Payday loans
Home Publications Journal Publications

Journal Publications

This section contains all refereed journal publications that have some connection either with the Mace Head Research Station or with members, both present and past, of the Atmospheric Physics Research Cluster at NUI, Galway.

Click on the "Search Document" icon above to find a publication based on the search criteria you create.

 


Documents

Order by : Name | Date | Hits [ Ascendant ]

On the spatial extent and evolution of coastal aerosol plumes On the spatial extent and evolution of coastal aerosol plumes

Date added: 07/31/2002
Date modified: 07/23/2009
Filesize: 757.91 kB

Colin O'Dowd.On the spatial extent and evolution of coastal aerosol plumes, J. Geophys. Res, 107, 10.1029/2001JD000422, 2002.


Abstract


Airborne mapping and pseudo-Lagrangian experiments were conducted in coastal and tidal-induced nucleation plumes along the west coast of Ireland in June 1999. The mapping flights confirmed that the source of the previously reported coastal nucleation events is indeed the tidal zone around the coastline. Additionally, the mapping flights also confirmed that coastal nucleation is typically ubiquitous along the coastline, at least on the Irish coast. Along with the large horizontal extent of coastal nucleation events, these new particles were observed to be mixed up to >1000 m in the vertical despite slightly stable meteorological conditions. On the clean air mapping flight the background particle concentration (r > 1.5 nm) was observed to increase from <1000 cm−3 to >100,000 cm−3, while accumulation mode (r > 50 nm) particle concentration remained constant at approximately 50 cm−3. During a semipolluted mapping flight, concentrations increased from 3000 to >100,000 cm−3 in places. The enhancement in particle concentration was confirmed to be in the size range 1.5–5 nm radius at the start of the nucleation event, while growth into larger sizes was observed later. During this semipolluted event, owing to favorable wind conditions, it was possible to perform a pseudo-Lagrangian experiment in a coastal plume advecting out over the northeast Atlantic. This plume was observed to be >60 km in width and >1000 m in the vertical and was encountered for >250 km off the coast. During this plume evolution the growth of the new particle mode at sizes <5 nm up to sizes >40 nm was observed. After the plume had evolved for 3 hours, increases in scattering coefficients were observed along with significant increases in cloud condensation nuclei concentrations. These results confirm that the spatial extent of tidal-related particle production is regionally significant, and after a few hours, the growth of these recently formed coastal aerosols significantly increase the concentration of radiatively active aerosol particles.

Nolan–Pollak type CN counters in the Vienna aerosol workshop Nolan–Pollak type CN counters in the Vienna aerosol workshop

Date added: 07/31/2002
Date modified: 07/03/2009
Filesize: 321.73 kB

Gras, J.L., J. Podzimek, T.C. O'Connor, K-H Enderle, Nolan-Pollak type CN counters in the Vienna aerosol workshop. Atmos. Res. 62, 239-254, 2002.


Abstract

 

Three standard Nolan-Pollak (N-P) and a modified N-P design condensation nucleus (CN) counters were included in the Vienna Workshop on Intercomparison of Condensation Nuclei and Aerosol Particle counters. These counters came from diverse backgrounds, namely programs in USA, Europe and Australia. In this work, principles of the operation and previous history of calibration of the N-P expansion counter are briefly reviewed and comparisons between the particular counters used in the workshop are presented and discussed. Counting agreement was found to be very good between the N-P counters, typically better than ± 12% for a range of aerosol sizes and compositions from a minimum diameter of 4 nm. The independently calibrated GIV CNC-440 (modified N-P type counter) also agreed well with the N-P counters. The minimum size sensitivity of the N-P counter was examined showing a lower detection limit for insoluble (Ag) particles of around 2.6 ± 0.3 nm diameter.

Meteorological influences on coastal new particle formation Meteorological influences on coastal new particle formation

Date added: 07/31/2002
Date modified: 07/23/2009
Filesize: 1.07 MB
Gerrit de Leeuw, Gerard Kunz, Gintautas Buzorius, and Colin O'Dowd, Meteorological influences on coastal new particle formation, J. Geophys. Res. 107, 10.1029/2001JD001478, 2002.

Abstract


The meteorological situation at the midlatitude coastal station of Mace Head, Ireland, is described based on observations during the New Particle Formation and Fate in the Coastal Environment (PARFORCE) experiments in September 1998 and June 1999. Micrometeorological sensors were mounted near the shore line on a small mast with a height of 3 m and on a 22 m high tower at about 100 m away from the sea. Turbulent fields of wind speed, air temperature, and water vapor were measured. Parameters such as the friction velocity, drag coefficient, kinematic fluxes of heat and water vapor, and various variances were derived. The influence of meteorological parameters on coastal nucleation events is examined, and it is found that the occurrence of nucleation is, more or less, independent of air mass origin and is primarily driven by the occurrence of exposed shore areas during low tide and solar radiation. Micrometeorological influences were also examined in terms of promoting particle production events in this environment. A positive correlation was found between kinematic heat flux and particle production probability. In contrast, a strong negative correlation was found between production probability and both kinematic water vapor fluxes and relative humidity. These results indicate that the occurrence of new particle production events in the coastal zone are most probable during conditions when the shore area containing coastal biota has dried out and the biota are exposed directly to the solar radiation flux and increased shore, or surface, temperatures. These conditions correspond to drying and stressing of the biota, which is known to increase the emissions of biogenic vapors.

Marine aerosol formation from biogenic iodine emissions Marine aerosol formation from biogenic iodine emissions

Date added: 07/31/2002
Date modified: 07/02/2009
Filesize: 373.3 kB

O'Dowd, C.D., J.L. Jimenez, R. Bahreini, R.C. Flagan, J.H. Seinfeld, K. Hämeri, L. Pirjola, M. Kulmala, S.G. Jennigns and T. Hoffmann, Marine aerosol formation from biogenic iodine emissions, Nature, 417, 632-636, 2002.


Abstract


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 budget1, 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 regulation2, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined3, 4. 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.

LIDAR studies of the atmospheric boundary layer and locally generated sea spray aerosol plumes at Ma LIDAR studies of the atmospheric boundary layer and locally generated sea spray aerosol plumes at Ma

Date added: 07/31/2002
Date modified: 07/02/2009
Filesize: 798.06 kB
Gerard Kunz, Gerrit de Leeuw, Colin O'Dowd, Edo Becker.LIDAR studies of the atmospheric boundary layer and locally generated sea spray aerosol plumes at Mace Head. J. Geophys. Res., 107, 10.1029/2001JD001240, 2002.

Abstract

 

A scanning backscatter lidar was used to measure the depth and structure of the coastal atmospheric boundary layer and the evolution of primary aerosol (sea spray) plumes produced by breaking waves during the New Particle Formation and Fate in the Coastal Environment (PARFORCE) campaign at the Mace Head Atmospheric Research Station (Ireland) in September 1998 and in June 1999. The PBL structure was observed to vary from a single-layer well-mixed structure to multilayered structures. Comparison with in situ aircraft measurements of temperature and humidity exhibited good agreement. Using the lidar in the scanning mode allowed two-dimensional profiling over a spatial scale of 10 km, revealing significant primary aerosol plumes produced by breaking waves, particularly in the surf zone and at high wind speeds on the open sea. The initial plume heights were some tens of meters and evolved to hundreds of meters while transported over only a few kilometers from the source. The plumes were traceable to distances of more than 10 km down wind from the source.

Intercomparison of number concentration measurements by various aerosol particle counters Intercomparison of number concentration measurements by various aerosol particle counters

Date added: 07/31/2002
Date modified: 07/02/2009
Filesize: 535.01 kB

Ankilov, A., A Baklanov, M. Colhoun, K-H. Enderle, J. Gras, Yu Jualanov, D. Kaller, A. Linder, A.A. Lushnikov, R. Mavliev, F. McGovern, A. Mirme, T.C. O'Connor, J. Podzimek, O. Prining, G.P. Reischl, R. Rudolf, G.J. Sem, W.W. Szymanski, E. Tamm, A.E. Vrtala, P.E. Wagner, W. Winklmayr and V. Zagaynov, Intercomparison of number concentration measurements by various aerosol particle counters. Atmos. Res. 62, 177-208, 2002.


Abstract

 

Total aerosol particle number concentrations, as measured by means of 16 different measurement systems, have been quantitatively compared during an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (ICCP-IUGG). The range of measuring instruments includes Pollak counters (PCO) in use already for several decades, presently available commercial particle counters, as well as laboratory prototypes. The operation of the instruments considered was based on different measurement principles: (1) adiabatic expansion condensation particle counter, (2) flow diffusion condensation particle counter, (3) turbulent mixing condensation particle counter, (4) laser optical particle counter, and (5) electrostatic particle measurement system. Well-defined test aerosols with various chemical compositions were considered: DEHS, sodium chloride, silver, hydrocarbons, and tungsten oxide. The test aerosols were nearly monodispersed with mean particle diameters between 4 and 520 nm, the particle number concentrations were varied over a range from about 4 × 101 to 7 × 106 cm-3. A few measurements were performed with two-component aerosol mixtures. For simultaneous concentration measurements, the various instruments considered were operated under steady state conditions in a linear flow system. A series of at least 10 single concentration measurements was performed by each individual instrument at each set of test aerosol parameters. The average of the concentration data measured by the various instruments was defined as a common reference. The number concentrations obtained from the various instruments typically agreed within a factor of about two over the entire concentration range considered. The agreement of the measured concentrations is notable considering the various different measurement principles applied in this study, and particularly in view of the broad range of measurement instruments used. Significant deviations and nonlinear response were observed only in a few cases and are possibly related to calibration errors. For certain conditions, a dependence of aerosol counter response on particle composition has been found. The scatter of the number concentrations obtained from each individual instrument during measurements with constant test aerosol typically did not exceed 20% to 25%. At concentrations below 103 cm-3, however, several of the instruments, including electrostatic particle measurement systems, tend to show increased experimental scatter.

Importance of organic and black carbon in atmospheric aerosols at Mace Head, on the West Coast of Ireland (53°19′N, 9°54′W) Importance of organic and black carbon in atmospheric aerosols at Mace Head, on the West Coast of Ireland (53°19′N, 9°54′W)

Date added: 07/31/2002
Date modified: 07/24/2009
Filesize: 146.78 kB

Kleefeld, S., Hoffer, A., Krivacsy, and Jennings, S.G., 2002. Importance of organic and black carbon at Mace Head, on the west coast of Ireland (53 019’N, 9 054’W), Atmos. Environ., 36, pp. 4479-4490.


