Self-Nucleation in the Sulfuric Acid-Water System

Doyle, George J.

doi:10.1063/1.1701218

Cited by 270 publications

(97 citation statements)

References 16 publications

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“…The presence of non-volatile vapours is essential for the growth of freshly formed particles. Binary nucleation of water and sulphuric acid needs conditions of low temperature, high relative humidities, aerosol concentrations and a high amount of sulphuric acid (Doyle, 1961;Raes et. al, 1992;Kulmala et al, 2000).…”

Section: Introductionmentioning

confidence: 99%

ALADINA – an unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer

Altstädter

Platis²,

Wehner

et al. 2015

Atmos. Meas. Tech.

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Abstract. This paper presents the unmanned research aircraft Carolo P360 "ALADINA" (Application of Light-weight Aircraft for Detecting IN situ Aerosol) for investigating the horizontal and vertical distribution of ultrafine particles in the atmospheric boundary layer (ABL). It has a wingspan of 3.6 m, a maximum take-off weight of 25 kg and is equipped with aerosol instrumentation and meteorological sensors. A first application of the system, together with the unmanned research aircraft MASC (Multi-Purpose Airborne Carrier) of the Eberhard Karls University of Tübingen (EKUT), is described. As small payload for ALADINA, two condensation particle counters (CPC) and one optical particle counter (OPC) were miniaturised by re-arranging the vital parts and composing them in a space-saving way in the front compartment of the airframe. The CPCs are improved concerning the lower detection threshold and the response time to less than 1.3 s. Each system was characterised in the laboratory and calibrated with test aerosols. The CPCs are operated in this study with two different lower detection threshold diameters of 11 and 18 nm. The amount of ultrafine particles, which is an indicator for new particle formation, is derived from the difference in number concentrations of the two CPCs ( N). Turbulence and thermodynamic structure of the boundary layer are described by measurements of fast meteorological sensors that are mounted at the aircraft nose. A first demonstration of ALADINA and a feasibility study were conducted in Melpitz near Leipzig, Germany, at the Global Atmosphere Watch (GAW) station of the Leibniz Institute for Tropospheric Research (TROPOS) on 2 days in October 2013. There, various ground-based instruments are installed for long-term atmospheric monitoring. The groundbased infrastructure provides valuable additional background information to embed the flights in the continuous atmospheric context and is used for validation of the airborne results. The development of the boundary layer, derived from backscatter signals of a portable Raman lidar POLLY XT , allows a quick overview of the current vertical structure of atmospheric particles. Ground-based aerosol number concentrations are consistent with the results from flights in heights of a few metres. In addition, a direct comparison of ALAD-INA aerosol data and ground-based aerosol data, sampling the air at the same location for more than 1 h, shows comparable values within the range of ± 20 %. MASC was operated simultaneously with complementary flight patterns. It is equipped with the same meteorological instruments that offer the possibility to determine turbulent fluxes. Therefore, additional information about meteorological conditions was collected in the lowest part of the atmosphere. Vertical profiles up to 1000 m in altitude indicate a high variability with distinct layers of aerosol, especially for the small particles of a few nanometres in diameter on 1 particular day. The stratification was almost neutral and two significant aerosol layers were detect...

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Section: Introductionmentioning

confidence: 99%

ALADINA – an unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer

Altstädter

Platis²,

Wehner

et al. 2015

Atmos. Meas. Tech.

View full text Add to dashboard Cite

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“…Small binary clusters of H 2 O and H 2 SO 4 play a crucial role in atmospheric processes ranging from ordinary vapor-to-liquid nucleation [1][2][3][4][5] to acid rain formation [6][7][8] and ozone depletion mechanisms. 9-11 Doyle's early work 2 predicted that even in undersaturated atmospheres a sulfuric acid vapor pressure of 10 -9 Torr can produce binary nucleation with water.…”

Section: Introductionmentioning

confidence: 99%

Monte Carlo Simulations of Small Sulfuric Acid−Water Clusters

Kathmann

Hale

2001

J. Phys. Chem. B

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Effective atom-atom potentials are developed for binary sulfuric acid-water clusters and applied in a Bennett Metropolis Monte Carlo calculation to determine free energy differences for small neighboring sized clusters of fixed composition at 298 K. The atom-atom pair potentials consist of Lennard-Jones short-range and Coulombic long-range terms and assume rigid SO 4 2δ-with two unconstrained H δ+ and rigid H 2 O molecules interacting via revised central force (RSL2) potentials. The potential parameters are determined from both ab initio studies and tests of the potential using the statistical mechanical formalism for binary cluster size distributions. In the potential tests, fixed composition free energy differences, δf km,m , for [H 2 O] km [H 2 SO 4 ] m clusters are plotted versus (km + m) -1/3 , and the resulting slope and intercept (in the large cluster regime) are used to extract model dependent binary liquid surface tension and partial vapor pressures at 298 K. The potential parameters are adjusted to obtain approximate agreement with experimental surface tension and partial vapor pressures for k ) 1 and 4 (84% and 57% weight percent H 2 SO 4 , respectively). The free energy differences for m e 15 are presented, together with internal cluster energy contributions, snapshots of cluster structure, and evidence for onset of the large cluster regime near m ) 5. The long-range goals have been to test the free energy difference procedure for studying binary cluster properties and to develop model potentials appropriate for the simulation of small binary clusters at low temperatures characteristic of stratospheric sulfuric acid-water aerosols.

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“…For the binary nucleation, we applied the classical theory for the water-sulfuric acid system with Zeldovich factor modification (cf. Doyle, 1961;Seinfeld and Pandis, 2006, pp. 514-520) but ignored the hydrate formation effect.…”

Section: Aerosol Parcel Model and Simulation Setupmentioning

confidence: 99%

Aerosol nucleation spikes in the planetary boundary layer

2011

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Abstract. Photochemically driven nucleation bursts, which typically occur within a few hours after sunrise, often produce strong aerosol number concentration (ANC) fluctuations. The causes of such ANC spikes were investigated using a detailed aerosol model running in the parcel mode. Two potential mechanisms for the ANC spikes were proposed and simulated. The blocking of actinic flux by scattered clouds can significantly influence new particle production, but this does not cause strong fluctuations in the number of aerosols within sizes greater than the detection limit of our measurements. A more plausible mechanism is the turbulence eddy effect. Strong aerosol nucleation may occur in both updrafts and downdrafts, while the cloud formation at the boundary layer top strongly reduces the number of aerosols. As the number of aerosols is sensitive to turbulence eddy and cloud formation properties, a changing turbulence condition would result in large fluctuations in the evolution of ANC similar to that observed at the surface.

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Self-Nucleation in the Sulfuric Acid-Water System

Cited by 270 publications

References 16 publications

ALADINA – an unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer

ALADINA – an unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer

Monte Carlo Simulations of Small Sulfuric Acid−Water Clusters

Aerosol nucleation spikes in the planetary boundary layer

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