase flow boiling/condensation facility for the International Space Station (ISS) to serve as primary platform for obtaining two-phase flow and heat transfer data in microgravity.

Evaluation of selected chemical processes for production of low-cost silicon, phases 1 and 2

NASA Technical Reports Server (NTRS)

Blocher, J. M.; Browning, M. F.

1978-01-01

A miniplant, consisting of a 5 cm-diameter fluidized-bed reactor and associated equipment was used to study the deposition parameters, temperature, reactant composition, seed particle size, bed depth, reactant throughput, and methods of reactant introduction. It was confirmed that the permissible range of fluidized-bed temperature was limited at the lower end by zinc condensation (918 C) and at higher temperatures by rapidly decreasing conversion efficiency. Use of a graded bed temperature was shown to increase the conversion efficiency over that obtained in an isothermal bed. Other aspects of the process such as the condensation and fused-salt electrolysis of the ZnCl2 by-product for recycle of zinc and chlorine were studied to provide information required for design of a 50 MT/year experimental facility. In view of the favorable technical and economic indications obtained, it was recommended that construction and operation of the 50 MT/year experimental facility be implemented.

Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors.

PubMed

Abdelsayed, Victor; El-Shall, M Samy

2014-08-07

This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicates that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong correlation is found between the seed nanoparticle's size and the degree of the supersaturation of the condensing vapor. This result and the agreement among the calculated Kelvin diameters and the size of the nucleating Al nanoparticles determined by transmission electron microscopy provide strong proof for the development of a new approach for the separation and characterization of heterogeneous nuclei formed in organic vapors. These processes can take place in the atmosphere by a combination of several organic species including polar compounds which could be very efficient in activating charged nanoparticles and cluster ions of atmospheric relevance.

Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: Nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Abdelsayed, Victor; Samy El-Shall, M., E-mail: mselshal@vcu.edu

This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicatesmore » that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong correlation is found between the seed nanoparticle's size and the degree of the supersaturation of the condensing vapor. This result and the agreement among the calculated Kelvin diameters and the size of the nucleating Al nanoparticles determined by transmission electron microscopy provide strong proof for the development of a new approach for the separation and characterization of heterogeneous nuclei formed in organic vapors. These processes can take place in the atmosphere by a combination of several organic species including polar compounds which could be very efficient in activating charged nanoparticles and cluster ions of atmospheric relevance.« less

Condensate fluctuations of interacting Bose gases within a microcanonical ensemble.

PubMed

Wang, Jianhui; He, Jizhou; Ma, Yongli

2011-05-01

Based on counting statistics and Bogoliubov theory, we present a recurrence relation for the microcanonical partition function for a weakly interacting Bose gas with a finite number of particles in a cubic box. According to this microcanonical partition function, we calculate numerically the distribution function, condensate fraction, and condensate fluctuations for a finite and isolated Bose-Einstein condensate. For ideal and weakly interacting Bose gases, we compare the condensate fluctuations with those in the canonical ensemble. The present approach yields an accurate account of the condensate fluctuations for temperatures close to the critical region. We emphasize that the interactions between excited atoms turn out to be important for moderate temperatures.

Emission characteristics for gaseous- and size-segregated particulate PAHs in coal combustion flue gas from circulating fluidized bed (CFB) boiler.

PubMed

Wang, Ruwei; Liu, Guijian; Sun, Ruoyu; Yousaf, Balal; Wang, Jizhong; Liu, Rongqiong; Zhang, Hong

2018-07-01

The partitioning behavior of polycyclic aromatic hydrocarbons (PAHs) between gaseous and particulate phases from coal-fired power plants (CFPPs) is critically important to predict PAH removal by dust control devices. In this study, 16 US-EPA priority PAHs in gaseous and size-segregated particulate phases at the inlet and outlet of the fabric filter unit (FFs) of a circulating fluidized bed (CFB) boiler were analyzed. The partitioning mechanisms of PAHs between gaseous and particulate phases and in particles of different size classes were investigated. We found that the removal efficiencies of PAHs are 45.59% and 70.67-89.06% for gaseous and particulate phases, respectively. The gaseous phase mainly contains low molecular weight (LMW) PAHs (2- and 3-ring PAHs), which is quite different from the particulate phase that mainly contains medium and high molecular weight (MMW and HMW) PAHs (4- to 6-ring PAHs). The fractions of LMW PAHs show a declining trend with the decrease of particle size. The gas-particle partitioning of PAHs is primarily controlled by organic carbon absorption, in addition, it has a clear dependence on the particle sizes. Plot of log (TPAH/PM) against logD p shows that all slope values were below -1, suggesting that PAHs were mainly adsorbed to particulates. The adsorption effect of PAHs in size-segregated PMs for HMW PAHs is more evident than LMW PAHs. The particle size distributions (PSDs) of individual PAHs show that most of PAHs exhibit bi-model structures, with one mode peaking in the accumulation size range (2.1-1.1 μm) and another mode peaking in coarse size range (5.8-4.7 μm). The intensities of these two peaks vary in function of ring number of PAHs, which is likely attributed to Kelvin effect that the less volatile HMW PAH species preferentially condense onto the finer particulates. The emission factor of PAHs was calculated as 3.53 mg/kg of coal burned, with overall mean EF PAH of 0.55 and 2.98 mg/kg for gaseous and particulate phase, respectively. Moreover, the average emission amount of PAHs for the investigated CFPP was 1016.6 g/day and 371073.6 g/y, respectively. Copyright © 2018 Elsevier Ltd. All rights reserved.