Abstract


The mass concentrations of total organic carbon (TC) and its chemical fractions, water-soluble organic carbon (WSOC), water-insoluble organic carbon (WISOC), and black carbon (BC), were determined in marine aerosols, which were collected during the period July 1998-September 1999 at the Mace Head Atmospheric Research Station on the west coast of Ireland. In addition, mass concentrations of major inorganic ions, like non-sea-salt (NSS) sulphate, and mass concentrations of dicarboxylic acids have been measured separately within the water-soluble aerosol fraction. The aerosol samples were classified into clean marine aerosol samples and modified marine aerosol samples according to the origin of air masses arriving at Mace Head, and using BC as a tracer for anthropogenic pollution. Following this classification, the data set was further divided into samples taken during summertime and wintertime. An average TC mass concentration of 591±75 ng/m3 was determined for all aerosol samples taken at Mace Head. WSOC was found to be the dominating fraction in modified marine aerosol samples, followed by WISOC and BC, whereas in clean marine aerosol samples WISOC was the main fraction, followed by WSOC, and BC. A comparison of the mass concentration of the water-soluble organic matter to the main water-soluble inorganic component, NSS sulphate, gave an average ratio of 0.72±0.10, which increased to 1.59±0.23 when considering solely clean marine aerosol samples. The dominating dicarboxylic acid found in carbonaceous aerosols at Mace Head was oxalic acid, followed by malonic acid. Both diacids were responsible for about 14±2% of the WSOC (in terms of carbon).

Gas-Aerosol Relationships of OH, H2SO4, and MSA Observations in the Coastal Marine Boundary Layer at Mace Head Gas-Aerosol Relationships of OH, H2SO4, and MSA Observations in the Coastal Marine Boundary Layer at Mace Head

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 542.87 kB
H. Berresheim, T. Elste, H.G. Tremmel, C O'Dowd, A.Allen, H.C. Hansson, K Rosman, M. dal Maso, J. Makela, and Markku Kulmala. Gas-Aerosol Relationships of OH, H2SO4, and MSA: Observations in the Coastal Marine Boundary Layer at Mace Head, Ireland. J. Geophys. Res., 107, 10.1029/2000JD000229, 2002.

Abstract

 

Atmospheric concentrations of gaseous sulfuric acid (H2SO4), methane sulfonic acid (MSA), and hydroxyl radicals (OH) were measured by chemical ionization mass spectrometry (CIMS) during the second New Particle Formation and Fate in the Coastal Environment (PARFORCE) campaign in June 1999 at Mace Head, Ireland. Overall median concentrations in marine background air were 1.5, 1.2, and 0.12 × 106 cm−3, respectively. H2SO4 was also present at night indicating significant contributions from nonphotochemical sources. A strong correlation was found between daytime OH and H2SO4 levels in clean marine air suggesting a fast local production of H2SO4 from sulfur precursor gases. Steady state balance calculations of ambient H2SO4 levels agreed with measured concentrations if either very low H2SO4 sticking coefficients (0.02–0.03) or sources in addition to the SO2 + OH reaction were assumed. Overall, variations in ambient H2SO4 levels showed no correlation with either the tidal cycle or ultrafine particle (UFP) concentrations. However, on particular days an anticorrelation between H2SO4 and UFP levels was occasionally observed providing evidence for the contribution of H2SO4 to new particle formation and/or particle growth. Gaseous MSA concentrations were inversely correlated with dew point temperature reflecting a highly sensitive gas-particle partitioning equilibrium of this compound. The present observations seriously question the general use of MSA as a conservative tracer to infer the relative production yield of H2SO4 from dimethylsulfide (DMS) oxidation. MSA/H2SO4 concentration ratios typically ranged between 0.06 and 1.0 in marine air at ground level. Measured diel OH profiles showed a significant deviation from concurrent variations of the ozone photolysis frequency. They also showed up to 1 order of magnitude lower values compared to OH concentrations calculated with a simple photochemical box model. These differences were most pronounced during particle nucleation events occurring on sunny days around noon and at low tide. The present results suggest that both the oxidation capacity and the particle formation potential in the coastal boundary layer were significantly affected by reactions of unknown compounds prevailing in this type of environment.

First experimental evidence of new particle formation from organic vapours over forests First experimental evidence of new particle formation from organic vapours over forests

Date added: 07/31/2002
Date modified: 07/01/2009
Filesize: 97.37 kB

O'Dowd, C.D. K. Hämeri, P. Aalto, and M. Kulmala, First experimental evidence of new particle formation from organic vapours over forests, Nature, 416, 497-498, 2002.


Abstract


Aerosol particles produced over forested areas may affect climate by acting as nuclei for cloud condensation, but their composition (and hence the chemical species that drive their production) remains an open question. Here we show, to our knowledge for the first time, that these newly formed particles (3–5 nm in diameter) are composed primarily of organic species, such as cis-pinonic acid and pinic acid, produced by oxidation of terpenes in organic vapours released from the canopy

Experimental studies of the effect of rough surfaces and air speed on aerosol deposition in a test chamber Experimental studies of the effect of rough surfaces and air speed on aerosol deposition in a test chamber

Date added: 07/31/2002
Date modified: 07/01/2009
Filesize: 915.07 kB

Lai, A.C.K., Byrne and AJH Goddard. Experimental studies of the effect of rough surfaces and air speed on aerosol deposition in a test chamber. Aerosol Science and Technology, 36: 973-982, 2002.


Abstract

 

Understanding the fate of particles indoors is important for human health assessment because deposited particles, unless resuspended, cannot be inhaled. To complement studies in real buildings, where control of variables is often difficult, an experimental test chamber facility (8 m3) was designed to study particle deposition under well-stirred conditions using monodisperse tracer aerosol particles in the range of 0.7 to 5.4 mum. The use of neutron-activatable tracers facilitated simultaneous surface sampling and aerosol concentration decay measurements.

 

Aerosol deposition on both smooth surfaces and regular arrays of three-dimensional roughness elements under 3 different airflow speeds was investigated in the test chamber.It was expected that the texture of the chamber surface would significantly influence particle deposition, but some counterintuitive results were observed: under the lowest airflow condition and for the smallest particle size, particle deposition onto rough samples was found to be less than on the corresponding smooth surfaces.

 

The ratio of particle deposition on rough surfaces relative to smooth surfaces increased with particle size and magnitude of airflow. For the largest particle size and airflow speed, particle deposition on the rough surfaces exceeded that on the smooth surfaces by a factor of 3.

Evaluating measurements new particle concentrations, source rates and spatial scales during .. Evaluating measurements new particle concentrations, source rates and spatial scales during ..

Date added: 07/31/2002
Date modified: 07/24/2009
Filesize: 863.78 kB

Kaarle Hameri , Colin O'Dowd, Claudia Hoell, Evaluating measurements new particle concentrations, source rates and spatial scales during coastal nucleation events using condensation particle counters. ,JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 107, NO. D19, 8101, doi:10.1029/2001JD000411, 2002


Abstract


Condensation particle counters (CPCs), used to examine particle production in the coastal environment, are evaluated for their ability to differentiate ultrafine sizes between 3 and 10 nm, along with their ability to count high total particle number concentrations encountered during coastal nucleation events. Four ultrafine particles counters, with a 3 nm detection limit, were deployed in a spatial array comprising a triangular distribution with nodes approximately 100 m apart (two at 3 m height, one at 10 m). A fourth node was deployed at 20 m. The 10 m and 20 m node comprised additional CPCs with detection limits of 5 and 10 nm. Size cutoff efficiency calibrations were performed in the field, and all CPCs were found to be within the manufacturer's specifications. During the nucleation events it was found that peak particle concentrations of the order of 180,000 cm−3 were encountered, and as a result, coincidence calibrations were also performed in the laboratory. It was found that, at concentrations over 100,000 cm−3, the CPCs significantly underestimated the true concentrations by a factor of about 5–6. Total particle concentrations were also measured using a 30-times dilution system and an ultrafine CPC, along with integrated total concentration derived from the ultrafine Differential Mobility Particle Sizer (DMPS). Comparison of laboratory-derived corrections for coincidence and both the diluted CPC total concentrations and DMPS concentrations revealed very good agreement and confirmed that peak particle concentrations during coastal nucleation bursts result in new particle concentrations as high as 1.2 × 106 cm−3. The DMPS total concentration was somewhat lower than the diluted CPC concentration, suggesting that the recommended method of measuring such high concentrations is to dilute the sample significantly. The lower concentrations from the DMPS are partially due to the 10 min integration time being insufficient to resolve peaks seen by the CPC operated at 1 Hz. Taking the corrected concentrations in account, 3 nm particle source rates were calculated to be >105 cm−3 s−1. The spatial array of CPCs revealed that within the general coastal nucleation plume, there are numerous microplumes with spatial scales of the order of 10–100 m when sampling is conducted near the source region. Further from the source region these microplumes merge into the general coastal plume.

Continuous observations of carbon dioxide at Mace Head, Ireland from 1995 to 1999 and its net European ecosystem exchange Continuous observations of carbon dioxide at Mace Head, Ireland from 1995 to 1999 and its net European ecosystem exchange

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 376.57 kB
Derwent, R.G., Ryall, D.B., Manning, A.J., Simmonds, P.G., O’Doherty, S., Biraud, s., Ciais, P., Ramonet, M., and Jennings, S.G., 2002. Continuous observations of carbon dioxide at Mace Head, Ireland from 1995 to 1999 and its net European ecosystem exchange, Atmos. Environ., 36, pp. 2799 – 2807.

Abstract


A 5-yr record of continuous high-frequency carbon dioxide CO2 observations over the 1995-1999 period for the Mace Head Atmospheric Research Station has been examined to reveal a complex interplay between local- and regional-scale sources and sinks. During the winter months, an additional CO2 source, over and above fossil fuel combustion, is required to support the observed concentrations of CO2 in European regionally polluted air masses. During the summer months, an additional CO2 sink is required. Over the entire study period, the additional net European ecosystem exchange source-sink required is -0.36+/-0.4Gtonne Cyr-1.

Coastal new particle formation Environmental conditions and aerosol physico-chemical characteristics during nucleation bursts Coastal new particle formation Environmental conditions and aerosol physico-chemical characteristics during nucleation bursts

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 1.31 MB
Colin D. O'Dowd, Kaarle Hämeri, Jyrki Mäkelä, Minna Väkeva, Pasi Aalto, Gerrit de Leeuw, Gerard Kunz, Harald Berresheim, Hans-Christen Hansson, Edo Becker, Andrew G. Allen, Roy M. Harrion, Christoph Kleefeld, Michael Geever, S. Gerard Jennings, Harald Berresheim, and Markku Kulmala.Coastal new particle formation: Environmental conditions and aerosol physico-chemical characteristics during nucleation bursts. J. Geophys. Res. 107, 10.1029/2000JD000206, 2002.

Abstract


Nucleation mode aerosol was characterized during coastal nucleation events at Mace Head during intensive New Particle Formation and Fate in the Coastal Environment (PARFORCE) field campaigns in September 1998 and June 1999. Nucleation events were observed almost on a daily basis during the occurrence of low tide and solar irradiation. In September 1998, average nucleation mode particle concentrations were 8600 cm−3 during clean air events and 2200 cm−3 during polluted events. By comparison, during June 1999, mean nucleation mode concentrations were 27,000 cm−3 during clean events and 3350 cm−3 during polluted conditions. Peak concentrations often reached 500,000–1,000,000 cm−3 during the most intense events and the duration of the events ranged from 2 to 8 hours with a mean of 4.5 hours. Source rates for detectable particle sizes (d > 3 nm) were estimated to be between 104 and 106 cm−3 s−1 and initial growth rates of new particles were as high as 0.1–0.35 nm s−1 at the tidal source region. Recently formed 8 nm particles were subjected to hygroscopic growth and were found to have a growth factor of 1.0–1.1 for humidification at 90% relative humidity. The low growth factors implicate a condensable gas with very low solubility leading to detectable particle formation. It is not clear if this condensable gas also leads to homogeneous nucleation; however, measured sulphuric acid and ammonia concentration suggest that ternary nucleation of thermodynamically stable sulphate clusters is still likely to occur. In clear air, significant particle production (>105 cm−3) was observed with sulphuric acid gas-phase concentration as low as 2 × 106 molecules cm−3 and under polluted conditions as high as 1.2 × 108 molecules cm−3.

Biogenic iodine emissions and identification of end products in coastal ultrafine particles during nucleation bursts Biogenic iodine emissions and identification of end products in coastal ultrafine particles during nucleation bursts

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 703.95 kB
J.M. Mäkelä, T. Hoffmann, C. Holzke, M. Väkevä, T. Suni, T. Mattila, P.P. Aalto, U. Tapper, E.I. Kauppinen and C.D. O'Dowd, Biogenic iodine emissions and identification of end products in coastal ultrafine particles during nucleation bursts. J. Geophys. Res. 107, 10.1029/2001JD000580,

Abstract


Ultrafine particles sampled during new particle formation bursts observed in the coastal zone were studied with transmission electron microscopy (TEM) and elemental analysis using energy-dispersive X ray (EDX). It was observed that both iodine and sulphur were present in the new particles with diameter below 10 mn. Gaseous emissions of halogen compounds from seaweeds were also measured at the same location during low-tide particle nucleation episodes. Based on the presence of iodine in the particle phase during low-tide nucleation bursts, and the significant emission of iodine compounds from the seaweeds during these periods, it is apparent that part of the biogenic iodine species emitted from the seaweeds end up in the ultrafine particulate phase. It was not possible to quantitatively determine the iodine content in the particles; however, in most cases the relative contribution from iodine and sulphate was similar, while some cases indicated no sulphate. On larger sized particles the contribution of sulphate was significantly higher than iodine. It appears that the condensable species leading to the appearance of new particles in the coastal atmosphere is an iodine species. Whether or not this iodine species also participates in the nucleation of new stable clusters could not be completely verified.

Aerosol formation during PARFORCE: Ternary nucleation of H2SO4, NH3 and H2O Aerosol formation during PARFORCE: Ternary nucleation of H2SO4, NH3 and H2O

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 354.52 kB
Markku Kulmala, Pekka Korhonen, Ismo Napari, Robert Jansson, Harald Berresheim, and Colin O'Dowd, Aerosol formation during PARFORCE: Ternary nucleation of H2SO4, NH3 and H2O, J. Geophys. Res., 107, 10.1029/2001JD000900, 2002.

Abstract


A new version of a ternary nucleation (sulphuric acid-ammonia-water) model based on classical nucleation theory, but with an improved ability to predict nucleation rates over a larger temperature range (258–303 K) compared with previous work, is presented. The modeled nucleation rates are given as a function of temperature and ambient acid and ammonia concentrations. For the first time the predicted ternary nucleation rates are compared to the observed particle production rates using measured ambient sulphuric acid and ammonia concentrations as input data. The ambient gas concentrations were measured simultaneously to aerosol formation rates during the 1999 New Particle Formation and Fate in the Coastal Environment (PARFORCE) coastal field campaign at Mace Head. According to the results, daytime ambient acid and ammonia concentrations were significantly higher than required by model calculations to induce the formation of new particles by homogeneous ternary nucleation. However, binary nucleation of sulphuric acid-water molecules is not able to predict new particle formation since the binary nucleation rate is far too small. We conclude that all particle formation events observed at coastal sites can be initiated by ternary nucleation of sulphuric acid, ammonia, and water vapor. However, related studies illustrate that ambient sulphuric acid concentrations are, nevertheless, insufficient to explain observed rapid growth of particles from 1 to 3 nm sizes which can be detected by current instrumentation.

A model prediction of the yield of CCN from coastal nucleation events A model prediction of the yield of CCN from coastal nucleation events

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 352.77 kB
Liisa Pirjola, Colin O'Dowd, Markku Kulmala, A model prediction of the yield of CCN from coastal nucleation events, J. Geophys. Res., 107, 10.1029/2000JD000213, 2002.

Abstract


The formation and evolution of new particles during coastal nucleation events are examined using the aerosol dynamic and gas-phase chemistry model AEROFOR2. Coastal regions are known to be a strong source of natural aerosol particles and are also strong sources of biogenic vapors which can condense onto aerosol particles, thus resulting in particle growth. A number of model simulations were performed to determine the instantaneous nucleation rate along with the source rate of a generic biogenic vapor leading to the observed particle size distributions which indicate the rapid appearance of ∼105–106 cm−3 nucleation mode particles in this environment. Model calculations suggest values of 3 × 105 cm−3 s−1 to 3 × 106 cm−3 s−1 for the instantaneous nucleation rate and a value of 5 × 107 cm−3 s−1 for the condensable vapor source rate in order to reproduce the observed concentrations. A significant fraction of these new particles survive to grow into cloud condensation nuclei (CCN) sizes for supersaturations typically encountered in boundary layer clouds during subsequent evolution over 3 days under clear-sky conditions, thus contributing to the indirect radiative effect of aerosols. The amount of CCN is mainly affected by coagulation between particles and condensation of the biogenic vapor and, to a lesser extent, by condensation of sulphuric acid formed by DMS oxidation. In all simulated cases, an increase of more than 100% in CCN concentration, for supersaturations >0.35% was observed.

A dedicated study of new particle formation and fate in the coastal environment (PARFORCE) Overview of objectives and initial achievements A dedicated study of new particle formation and fate in the coastal environment (PARFORCE) Overview of objectives and initial achievements

Date added: 07/31/2002
Date modified: 07/27/2009
Filesize: 448.25 kB
C. D. O'Dowd, K. Hämeri, J.M. Mäkelä, M. Kulmala, L. Pirjola, H. Berresheim, S.G. Jennings, H-C Hansson, G. de Leeuw, A.G. Allen, C.N. Hewitt, A. Stroh, and Y. Viisanen. A dedicated study of new particle formation and fate in the coastal environment (PARFORCE): Overview of objectives and initial achievements. J. Geophys. Res. 107, 10.1029/2001000555, 2002.

Abstract


A dedicated study into the formation of new particles, New Particle Formation and Fate in the Coastal Environment (PARFORCE), was conducted over a period from 1998 to 1999 at the Mace Head Atmospheric Research Station on the western coast of Ireland. Continuous measurements of new particle formation were taken over the 2-year period while two intensive field campaigns were also conducted, one in September 1998 and the other in June 1999. New particle events were observed on ∼90% of days and occurred throughout the year and in all air mass types. These events lasted for, typically, a few hours, with some events lasting more than 8 hours, and occurred during daylight hours coinciding with the occurrence of low tide and exposed shorelines. During these events, peak aerosol concentrations often exceeded 106 cm−3 under clean air conditions, while measured formation rates of detectable particle sizes (i.e., d > 3 nm) were of the order of 104–105 cm−3 s−1. Nucleation rates of new particles were estimated to be, at least, of the order of 105–106 cm−3 s−1 and occurred for sulphuric acid concentrations above 2 × 106 molecules cm−3; however, no correlation existed between peak sulphuric acid concentrations, low tide occurrence, or nucleation events. Ternary nucleation theory of the H2SO4-H2O-NH3 system predicts that nucleation rates far in excess of 106 cm−3 s−1 can readily occur for the given sulphuric acid concentrations; however, aerosol growth modeling studies predict that there is insufficient sulphuric acid to grow new particles (of ∼1 nm in size) into detectable sizes of 3 nm. Hygroscopic growth factor analysis of recently formed 8-nm particles illustrate that these particles must comprise some species significantly less soluble than sulphate aerosol. The nucleation-mode hygroscopic data, combined with the lack of detectable VOC emissions from coastal biota, the strong emission of biogenic halocarbon species, and the fingerprinting of iodine in recently formed (7 nm) particles suggest that the most likely species resulting in the growth of new particles to detectable sizes is an iodine oxide as suggested by previous laboratory experiments. It remains an open question whether nucleation is driven by self nucleation of iodine species, a halocarbon derivative, or whether first, stable clusters are formed through ternary nucleation of sulphuric acid, ammonia, and water vapor, followed by condensation growth into detectable sizes by condensation of iodine species. Airborne measurements confirm that nucleation occurs all along the coastline and that the coastal biogenic aerosol plume can extend many hundreds of kilometers away from the source. During the evolution of the coastal plume, particle growth is observed up to radiatively active sizes of 100 nm. Modeling studies of the yield of cloud-condensation nuclei suggest that the cloud condensation nuclei population can increase by ∼100%. Given that the production of new particles from coastal biogenic sources occurs at least all along the western coast of Europe, and possibly many other coastlines, it is suggested that coastal aerosols contribute significantly to the natural background aerosol population.

The Relative Contribution of sub and super micron particles to aerosol light scattering .. The Relative Contribution of sub and super micron particles to aerosol light scattering ..

Date added: 07/31/2002
Date modified: 07/08/2009
Filesize: 905.05 kB

Christoph Kleefeld, Colin O'Dowd, Sarah O'Reilly, S. Gerard Jennings, Pasi Alto, Edo, Becker, Gerard Kunz, Gerrit de Leeuw.The Relative Contribution of sub and super micron particles to aerosol light scattering in the marine boundary layer (MBL), J. Geophys. Res., 107, 10.1029/2000JD000262, 2002.