Condensation and single-phase heat transfer coefficient and flow regime visualization in microchannel tubes for HFC-134A

NASA Astrophysics Data System (ADS)

Wang, Wei-Wen William

This dissertation is to document experimental, local condensation and single-phase heat transfer and flow data of the minute diameter, microchannel tube and to develop correlation methods for optimizing the design of horizontal-microchannel condensers. It is essential to collect local data as the condensation progresses through several different flow patterns, since as more liquid is formed, the mechanism conducting heat transfer and flow is also changing. Therefore, the identification of the flow pattern is as important as the thermal and dynamic data. The experimental results were compared with correlation and flow regime maps from literature. The experiment using refrigerant HFC-134a in flat, multi-port aluminum tubing with 1.46mm hydraulic diameter was conducted. The characteristic of single-phase friction can be described with the analytical solution of square channel. The Gnielinski correlation provided good prediction of single-phase turbulent flow heat transfer. Higher mass fluxes and qualities resulted in increased condensation heat transfer and were more effective in the shear-dominated annular flow. The effect of temperature gradient from wall to refrigerant attributed profoundly in the gravity-dominated wavy/slug flow. Two correlation based on different flow mechanisms were developed for specified flow regimes. Finally, an asymptotic correlation was successfully proposed to account for the entire data regardless of flow patterns. Data taken from experiment and observations obtained from flow visualization, resulted in a better understanding of the physics in microchannel condensation, optimized designs in the microchannel condensers are now possible.

Non-linear photochemical pathways in laser-induced atmospheric aerosol formation

PubMed Central

Mongin, Denis; Slowik, Jay G.; Schubert, Elise; Brisset, Jean-Gabriel; Berti, Nicolas; Moret, Michel; Prévôt, André S. H.; Baltensperger, Urs; Kasparian, Jérôme; Wolf, Jean-Pierre

2015-01-01

We measured the chemical composition and the size distribution of aerosols generated by femtosecond-Terawatt laser pulses in the atmosphere using an aerosol mass spectrometer (AMS). We show that nitric acid condenses in the form of ammonium nitrate, and that oxidized volatile organics also contribute to particle growth. These two components account for two thirds and one third, respectively, of the dry laser-condensed mass. They appear in two different modes centred at 380 nm and 150 nm. The number concentration of particles between 25 and 300 nm increases by a factor of 15. Pre-existing water droplets strongly increase the oxidative properties of the laser-activated atmosphere, substantially enhancing the condensation of organics under laser illumination. PMID:26450172

Phase-driven collapse of the Cooper condensate in a nanosized superconductor

NASA Astrophysics Data System (ADS)

Ronzani, Alberto; D'Ambrosio, Sophie; Virtanen, Pauli; Giazotto, Francesco; Altimiras, Carles

2017-12-01

Superconductivity can be understood in terms of a phase transition from an uncorrelated electron gas to a condensate of Cooper pairs in which the relative phases of the constituent electrons are coherent over macroscopic length scales. The degree of correlation is quantified by a complex-valued order parameter, whose amplitude is proportional to the strength of the pairing potential in the condensate. Supercurrent-carrying states are associated with nonzero values of the spatial gradient of the phase. The pairing potential and several physical observables of the Cooper condensate can be manipulated by means of temperature, current bias, dishomogeneities in the chemical composition, or application of a magnetic field. Here we show evidence of complete suppression of the energy gap in the local density of quasiparticle states (DOS) of a superconducting nanowire upon establishing a phase difference equal to π over a length scale comparable to the superconducting coherence length. These observations are consistent with a complete collapse of the pairing potential in the center of the wire, in accordance with theoretical modeling based on the quasiclassical theory of superconductivity in diffusive systems. Our spectroscopic data, fully exploring the phase-biased states of the condensate, highlight the profound effect that extreme phase gradients exert on the amplitude of the pairing potential. Moreover, the sharp magnetic response (up to 27 mV/Φ0) observed near the onset of the superconducting gap collapse regime is exploited to realize magnetic flux detectors with noise-equivalent resolution as low as 260 n Φ0/√{Hz} .