Abstract

 

Measurements of the aerosol light scattering coefficient (ssp) at a wavelength of l = 550 nm were conducted at a coastal atmospheric research station in the east Atlantic Ocean during June 1999. Size distribution measurements between diameters of 3 nm and 40 mm (at ambient humidity) were used to derive scattering coefficients from Mie theory. The calculated scattering coefficients were about a factor of 7.4 higher than the measured scattering coefficients. The discrepancy was explained by a reduced cutoff of the sampling system at particle diameters between 6 and 8 mm, dependent on wind speed. The calculated aerosol scattering was about 1 order of magnitude higher than previously reported measurements in the MBL and is attributed to supermicrometer particles at sizes d > 10 mm dominating aerosol scattering. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 3359 Meteorology and  Atmospheric Dynamics: Radiative processes; KEYWORDS: light scattering, sea-salt aerosol, marine boundary layer, particle size distribution, Mie theory

 

Modelling of indoor exposure to nitrogen dioxide in the UK Modelling of indoor exposure to nitrogen dioxide in the UK

Date added: 08/31/2001
Date modified: 07/03/2009
Filesize: 346.84 kB

Dimitroulopoulou, C., Ashmore, M.R., Byrne, M.A. and Kinnersley, R.P. Modelling of indoor exposure to nitrogen dioxide in the UK. Atmos. Environ., 35, 269-279, 2001.


Abstract


A dynamic multi-compartment computer model has been developed to describe the physical processes determining indoor pollutant concentrations as a function of outdoor concentrations, indoor emission rates and building characteristics. The model has been parameterised for typical UK homes and workplaces and linked to a time-activity model to calculate exposures for a representative homemaker, schoolchild and office worker, with respect to NO2. The estimates of population exposures, for selected urban and rural sites, are expressed in terms of annual means and frequency of hours in which air quality standards are exceeded. The annual mean exposures are estimated to fall within the range of 5-21 ppb for homes with no source, and 21-27 ppb for homes with gas cooking, varying across sites and population groups. The contribution of outdoor exposure to annual mean NO2 exposure varied from 5 to 24%, that of indoor penetration of outdoor air from 17 to 86% and that of gas cooking from 0 to 78%. The frequency of exposure to 1 h mean concentrations above 150 ppb was very low, except for people cooking with gas.

Sources and source variations for aerosol at Mace Head, Ireland Sources and source variations for aerosol at Mace Head, Ireland

Date added: 08/07/2001
Date modified: 07/23/2009
Filesize: 575.5 kB

JR Huang S., Arimoto R., Rahn K. A. (2000) Sources and source variations for aerosol at Mace Head, Ireland. Atmos. Environ. 35, 1421-1437.


Abstract


The sources and source variations for aerosol at Mace Head, Ireland, were studied by applying positive matrix factorization (PMF), a variant of factor analysis, to a 5-yr data set for bulk aerosol. Signals for the following six sources were evident year round: (1) mineral dust, (2) sea salt, (3) general pollution, (4) a secondary SO42--Se signal that is composed of both natural (marine) and pollution (coal) components, (5) ferrous industries, (6) and a second marine (possibly biogenic) source. Analyses of seasonally stratified data suggested additional sources for iodine and oil emissions but these were present only in certain seasons, respectively. The marine signal is particularly strong in winter. The main pollution transport from Europe to Mace Head occurs in May, but the influence of continental European emissions is evident throughout the year. Mineral aerosol evidently follows a transport pathway similar to that of pollution aerosol, i.e., recirculation via the westerlies brings pollutants mixed with dust to the site from nearby land, i.e., Ireland, the United Kingdom, and the Belgium, Netherlands, and Luxemburg (Benelux) region, with some inputs from Scandinavia, Western Europe, Eastern Europe, and even the Mediterranean region. Compared with Bermuda, aerosol at Mace Head has stronger marine sources (especially marine-derived secondary SO42- and Se) but weaker crustal and oil signals. Transport across the North Atlantic, especially in winter, cannot be ruled out.

Estimating source regions of European emissions of trace gases from observations at Mace Head Estimating source regions of European emissions of trace gases from observations at Mace Head

Date added: 08/07/2001
Date modified: 07/27/2009
Filesize: 1004.2 kB

D.B. Ryall, R.G. Derwent, P.G. Simmonds, and S.J.O'Doherty. Estimating source regions of European emissions of trace gases from observations at Mace Head. Atmos. Environ. Vol 35, (2001), 2,507-25,23.


Abstract


A technique is described for identifying probable source locations for a range of greenhouse and ozone-depleting trace gases from the long-term measurements made at Mace Head, Ireland. The Met. Office's dispersion model NAME is used to predict concentrations at Mace Head from all possible sources in Europe, then source regions identified as those which consistently lead to elevated concentrations at Mace Head. Estimates of European emissions and their distribution are presented for a number of trace gases for the period 1995-1998. Estimated emission patterns are realistic, given the nature and varied applications of the species considered. The results indicate that whilst there are limitations, useful information about source distribution can be extracted from continuous measurements at a remote site. It is probable that much improved estimates could be derived if observations were available from a number of sites. The ability to assess emissions has obvious implications in monitoring compliance with internationally agreed quota and protocols.

 

Determination of biogenic volatile organic compounds (C8–C16) in the coastal atmosphere at Mace Determination of biogenic volatile organic compounds (C8–C16) in the coastal atmosphere at Mace

Date added: 08/07/2001
Date modified: 07/27/2009
Filesize: 357.39 kB

Determination of biogenic volatile organic compounds (C8 - C16) in the coastal atmosphere at Mace Head, Ireland (2001) J. Sartin, C.J. Halsall, B. Davison, S. Owen and C.N. Hewitt, Analytica Chimica Acta, 428, 61-72


Abstract


A methodology describing the sampling and analysis of biogenic volatile organic compounds (VOCs) in ambient coastal air is presented. Air samples were collected during a field campaign (September 1998) at Mace Head on the west coast of Ireland. In addition, air samples from seaweed enclosures were taken to assess the VOC source potential of macro-algae at low tide. VOC identification was confirmed using GC-MS and an n-alkane retention index, with quantification carried out using GC-FID. A suite of compounds (C8-C16) were routinely quantified; these included a series of n-alkanes (C11-C16) and oxygenated hydrocarbons (C8-C14). Their mixing ratios in coastal air ranged from <10-400 parts per trillion (pptv). The most abundant oxygenates included 2-ethyl-1-hexanol (mean = 175 pptv) and two ubiquitous ketones (geranyl acetone and 6-methyl-5-hepten-2-one) with average mixing ratios of 123 and 28 pptv, respectively. Air mass back trajectories indicated higher levels of the oxygenates when air flow was off the land (easterly continental) rather than from the ocean, although the opposite was observed for the n-alkanes. Mixing ratios of the n-alkanes (>C12) were significantly higher in the seaweed enclosure air than in ambient air, suggesting seaweed to be a source of long chain n-alkanes. Oxygenates, however, did not show a significant difference between enclosure and ambient air. Unlike studies carried out in the vicinity of woodlands, no monoterpenes or sesquiterpenes were detected in this study.

 

Comparisons of coarse-mode aerosol nitrate and ammonium at two polluted coastal sites Comparisons of coarse-mode aerosol nitrate and ammonium at two polluted coastal sites

Date added: 08/07/2001
Date modified: 07/27/2009
Filesize: 413.74 kB

Yeatman S.G., Spokes L.J., Jickells T.D. (2001) Comparison of coarse mode aerosol nitrate and ammonium at two polluted coastal sites. Atmospheric Environment 35 1321-1335.


Abstract


Direct atmospheric fixed-nitrogen deposition can contribute to eutrophication in coastal and estuarine waters and can be enhanced by heterogeneous reactions between gaseous atmospheric nitrogen species and aerosol sea salt, which increase deposition rates. Size-segregated aerosol samples were collected from two coastal sites: Weybourne, England and Mace Head, Ireland. Major-ion aerosol concentrations were determined and temporal patterns were interpreted with the use of air-mass back trajectories. Low levels of terrestrially derived material were seen during periods of clean, onshore flow, with respective concentration ranges for nitrate and ammonium of 0.47-220 and below detection limit to 340 nmol/m3. Corresponding levels of marine derived material during these periods were high, with sodium concentrations ranging from 39 to 1400 nmol/m3. Highest levels of terrestrially derived material were seen during polluted, offshore flow, where the air had passed recently over strong source regions of the UK and northern Europe, with concentration ranges of nitrate and ammonium of 5.6-790 and 9.7-1000 nmol/m3, respectively. During polluted flow ∼40-60% of the nitrate was found in the coarse mode (>1 μm diameter) and under clean marine conditions almost 100% conversion was seen. In addition, the data suggests strong evidence for dissolution, coagulation processes that also shift nitrate to the coarse mode. Furthermore, such processes are thought also to give rise to the size-shifting of aerosol ammonium, since significant coarse-mode fractions of this species (∼19-45%) were seen at both sites. A comparison of the relative importance of nitrate and ammonium in the overall dry deposition of inorganic fixed-nitrogen at each site indicates that at Weybourne the mass-weighted dry deposition velocity of the latter is around double that seen at Mace Head with its resultant contribution to the overall inorganic nitrogen dry flux exceeding that of nitrate.

 

Can the study of nitrogen isotopic composition in size-segregated aerosol nitrate and ammonium Can the study of nitrogen isotopic composition in size-segregated aerosol nitrate and ammonium

Date added: 08/07/2001
Date modified: 07/27/2009
Filesize: 186.81 kB

S.G. Yeatman, L.J. Spokes, P.F. Dennis, T.D. Jickells, Can the study of nitrogen isotopic composition in size-segregated aerosol nitrate and ammonium be used to investigate atmospheric processing mechanisms?, Atmospheric Environment 35 (2001) 1337}1345


Abstract


Atmospheric fixed-nitrogen deposition can contribute to eutrophication in coastal and estuarine waters. Stable nitrogen isotope data can provide important information regarding the sources and processing of atmospheric fixed-nitrogen species and is thus important in controlling eutrophication. Size-segregated aerosol samples were collected from two coastal sites: Weybourne, England and Mace Head, Ireland and also aboard the RRS Challenger in the Eastern Atlantic Ocean. Aerosol concentrations of ammonium and nitrate were determined prior to δ15N isotopic analysis. The isotopic enrichment factor, ε, was calculated for both the species by subtracting the respective δ15N values of the coarse-mode fraction (>1 μm diameter) from those of the fine-mode fraction (<1 μm diameter). Variations in this parameter were observed as weak functions of the percentage of each species in the coarse mode and of meteorological condition. As a result, the presence of two different size-shift processes (dissociation/gas scavenging and dissolution/coagulation) is proposed, consistent with similar arguments based upon major-ion data obtained from the same suite of samples. Dissolution/coagulation processes appear to exhibit negative isotopic enrichment factors whereas dissociation/gas scavenging processes appear to exhibit positive enrichment factors, suggesting that they may be reversible and thermodynamically driven. In offshore-flowing air masses just entering the marine environment, transferral of nitrate to the coarse mode by initial dissociation of NH4NO3 followed by scavenging of the HNO3 produced appears to be significantly more important than in samples of onshore, marine dominated air. In contrast, ammonium appears to be transferred to the coarse mode during offshore flow largely via the dissolution and coagulation of aerosol ammonium, nitrate and sulphate-containing species. During onshore flow, the uptake of gaseous NH3, arising from the continued dissociation of NH4NO3, seems to become increasingly important.

 

The Evolution of Condensation Nucleus Counters The Evolution of Condensation Nucleus Counters

Date added: 08/07/2001
Date modified: 07/07/2009
Filesize: 7.48 MB
O'Connor Tom,  The Evolution of Condensation Nucleus Counters , The Aerosol Society Newsletter, pg 5-8, March 2001

Abstract

 


Tropospheric concentrations of the chlorinated solvents, tetrachloroethene and trichloroethene, Tropospheric concentrations of the chlorinated solvents, tetrachloroethene and trichloroethene,

Date added: 08/07/2001
Date modified: 07/23/2009
Filesize: 573.98 kB

Dimmer, C.H., McCulloch, A., Simmonds, P.G., Nickless, G. Bassford, M.R. and Smythe-Wright, D. Tropospheric concentrations of the chlorinated solvents, tetrachloroethene, and trichloroethene, measured in the remote Northern Hemisphere, Atmospheric Environment, 35, 2001, 1171-1182.


Abstract


A fully automated twin ECD gas chromatograph system with sample enriching adsorption-desorption primary stage was deployed on two field campaigns - Ny-Ålesund, Svalbard, Arctic Norway (July-September 1997), and the RRS Discovery CHAOS cruise of the northeast Atlantic (April-May 1998). Concentrations of an extensive set of halocarbons were detected at hourly intervals at pptv levels. We present the results obtained for the chlorinated solvents, tetrachloroethene (PCE) and trichloroethene (TCE). Average baseline PCE and TCE concentrations of 1.77 and 0.12 pptv, respectively, were recorded in Ny-Ålesund. During pollution incidences, concentrations rose to 5.61 (PCE) and 3.18 pptv (TCE). The cruise data showed average concentrations ranging from 4.26 (PCE) and 1.66 pptv (TCE) for air masses originating over the North Atlantic and Arctic open oceans, to maxima of 15.59 (PCE) and 17.51 pptv (TCE) for polluted air masses from Northern Europe. The data sets emphasise the difficulties in defining remote sites for background tropospheric halocarbon measurements, as Ny-Ålesund research station proved to be a source of tetrachloroethene. The data also suggest possible oceanic emissions of trichloroethene in the sub-tropical ocean.

 

Atmospheric mercury distribution in Northern Europe and in Atmospheric mercury distribution in Northern Europe and in

Date added: 08/06/2001
Date modified: 07/27/2009
Filesize: 238.69 kB

I. Wangberg, J. Munthe, N. Pirrone, A. Iverfeldt, E. Bahlman, P. Costa, R. Ebinghaus, X. Feng, R. Ferrara, K. Gardfeldt, H. Kock, E. Lanzillotta, Y. Mamane, F. Mas, E. Melamed, Y. Osnat, E. Prestbo, J. Sommar, S. Schmolke, G. Spain, F. Sprovieri, G. Tuncel, Atmospheric mercury distribution in Northern Europe and in the Mediterranean region, Atmospheric EnvironmentVolume 35, Issue 17, , June 2001, Pages 3019-3025.


Abstract


Mercury species in air have been measured at five sites in Northwest Europe and at five coastal sites in the Mediterranean region during measurements at four seasons. Observed concentrations of total gaseous mercury (TGM), total particulate mercury (TPM) and reactive gaseous mercury (RGM) were generally slightly higher in the Mediterranean region than in Northwest Europe. Incoming clean Atlantic air seems to be enriched in TGM in comparison to air in Scandinavia. Trajectory analysis of events where high concentrations of TPM simultaneously were observed at sites in North Europe indicate source areas in Central Europe and provide evidence of transport of mercury on particles on a regional scale.

 

Atmospheric mercury distribution in Northern Europe and in Atmospheric mercury distribution in Northern Europe and in

Date added: 08/06/2001
Date modified: 06/30/2009
Filesize: 238.69 kB

I. Wangberg, J. Munthe, N. Pirrone, A. Iverfeldt, E. Bahlman, P. Costa, R. Ebinghaus, X. Feng, R. Ferrara, K. Gardfeldt, H. Kock, E. Lanzillotta, Y. Mamane, F. Mas, E. Melamed, Y. Osnat, E. Prestbo, J. Sommar, S. Schmolke, G. Spain, F. Sprovieri, G. Tuncel, Atmospheric mercury distribution in Northern Europe and in the Mediterranean region, Atmospheric EnvironmentVolume 35, Issue 17, , June 2001, Pages 3019-3025.


Abstract

 

Mercury species in air have been measured at five sites in Northwest Europe and at five coastal sites in the Mediterranean region during measurements at four seasons. Observed concentrations of total gaseous mercury (TGM), total particulate mercury (TPM) and reactive gaseous mercury (RGM) were generally slightly higher in the Mediterranean region than in Northwest Europe. Incoming clean Atlantic air seems to be enriched in TGM in comparison to air in Scandinavia. Trajectory analysis of events where high concentrations of TPM simultaneously were observed at sites in North Europe indicate source areas in Central Europe and provide evidence of transport of mercury on particles on a regional scale.

 

Production of peroxy radicals at night via reactions of ozone and the nitrate radical in the ma Production of peroxy radicals at night via reactions of ozone and the nitrate radical in the ma

Date added: 08/06/2001
Date modified: 07/23/2009
Filesize: 1.44 MB

Salisbury, G., et al. (2001), Production of peroxy radicals at night via reactions of ozone and the nitrate radical in the marine boundary layer, J. Geophys. Res., 106(D12), 12,669–12,687.


Abstract


In this paper, a substantial set of simultaneous measurements of the sum of peroxy radicals, [HO2+RO2], NO3, hydrocarbons (HCs), and ozone, taken at Mace Head on the Atlantic coast of Ireland in spring 1997, is presented. Conditions encountered during the experiment ranged from semipolluted air masses advected from Britain and continental Europe to clean air masses off the North and mid-Atlantic, where mixing ratios of pollution tracers approached Northern Hemispheric background mixing ratios. Average mixing ratios of peroxy radicals varied from 2.5 to 5.5 parts per trillion by volume (pptv) at night depending on wind sector, and were observed to decay only very slowly from late afternoon to early morning (0.1–0.5 pptv h−1). Measurements of OH and HO2 on two nights using the Fluorescence Assay by Gas Expansion (FAGE) technique give an upper limit for [OH] of 2.5×105 molecules cm−3 and an average upper limit [HO2]/[HO2+RO2] ratio of 0.27. A modeling study of the 1/e lifetimes of the peroxy radicals, assuming no radical production at night, yielded mean lifetimes of between ∼ 8–23 min for HO2 and 3–18 min for CH3O2. Given these lifetimes, it may be concluded that the peroxy-radical mixing ratios observed could not be maintained without substantial production at night. No significant correlation is observed between measured [HO2+RO2] and [NO3] under any conditions. Calculation of the reaction rates for ozone and NO3 with hydrocarbons (HCs) shows that the ozone-initiated oxidation routes of HCs outweighed those of NO3 in the NE, SE and NW wind sectors. In the SW sector, however, the two mechanisms operated at similar rates on average, and oxidation by NO3 was the dominant route in the westerly sector. The oxidation of alkenes at night by ozone was greater by a factor of 4 than that by NO3 over the whole data set. The HC degradation rates from the three “westerly” sectors, where tracer mixing ratios were relatively low, may be representative of the nighttime oxidative capacity of the marine boundary layer throughout the background Northern Hemisphere. Further calculations using literature values for OH yields and inferred RO2 yields from the ozone-alkene reactions show that peroxy radicals derived from the ozone reactions were likely to make up the major part of the peroxy-radical signal at night (mean value 66%). However, the NO3 source was of similar magnitude in the middle of the night, when [NO3] was generally at its maximum. The estimated total rates of formation of peroxy radicals are much higher under semipolluted conditions (mean 8.0×104 molecules cm−3 s−1 in the SE wind sector) than under cleaner conditions (mean 2.4×104 molecules cm−3 s−1 in the westerly wind sector). A model study using a campaign-tailored box model (CTBM) for semipolluted conditions shows that the major primary sources of OH, HO2, and CH3O2 (the most abundant organic peroxy radical) were the Criegee biradical intermediates formed in the reactions of ozone with alkenes.

 

On the formation, growth and composition of nucleation mode particles On the formation, growth and composition of nucleation mode particles

Date added: 08/06/2001
Date modified: 07/03/2009
Filesize: 428.69 kB

Kulmala, M.,M. Dal Maso, J.M. Mäkelä, L. Pirjola, M. Väkevä, P. Aalto, P. Miikkulainen, K. Hämeri and C.D. O'Dowd, On the Formation, growth and composition of nucleation mode particles, Tellus B, 53, 479-490,, 2001


Abstract


Taking advantage of only the measured aerosol particles spectral evolution as a function of time, a new analytical tool is developed to derive formation and growth properties of nucleation mode aerosols. This method, when used with hygroscopic growth‐factors, can also estimate basic composition properties of these recently‐formed particles. From size spectra the diameter growth‐rate can be obtained, and aerosol condensation and coagulation sinks can be calculated. Using this growth‐rate and condensation sink, the concentration of condensable vapours and their source rate can be estimated. Then, combining the coagulation sink together with measured number concentrations and apparent source rates of 3 nm particles, 1 nm particle nucleation rates and concentration can be estimated. To estimate nucleation rates and vapour concentration source rates producing new particle bursts over the Boreal forest regions, three cases from the BIOFOR project were examined using this analytical tool. In this environment, the nucleation mode growth‐rate was observed to be 2–3 nm hour−1, which required a condensable vapour concentration of 2.5–4×107 cm−3 and a source rate of approximately 7.5–11×104 cm−3 s−1 to be sustained. The formation rate of 3 nm particles was ≈1 particle cm−3 s−1 in all three cases. The estimated formation rate of 1 nm particles was 10–100 particles cm−3 s−1, while their concentration was estimated to be between 10,000 and 100,000 particles cm−3. Using hygroscopicity data and mass flux expressions, the mass flux of insoluble vapour is estimated to be of the same order of magnitude as that of soluble vapour, with a soluble to insoluble vapour flux ratio ranging from 0.7 to 1.4 during these nucleation events.