[Role of mexidol (2-ethyl-6-methyl-3-hydroxypyridine succinate) in the obtaining of stabilized magnetite nanoparticles for biomedical application].

PubMed

Vazhnichaya, Ye M; Mokliak, Ye V; Kurapov, Yu A; Zabozlaev, A A

2015-01-01

Magnetite nanoparticles (NPs) are studied as agents for magnetic resonance imaging, hyperthermia of malignant tumors, targeted drug delivery as well as anti-anemic action. One of the main problems of such NPs is their aggregation that requires creation of methods for magnetite NPs stabilization during preparation of liquid medicinal forms on their basis. The present work is devoted to the possibility of mexidol (2-ethyl-6-methyl-3-hydroxypyridine succinate) use for solubilization of magnetite NPs in hydrophilic medium. For this purpose, the condensate produced by electron-beam evaporation and condensation, with magnetite particles of size 5-8 nm deposited into the crystals of sodium chloride were used in conjunction with substance of mexidol (2-ethyl-6-methyl-3-hydroxypyridine succinate), and low molecular weight polyvinylpyrrolidone (PVP). The NP condensate was dispersed in distilled water or PVP or mexidol solutions. NPs size distribution in the liquid phase of the systems was determined by photon correlation spectroscopy, iron (Fe) concentration was evaluated by atomic emission spectrometry. It is shown that in the dispersion prepared in distilled water, the major amount of NPs was of 13-120 nm in size, in mexidol solution - 270-1700 nm, in PVP solution - 30-900 nm. In the fluid containing magnetite NPs together with mexidol and PVP, the main fraction (99.9%) was characterized by the NPs size of 14-75 nm with maximum of 25 nm. This system had the highest iron concentration: it was similar to that in the sample with mexidol solution and 6.6-7.3 times higher than the concentration in the samples with distilled water or PVP. Thus, in the preparation of aqueous dispersions based on magnetite NPs condensate, mexidol provides a transition of Fe to the liquid phase in amount necessary to achieve its biological activity, and PVP stabilizes such modified NPs.

Gas-Liquid Processing in Microchannels

DOE Office of Scientific and Technical Information (OSTI.GOV)

TeGrotenhuis, Ward E.; Stenkamp, Victoria S.; Twitchell, Alvin

Processing gases and liquids together in microchannels having at least one dimension <1 mm has unique advantages for rapid heat and mass transfer. One approach for managing the two phases is to use porous structures as wicks within microchannels to segregate the liquid phase from the gas phase. Gas-liquid processing is accomplished by providing a gas flow path and inducing flow of the liquid phase through or along the wick under an induced pressure gradient. A variety of unit operations are enabled, including phase separation, partial condensation, absorption, desorption, and distillation. Results are reported of an investigation of microchannel phasemore » separation in a transparent, single-channel device. Next, heat exchange is integrated with the microchannel wick approach to create a partial condenser that also separates the condensate. Finally, the scale-up to a multi-channel phase separator is described.« less

Incoherent population mixing contributions to phase-modulation two-dimensional coherent excitation spectra

NASA Astrophysics Data System (ADS)

Grégoire, Pascal; Srimath Kandada, Ajay Ram; Vella, Eleonora; Tao, Chen; Leonelli, Richard; Silva, Carlos

2017-09-01

We present theoretical and experimental results showing the effects of incoherent population mixing on two-dimensional (2D) coherent excitation spectra that are measured via a time-integrated population and phase-sensitive detection. The technique uses four collinear ultrashort pulses and phase modulation to acquire two-dimensional spectra by isolating specific nonlinear contributions to the photoluminescence or photocurrent excitation signal. We demonstrate that an incoherent contribution to the measured line shape, arising from nonlinear population dynamics over the entire photoexcitation lifetime, generates a similar line shape to the expected 2D coherent spectra in condensed-phase systems. In those systems, photoexcitations are mobile such that inter-particle interactions are important on any time scale, including those long compared with the 2D coherent experiment. Measurements on a semicrystalline polymeric semiconductor film at low temperatures show that, in some conditions in which multi-exciton interactions are suppressed, the technique predominantly detects coherent signals and can be used, in our example, to extract homogeneous line widths. The same method used on a lead-halide perovskite photovoltaic cell shows that incoherent population mixing of mobile photocarriers can dominate the measured signal since carrier-carrier bimolecular scattering is active even at low excitation densities, which hides the coherent contribution to the spectral line shape. In this example, the intensity dependence of the signal matches the theoretical predictions over more than two orders of magnitude, confirming the incoherent nature of the signal. While these effects are typically not significant in dilute solution environments, we demonstrate the necessity to characterize, in condensed-phase materials systems, the extent of nonlinear population dynamics of photoexcitations (excitons, charge carriers, etc.) in the execution of this powerful population-detected coherent spectroscopy technique.