 

Effects of continental boundary layer evolution convection  turbulence and entrainment on... Effects of continental boundary layer evolution convection turbulence and entrainment on...

Date added: 08/06/2001
Date modified: 07/01/2009
Filesize: 740.44 kB

Nilsson, E.D., U. Rannik, G. Buzorius, C.D. O'Dowd, Effects of continental boundary layer evolution, convection, turbulence and entrainment on aerosol formation, Tellus B, 53, 441-461,, 2001.


Abstract


Aerosol nucleation events occurring in the continental boundary layer over the boreal forest region in Finland, during the BIOFOR experiment, have been examined to elucidate the rôle of micrometeorology in promoting such events. Invariably, during the spring campaign of 1999. nucleation events occurred in Arctic and polar air masses during cold air outbreaks. Under clear-sky conditions, typical of these synoptic meteorological patterns, the boundary layer evolution was characterized by the rapid growth of a mixed layer, convection and strong entrainment, first from the residual later and later from the free troposphere. It was found that the freshly nucleated particles were detected within two hours from the onset of strong turbulent kinetic energy, independent of how fast the boundary layer evolved. When considering the growth time from cluster size of ≃ 1 nm to detectable sizes of 3 nm. the nucleation and onset of strong turbulence coincided almost exactly. The most likely site for nucleation to take place was the mixed layer or the entrainment zone, while the forest canopy and the free troposphere could be excluded as the nucleation region. There are several possible explanations for the correlation between the onset of turbulence and nucleation: (1) new aerosols or clusters may have been entrained from the residual layer into the mixed layer where they then (in the case of clusters) underwent growth to detectable sizes: (2) two or more precursor gases may have been mixed with each other over the entrainment zone; (3) the adiabatic cooling in the rising convective plumes and the turbulent fluctuation in temperature and vapors by the entrainment flux may have enhanced aerosol formation; (4) a sudden decrease in preexisting aerosol due to dilution of the mixed layer aerosol by entrained air may have reduced the vapor sink enough to initiate nucleation. However, the lack of vertical profile measurements of nucleation mode aerosols, precursor vapors and turbulent fluctuations throughout and above the mixed-layer results in it remaining an open question as to which one of these processes dominates.

 

Estimating relationships between air mass origin and chemical composition Estimating relationships between air mass origin and chemical composition

Date added: 08/06/2001
Date modified: 07/27/2009
Filesize: 1.49 MB

Methven, J., M. Evans, P. Simmonds, and G. Spain (2001), Estimating relationships between air mass origin and chemical composition, J. Geophys. Res., 106(D5), 5005–5019.


Abstract


Observations of a chemical at a point in the atmosphere typically show sudden transitions between episodes of high and low concentration. Often these are associated with a rapid change in the origin of air arriving at the site. Lagrangian chemical models riding along trajectories can reproduce such transitions, but small timing errors from trajectory phase errors dramatically reduce the correlation between modeled concentrations and observations. Here the origin averaging technique is introduced to obtain maps of average concentration as a function of air mass origin for the East Atlantic Summer Experiment 1996 (EASE96, a ground-based chemistry campaign). These maps are used to construct origin averaged time series which enable comparison between a chemistry model and observations with phase errors factored out. The amount of the observed signal explained by trajectory changes can be quantified, as can the systematic model errors as a function of air mass origin. The Cambridge Tropospheric Trajectory model of Chemistry and Transport (CiTTyCAT) can account for over 70% of the observed ozone signal variance during EASE96 when phase errors are side-stepped by origin averaging. The dramatic increase in correlation (from 23% without averaging) cannot be achieved by time averaging. The success of the model is attributed to the strong relationship between changes in ozone along trajectories and their origin and its ability to simulate those changes. The model performs less well for longer-lived chemical constituents because the initial conditions 5 days before arrival are insufficiently well known.

 

Igac August 2001 Igac August 2001

Date added: 08/06/2001
Date modified: 08/06/2008
Filesize: 1.91 MB

Steady state modelling of hydroxyl radical concentrations at Mace Head during the EASE '97 camp Steady state modelling of hydroxyl radical concentrations at Mace Head during the EASE '97 camp

Date added: 08/06/2001
Date modified: 07/23/2009
Filesize: 564.23 kB
Savage, N.H., R.M. Harrison, P.S. Monks, and G. Salisbury, Steady state modelling of hydroxyl radical concentrations at Mace Head during the EASE '97 campaign. May 1997, Atmos.Env., 35(3), 515-524, 2001, (Ser. No. ACP111).

Abstract

 

Two different steady-state methods are applied to calculate OH radical concentrations based on the rates of known source and sink processes. The first method, which calculates only OH radical concentrations from measured data including HO2 gives good correlation with measured OH concentrations but overpredicts by 30%. The second method applied calculates OH, HO2 and RO2 radical concentrations simultaneously. This second method overestimates the measured concentrations of OH by almost 3 times. This apparent overprediction may be a result of calculated concentrations of HO2 which appear too high and may be indicative of a gap in our understanding of the relevant peroxy radical chemistry or a result of the limited peroxy radical chemistry assumed by the method.

Comparisons of aerosol nitrogen isotopic composition at two polluted coastal sites Comparisons of aerosol nitrogen isotopic composition at two polluted coastal sites

Date added: 08/06/2001
Date modified: 07/23/2009
Filesize: 281.41 kB

Yeatman, S.G. L.J. Spokes, P.F. Dennis and T.D. Jickells, Comparison of aerosol nitrogen isotope composition at two coastal sites, Atmos. Environ. 35, 1307-1320, 2001, (Ser. No. ACP125).


Abstract


Atmospheric fixed-nitrogen deposition can contribute to eutrophication in coastal and estuarine waters. Stable nitrogen isotope data can provide important information regarding the sources and processing of atmospheric fixed-nitrogen species and is thus important in controlling eutrophication. Size-segregated aerosol samples were collected from two coastal sites: Weybourne, England and Mace Head, Ireland and also aboard the RRS Challenger in the Eastern Atlantic Ocean. Aerosol concentrations of ammonium and nitrate were determined prior to δ15N isotopic analysis. For both species a significant difference in mean isotopic composition was seen between samples from Weybourne (+6±6‰ for ammonium and +7±6‰ for nitrate) and Mace Head and RRS Challenger campaigns (-9±8‰ for ammonium and -1±3‰ for nitrate). At each site a strong dependence of isotopic composition on the geographical origin of the sampled air mass was also observed. For aerosol ammonium, marine and terrestrially dominated samples were found to be isotopically distinct, perhaps reflecting the presence of oceanic sources of ammonia in addition to anthropogenic or natural terrestrial sources. Further distinctions were made within terrestrially dominated samples, possibly indicative of different types of animal husbandry regimes or other forms of anthropogenic activity. For aerosol nitrate, there was found to be generally less variation between samples at each site, although at Weybourne a significant difference was observed between the mean isotopic composition of samples originating from the northern UK (+15±3‰) and that of those originating from the southern UK (+10±3‰), suggesting that aerosol δ15N data might possibly facilitate source apportionment between NOx emissions from power stations and those from vehicle exhausts. The nitrate data also appeared to show seasonality with higher concentrations and lower δ15N values seen in the summer.

 

Biogenic fluxes of halomethanes from Irish peatland ecosystems Biogenic fluxes of halomethanes from Irish peatland ecosystems

Date added: 08/06/2001
Date modified: 07/01/2009
Filesize: 278.07 kB

Dimmer, C.H., P.G. Simmonds, G.N. Nickless, and M.R. Bassford, Biogenic fluxes of halomethanes from Irish Peatland Ecosystems, Atmos. Environ., 35(2), 321-330, 2001, (Ser. No. ACP108)


Abstract


Irish peatland ecosystems have been shown to be important sources of low molecular weight halocarbons. Emission of CH3Br, CH3Cl, CH3I and CHCl3 was recorded from all peatland sites monitored, with minor flux of other halocarbons at certain sites. Fluxes were found to be highly linked to incident light, with strong diurnal cycles recorded at all open peatland sites. Estimates of halomethane emissions, particularly from coastal peatland and conifer plantation forest floor sites, suggests that these ecosystems may make a significant contribution to the global budgets of several important halocarbons. Global annual fluxes of 4.7 (0.1-151.9), 0.9 (0.1-3.3), 5.5 (0.9-43.4), and 1.4 (0.1-12.8) Ggyr-1 for CHCl3, CH3Br, CH3Cl, and CH3I, respectively, were determined for peatland ecosystems.

 

Atmospheric inputs of trace metals to the Northeast Atlantic Ocean The importance of southeaste Atmospheric inputs of trace metals to the Northeast Atlantic Ocean The importance of southeaste

Date added: 08/06/2001
Date modified: 07/27/2009
Filesize: 209.3 kB

Spokes et al., 2001 L. Spokes, T. Jickells and K. Jarvis, Atmospheric inputs of trace metals to the northeast Atlantic Ocean: the importance of southeasterly flow, Marine Chemistry 76 (2001), pp. 319–330


Abstract


The study of aerosols and rainwater presented here demonstrates that episodic atmospheric deposition events associated with southeasterly flow are quantitatively significant for large areas of the North Atlantic Ocean. This paper considers aluminium and manganese, with predominantly crustal sources, and lead and zinc, which are mobilised into the atmosphere primarily through anthropogenic activity. High levels of all trace metals are associated with southeasterly flow from Europe as the air passes over heavily populated and industrialised regions before reaching the northeast Atlantic Ocean. Fluxes calculated using the 1% HNO3 acid soluble metal concentration show that, although the climatological norm for this area is westerly flow, short-lived southeasterly transport events dominate the input of trace metals to this ocean region. This material may be toxic to phytoplankton or may be represent a new source of nutrients to the biological community. A significant decrease in atmospheric lead levels in polluted air is seen between June 1996 and May 1997, reflecting the decrease in use of leaded fuels in Europe. Comparing atmospheric flux values to sediment trap metal fluxes shows that the atmosphere represents the dominant source of zinc to the deep ocean, whereas an additional, non-atmospheric, manganese source this required, perhaps from mobilisation of sedimentary material from the continental shelf or long range advection of manganese rich Saharan material.

 

Emissions of CH3Br, organochlorines, and organoiodines from temperate macroalgae Emissions of CH3Br, organochlorines, and organoiodines from temperate macroalgae

Date added: 08/05/2001
Date modified: 07/01/2009
Filesize: 249.05 kB

Baker1 J.M.; Sturges W.T.1; Sugier J.; Sunnenberg G.; Lovett A.A.; Reeves C.E.; Nightingale P.D.; Penkett S.A., Emissions of CH3Br, organochlorines, and organoiodines from temperate macroalgae, Chemosphere: Global Science Change, Volume 3, Number 1, January 2001 , pp. 93-106(14)


Abstract


The production rates of a range of low molecular weight halogenated organics have been determined in cultures of five temperate species of macroalgae collected from the north coast of Norfolk, England. Compounds studied included CH3Br, the chlorinated organics CH3Cl, CH2Cl2 and CHCl3, and the iodinated organics CH3I, C2H5I, and CH2ClI. Measurements of a wider range of halocarbon concentrations in an isolated rockpool and in air over the seaweed bed were also conducted to evaluate the local impact of the seaweeds on halocarbon concentrations in the natural environment. Estimates for the global emissions of some of the key halogenated compounds from macroalgae have been derived. In general macrophytes appear not to be globally significant producers of the particular halocarbons studied. In coastal regions, however, the impact on local atmospheric composition and chemistry could be greater.

 

In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998 In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998

Date added: 08/01/2001
Date modified: 07/24/2009
Filesize: 1.54 MB
O'Doherty, S., et al. (2001), In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998, J. Geophys. Res., 106(D17), 20,429–20,444.

Abstract


Measurements of atmospheric chloroform (CHCl3) by in situ gas chromatography using electron capture detection are reported from the Advanced Global Atmospheric Gases Experiment (AGAGE) network of atmospheric research stations. They are some of the most comprehensive in situ, high-frequency measurements to be reported for CHCl3 and provide valuable information not only on clean “baseline” mixing ratios but also on local and regional sources. Emissions from these sources cause substantial periodic increases in CHCl3 concentrations above their baseline levels, which can be used to identify source strengths. This is particularly the case for measurements made at Mace Head, Ireland. Furthermore, these local sources of CHCl3 emissions are significant in relation to current estimates of global emissions and illustrate that the understanding of competing sources and sinks of CHCl3 is still fragmentary. These observations also show that CHCl3 has a very pronounced seasonal cycle with a summer minimum and winter maximum presumably resulting from enhanced destruction by OH in the summer. The amplitude of the cycle is dependent on sampling location. Over the 57 months of in situ measurements a global average baseline concentration of 8.9±0.1 ppt was determined with no appreciable trend in the baseline detected.

Evidence for Substantial Variations of Atmospheric Hydroxyl Radicals in the Past Two Decades Evidence for Substantial Variations of Atmospheric Hydroxyl Radicals in the Past Two Decades

Date added: 08/01/2001
Date modified: 07/01/2009
Filesize: 1.28 MB

Prinn, R. G.; Huang, J.; Weiss, R. F.; Cunnold, D. M.; Fraser, P. J.; Simmonds, P. G.; McCulloch, A.; Harth, C.; Salameh, P.; O'Doherty, S.; Wang, R. H. J.; Porter, L.; Miller, B. R.,Evidence for Substantial Variations of Atmospheric Hydroxyl Radicals in the Past Two Decades, Science, Volume 292, Issue 5523, pp. 1882-1888 (2001).


Abstract


The hydroxyl radical (OH) is the dominant oxidizing chemical in the atmosphere. It destroys most air pollutants and many gases involved in ozone depletion and the greenhouse effect. Global measurements of 1,1,1-trichloroethane (CH3CCl3, methyl chloroform) provide an accurate method for determining the global and hemispheric behavior of OH. Measurements show that CH3CCl3 levels rose steadily from 1978 to reach a maximum in 1992 and then decreased rapidly to levels in 2000 that were lower than the levels when measurements began in 1978. Analysis of these observations shows that global OH levels were growing between 1978 and 1988, but the growth rate was decreasing at a rate of 0.23 +/- 0.18% year-2, so that OH levels began declining after 1988. Overall, the global average OH trend between 1978 and 2000 was -0.64 +/- 0.60% year-1. These variations imply important and unexpected gaps in current understanding of the capability of the atmosphere to cleanse itself.

Role of organic and black carbon in the chemical composition of atmospheric aerosol at European background sites Role of organic and black carbon in the chemical composition of atmospheric aerosol at European background sites

Date added: 08/01/2001
Date modified: 07/23/2009
Filesize: 205.08 kB

Krivacsy, Z., Hoffer, A., Sarvari, Zs., Temesi, D., Baltensperger, U., Nyeki, S., Weingartner, E., Kleefeld, S., Jennings, S.G., 2001. Role of organic and black carbon in the chemical composition of atmospheric ,aerosol at European background sites. Atmospheric Environment 35, 6231-6244.


Abstract


The mass concentrations of inorganic ions, water-soluble organic carbon, water-insoluble organic carbon and black carbon were determined in atmospheric aerosol collected at three European background sites: (1) the Jungfraujoch, Switzerland (high-alpine, PM2.5 aerosol); (2) K-puszta, Hungary (rural, PM1.0 aerosol); (3) Mace Head, Ireland (marine, total particulate matter). At the Jungfraujoch and K-puszta the contribution of carbonaceous compounds to the aerosol mass was higher than that of inorganic ions by 33% and 94%, respectively. At these continental sites about 60% of the organic carbon was water soluble, 55-75% of the total carbon proved to be refractory and a considerable portion of the water soluble, refractory organic matter was composed of humic-like substances. At Mace Head the mass concentration of organic matter was found to be about twice than that of nonsea-salt ions 40% of the organic carbon was water soluble and the amount of highly refractory carbon was low. Humic-like substances were not detected but instead low molecular weight carboxylic acids were responsible for about one-fifth of the water-soluble organic mass. These results imply that the influence of carbonaceous compounds on aerosol properties (e.g. hygroscopic, optical) might be significant.

Transport of boreal forest fire emissions from Canada to Europe Transport of boreal forest fire emissions from Canada to Europe

Date added: 07/31/2001
Date modified: 07/23/2009
Filesize: 2.14 MB

Forster, C., Wandinger, U., Wotawa, G., James, P., Mattis, I., Althausen, D., Simmonds, P., O'Doherty, S., Jennings, S. Gerard., Kleefeld, Christoph, Schneider, Johannes, Trickl, Thomas, Kreipl, Stephan, Jager, Horst, Stohl, Anreas. (2001). Transport of boreal forest fire emissions from Canada to Europe. J. Geophys. Res., 106, 22,887 - 22,906.


Abstract


In August 1998, severe forest fires occurred in many parts of Canada, especially in the Northwest Territories. In the week from August 5 to 11, more than 1000 different fires burned >1 x 106 ha of boreal forest, the highest 1-week sum ever reported throughout the 1990s. In this study we can unambigously show for the first time that these fires caused pronounced large-scale haze layers above Europe and that they influenced concentrations of carbon monoxide and other trace gases at the surface station Mace Head in Ireland over a period of weeks. Transport took place across several thousands of kilometers. An example of such an event, in which a pronounced aerosol layer was observed at an altitude of 3-6 km over Germany during August 1998, is investigated in detail. Backward trajectories ending at the measured aerosol layer are calculated and shown to have their origin in the forest fire region. Simulations with a particle dispersion model reveal how a substantial amount of forest fire emissions was transported across the Atlantic. The resulting aerosol lamina over Europe is captured well by the model. In addition, the model demonstrates that the forest fire emissions polluted large regions over Europe during the second half of August 1998. Surface measurements at Mace Head are compared to the model results for an anthropogenic and a forest fire carbon monoxide tracer, respectively. While wet deposition removed considerable amounts of aerosol during its transport, forest fire carbon monoxide reached Europe in copious amounts. It is estimated that during August 1998, 32%, 10%, and 58% of the carbon monoxide enhancement over the background level at Mace Head were caused by European and North American anthropogenic emissions and forest fire emissions, respectively.

Physical characterization of aerosol particles during nucleation events Physical characterization of aerosol particles during nucleation events

Date added: 07/31/2001
Date modified: 07/03/2009
Filesize: 435.73 kB

Aalto, P.P., K. Hämeri, E. Becker, R. Weber, J. Salm, J.M. Mäkelä, C. Hoell, C.D. O'Dowd, H. Karlsson, H-C. Hansson, M. Väkevä, I. Koponen, G. Buzorius, and M. Kulmala, Physical characteristics of aerosol particles during nucleation events. in press Tellus B, 53, 344-345,, 2001.


Abstract


Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July– 21 August 1998 and 20 March–24 April 1999) in Hyytia¨la¨, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm−3 and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm−3. A coarse mode was also present, extending up to sizes of 20 mm having a number concentration of 1.2 cm−3, volume mean diameter of 2.0 mm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm−3, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.

Overview of the international project on biogenic aerosol formation in the boreal forest Overview of the international project on biogenic aerosol formation in the boreal forest

Date added: 07/31/2001
Date modified: 07/22/2009
Filesize: 727.68 kB

Kulmala, M., K. Hämeri, P.P. Aalto, J.M. Makela, L. Pirjola, E.D. Nilsson, G. Buzorius, U. Rannik, M. Dal Maso, W. Seidl, T. Hoffmann, R. Janson, H-C. Hansson, Y. Viisanen, and A. Laaksonen, C.D. O'Dowd, Overview of the international project on biogenic aerosol formation in the boreal forest (BIOFOR), Tellus B, 324-343, 2001.


Abstract


Aerosol formation and subsequent particle growth in ambient air have been frequently observed at a boreal forest site (SMEAR II station) in Southern Finland. The EU funded project BIOFOR (Biogenic aerosol formation in the boreal forest has focused on: (a) determination of formation mechanisms of aerosol particles in the boreal forest site; (b) verification of emissions of secondary organic aerosols from the boreal forest site; and (c) quantification of the amount of condensable vapours produced in photochemical reactions of biogenic volatile organic compounds (BVOC) leading to aerosol formation. The approach of the project was to combine the continuous measurements with a number of intensive field studies. These field studies were organised in three periods, two of which were during the most intense particle production season and one during a non-event season. Although the exact formation route for 3 nm particles remains unclear, the results can be summarised as follows: Nucleation was always connected to Arctic or Polar air advecting over the site giving conditions for a stable nocturnal boundary layer followed by a rapid formation and growth of a turbulent convective mixed layer closely followed by formation of new particles. The nucleation seems to occur in the mixed layer or entrainment zone. However two more prerequisites seem to be necessary. A certain threshold of high enough sulphuric acid and ammonia concentrations is probably needed as the number of newly formed particles Was correlated with the product of the sulphuric acid production and the ammonia concentrations No such correlation was found with the oxidation products of terpenes. The condensation sink, i.e., effective particle area, is probably of importance as no nucleation was observed at high values of the condensation sink. From measurement of the hygroscopic properties of the nucleation particles it was found that inorganic compounds and hygroscopic organic compounds contributed both to the particle growth during daytime while at night time organic compounds dominated. Emissions rates for several gaseous compounds was determined. Using four independent ways to estimate the amount of the condensable vapour needed for observed growth of aerosol particles we get an estimate of 2-10 × 107 vapour molecules cm-3. The estimations for source rate give 7.5-11 x 104 cm-3 s-1. These results lead to the following conclusions: The most probable formation mechanism is ternary nucleation (water-sulphuric acid-ammonia). After nucleation, growth into observable sizes (≥3 nm) is required before new particles appear. The major part of this growth is probably due to condensation of organic vapours. However, there is lack of direct proof of this phenomenon because the composition of 1-5 nm size particles is extremely difficult to determine using the present state-of-art instrumentation.

Modelling the Contribution of Passive Smoking to Exposure to PM10 in UK Homes Modelling the Contribution of Passive Smoking to Exposure to PM10 in UK Homes

Date added: 07/31/2001
Date modified: 07/03/2009
Filesize: 426.21 kB

Dimitroulopoulou, C., Ashmore, M.R., and M.A. Byrne 2001. Modelling the contribution of passive smoking to exposure to PM10 in UK homes. Indoor and Built Environment, 10, 209-213, 2001.


Abstract

 

A physical compartmental model (INTAIR) has been parameterised to estimate P 1M0 concentrations and has been used to assess the contribution of smoking to P1M0 levels for typical homes in the UK. The results suggest that smoking activity at home increases the daily mean concentrations in the living room by 1-1.5 &- mu;3g.m per cigarette smoked, and may contribute significantly to personal exposures to PM10 The model simulations demonstrate that the contribution of smoking to daily mean concentrations is highly dependent on the air exchange rate between the room and outdoors.

Mid-latitude North-Atlantic aerosol characteristics in clean and polluted air Mid-latitude North-Atlantic aerosol characteristics in clean and polluted air

Date added: 07/31/2001
Date modified: 07/23/2009
Filesize: 574.87 kB
O'Dowd, C.D., E. Becker and M. Kulmala, Mid-latitude North-Atlantic aerosol characteristics in clean and polluted air, Atmos. Res., 58, 167-185, 2001.

Abstract


Aerosol number concentrations (r>1.5 nm) and size distributions (5 nm–150 μm radius) are reported for air masses typical of clean and polluted air masses over a North–East Atlantic coastal site (Mace Head). In clean marine air, total particle concentration is typically 400–600 cm−3, rising to between 600 and 1500 cm−3 for modified maritime air, and in the most polluted air, concentrations increase to ≈7000 cm−3. In all air masses, regular bursts of ultra-fine (1.5–5 nm) particles (UFP) were observed over several hours duration and coincided with low tide occurrence in the presence of solar radiation. During these bursts, measured UFP concentrations exceeded 180,000 cm−3. Typically, the sub-micron marine size distribution possessed a bi-modal shape, typical of cloud-induced aerosol growth, with an accumulation mode centred at 0.1–0.2 μm (radius) and a fine mode ≈0.02 μm, while super-micron sea-spray particles possessed a mode at ≈1–5 μm, extending to ≈10 μm under moderately low wind speeds of 5–6 m s−1. Under higher wind speed conditions (10–11 m s−1), a spume drop mode, extending to sizes of 150 μm, was observed. In anthropogenically influenced air masses, the sub-micron size distribution remained bi-modal, although to a lesser extent. Number concentration is dominated by sub-micron aerosol in all air masses, in marine air masses, surface area is generally dominated by super-micron particles, and volume is overwhelmingly dominated by the mode centred on 10 μm under moderate conditions, and 100 μm under higher winds. By comparison, in polluted air, surface area is dominated by sub-micron sizes and volume dominated by super-micron sizes. After nucleation bursts, growth of new, ultra-fine, particles into sizes in the accumulation mode can be observed under some conditions with growth rates of the order of 10 nm/h. Calculating the pre-existing aerosol condensation sink and the growth rate of newly formed particles allowed estimation of the condensing vapour concentration producing the observed growth along with the source rate of the condensing vapour. The concentration of condensable vapour and its source strength were 10–14×107 molecules cm−3 and 3–14×105 molecules cm−3 s−1, respectively.

Iodine Oxide Homogeneous Nucleation An Explanation for Coastal New Particle Production Iodine Oxide Homogeneous Nucleation An Explanation for Coastal New Particle Production

Date added: 07/31/2001
Date modified: 07/24/2009
Filesize: 423.83 kB

Hoffmann, T, CD O'Dowd, JH Seinfeld, Iodine oxides and new particle formation, Geophys. Res. Letts., 27, 1949-1952, 2001.


Abstract


A series of laboratory experiments on the chemical composition of aerosol particles formed after photodissociation of CH2I2, a major volatile alkyl halide released from macroalgae, have been performed in a laboratory scale reaction chamber using on-line atmospheric pressure chemical ionization mass spectrometry (APCI/MS). Based on the mass spectrometric results and the molecular properties of iodine oxides, we suggest that the self-nucleation of iodine oxides provides an efficient source of natural condensable material in coastal environments and discuss this concept focusing on OIO as one potential key species for new particle formation. The presented hypothesis not only fits the measured enrichment of iodine species in submicrometer particles, but also can explain the frequently observed nucleation bursts in the coastal boundary layer.

Hygroscopic and CCN properties of aerosol particles in boreal forests Hygroscopic and CCN properties of aerosol particles in boreal forests

Date added: 07/31/2001
Date modified: 07/02/2009
Filesize: 498.17 kB
Hämeri, K. J.M. Mäkelä, L. Pirjola, M. Väkevä, P. Aalto, P. Miikkulainen, and C.D. O'Dowd, Hygroscopic properties of boreal forest aerosol during nucleation events. Tellus B, 53, 359-378, 2001

Abstract


The measurements of the hygroscopic and cloud condensation nuclei (CCN) properties of submicrometer atmospheric aerosol particles were performed with two tandem differential mobility analysers (TDMA) and a CCN counter at the Hyytia¨ la¨ forest field station in south-central Finland during the BIOFOR campaign. The TDMAs were used to measure hygroscopic diameter growth factors of individual aerosol particles in the dry particle diameter range 10–365 nm when taken from the dry state (relative humidity RH<5%) to RH=90%. The CCN counter was used to study the activation of aerosol particles when exposed to supersaturated conditions. The measurements show clear diurnal pattern of particle solubility. The pattern was strongest for particles in nucleation and Aitken modes. The lowest growth factor (soluble fraction) values were detected during late evening and early morning and the maximum was observed during noon–afternoon. The highest soluble fractions were determined for nucleation mode particles. The response of hygroscopic growth to changes of relative humidity suggests that the soluble compounds are either fully soluble or deliquescent well before 70% RH. The hygroscopic growth was investigated additionally by a detailed model using the size-resolved composition from the impactor samples. The comparison between different instruments shows good consistency. We found good agreement for the 20 nm growth factors measured with two TDMAs, not only on average but also regarding the temporal variation. The similar conclusion was drawn for comparison of TDMA with CCNC for Aitken mode particles with dry sizes 50 and 73 nm. Differences between wet and dry spectra measured using APS and CSASP spectrometer probes were used to derive growth factors for coarse mode particles. Growth factors for coarse mode particles (Dp ca. 2 mm) ranged between 1.0 and 1.6. Agreement between the evolution of growth factors with time for both accumulation and coarse modes was observed regularly. However, similar portions of the data set also indicated clear differences and consequently different chemical compositions between both modes. When the differences between both modes were observed, the coarse mode always behaved in a less hygroscopic manner, with growth factors near one.

Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995–1998 Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995–1998

Date added: 07/31/2001
Date modified: 07/27/2009
Filesize: 364.88 kB

Derwent, R.G., Ryall, D.B., Jennings, S.G., Spain, T.G., and Simmonds, P.G. (2001). Black carbon aerosol and carbon monoxide in European regionally polluted air masses at Mace Head, Ireland during 1995-1998. Atmos. Environ., 35, 6371-6378.


Abstract


Continuous measurements of black carbon aerosol (BCA) at the Mace Head Atmospheric Research Station on the Atlantic Ocean coast of Ireland show the occurrence of dramatically elevated concentrations when regionally polluted air masses are advected to the station. These occurrences correlate well with similar elevations in carbon monoxide and a wide range of other trace gases monitored near-simultaneously with the BCA. Using daily sector allocation and a sophisticated Lagrangian dispersion model, two independent estimates of the European emission source strength of BCA that are required to explain the Mace Head observations have been made. The best estimates of the UK and European emission source strengths of BCA are 46±14 and [(482-511)±140]x103 tonnes/yr, respectively, and these estimates compare favourably with published inventories, at least to within ±25%, though they are considerably smaller than the emissions employed in some early global climate model studies.

Biogenic coastal aerosol production and its influence on aerosol radiative properties Biogenic coastal aerosol production and its influence on aerosol radiative properties

Date added: 07/31/2001
Date modified: 07/27/2009
Filesize: 562.71 kB
O'Dowd, C.D., Biogenic coastal aerosol production and its influence on aerosol radiative properties, J. Geophys. Res., 106, 1545-1550, 2001

Abstract


Coastal zones have been shown to provide a massive source of new, tidal-related, aerosol particles in the atmospheric boundary layer with concentrations exceeding 1,000,000 cm−3 during nucleation bursts sustained over many hours [O Dowd, 200O]. While coastal regions are very strong sources of natural aerosol particles, hithertofore, it has not been demonstrated that these particles contribute to aerosol-related radiative flux. In this brief report, evidence is presented for growth of these new particles, following tidal-related particle formation, into radiatively active particle sizes (i.e. radius>50 nm) where an increase in concentration of more than 300% can be seen. This increase of radiatively active particles concomitantly results in more than a threefold enhancement in both aerosol scattering ability (thereby influencing direct radiative flux) and cloud condensation nuclei (CCN) availability (thereby influencing indirect radiative flux). These results provide direct evidence for coastal biogenic emissions significantly enhancing the radiative flux potential of atmospheric aerosols.

«StartPrev12345678910NextEnd»
Page 6 of 11
Copyright © 2017 Atmospheric Physics Research Cluster. All Rights Reserved.
Joomla! is Free Software released under the GNU/GPL License.
 
None