Eddy Correlation Measurements of Ozone Fluxes over Coastal Waters West of Ireland

Measurements of ozone fluxes using the eddy-correlation (EC) technique were carried out for the first time at the Mace Head atmospheric research station, on the west coast of Ireland between August-October 2009. Vertical exchange of ozone was measured from a tower platform at 22 m above mean sea level to study fluxes over coastal waters excluding the tidal region. The results were averaged over 30 min and exhibited predominantly downward but also upward transport of ozone in the boundary layer. Data quality was found to be high based on inspection of cospectra and micrometeorological measurements. During the study period, a major physical influence on O3 fluxes was found to be wind speed. Measured fluxes were of the same magnitude as reported in previous open ocean studies ranging from approximately +0.2 to −0.5 μg m−2 s−1 (−0.017 μg m−2 s−1 on average, corresponding to a deposition velocity of 0.25 mm s−1 or a surface resistance of 4.13 s mm−1). These results are considered to represent ozone fluxes over shallow coastal waters west of Ireland for conditions during summer and fall not affected by phytoplankton blooms

Aerosol Distribution over Europe: a Model Evaluation Study with Detailed Aerosol Microphysics

This paper summarizes an evaluation of model simulations with a regional scale atmospheric climate-chemistry/ aerosol model called REMOTE, which has been extended by a microphysical aerosol module. Model results over Europe are presented and compared with available measurements in surface air focusing on the European distribution and variability of primary and secondary aerosols. Additionally, model results obtained with detailed aerosol microphysics are compared to those based on an aerosol bulk mass approach revealing the impact of dry deposition fluxes on atmospheric burden concentration. An improved determination of elevated ozone and sulfate concentrations could be achieved by considering a diurnal cycle in the anthropogenic emission fluxes. Deviation between modelled and measured organic carbon concentrations can be mainly explained by missing formation of secondary organic aerosols and deficiencies in emission data. Changing residential heating practices in Europe, where the use of wood is no longer restricted to rural areas, need to be considered in emission inventories as well as vegetation fire emissions which present a dominant source of organic carbon.JRC.DDG.H.2-Climate chang

Iodine oxide homogeneous nucleation: An explanation for coastal new particle production

A series of laboratory experiments on the chemical composition of aerosol particles formed after photodissociation of CH_2I_2, 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

Wind Speed Influences on Marine Aerosol Optical Depth

The Mulcahy (Mulcahy et al., 2008) power-law parameterization, derived at the coastal Atlantic station Mace Head, between clean marine aerosol optical depth (AOD) and wind speed is compared to open ocean MODIS-derived AOD versus wind speed. The reported AOD versus wind speed (U) was a function of ∼U2. The open ocean MODIS-derived AOD at 550 nm and 860 nm wavelengths, while in good agreement with the general magnitude of the Mulcahy parameterization, follows a power-law with the exponent ranging from 0.72 to 2.47 for a wind speed range of 2–18 m s−1. For the four cases examined, some MODIS cases underestimated AOD while other cases overestimated AOD relative to the Mulcahy scheme. Overall, the results from MODIS support the general power-law relationship of Mulcahy, although some linear cases were also encountered in the MODIS dataset. Deviations also arise between MODIS and Mulcahy at higher wind speeds (>15 m s−1), where MODIS-derived AOD returns lower values as compared to Mulcahy. The results also support the suggestion than wind generated sea spray, under moderately high winds, can rival anthropogenic pollution plumes advecting out into marine environments with wind driven AOD contributing to AOD values approaching 0.3

Simulating Marine New Particle Formation and Growth Using the M7 Modal Aerosol Dynamics Modal

Peer reviewe

Applicability of condensation particle counters to measure atmospheric clusters

This study presents an evaluation of a pulse height condensation particle counter (PH-CPC) and an expansion condensation particle counter (E-CPC) in terms of measuring ambient and laboratory-generated molecular and ion clusters. Ambient molecular cluster concentrations were measured with both instruments as they were deployed in conjunction with an ion spectrometer and other aerosol instruments in Hyytiälä, Finland at the SMEAR II station between 1 March and 30 June 2007. The observed cluster concentrations varied and ranged from some thousands to 100 000 cm -3. Both instruments showed similar (within a factor of ~5) concentrations. An average size of the detected clusters was approximately 1.8 nm. As the atmospheric measurement of sub 2-nm particles and molecular clusters is a challenging task, we conclude that most likely we were unable to detect the smallest clusters. Nevertheless, the reported concentrations are the best estimates to date for minimum cluster concentrations in a boreal forest environment

Is the Commission a "lawmaker"? : On the right of initiative, institutional transparency and public participation in decision-making: ClientEarth

Peer reviewe

Coastal iodine emissions: part 2. Chamber experiments of particle formation from Laminaria digitata-derived and laboratory-generated I2

Laboratory studies into particle formation from Laminaria digitata macroalgae were undertaken to elucidate aerosol formation for a range of I2 (0.3−76 ppbv) and O3(<3−96 ppbv) mixing ratios and light levels (EPAR = 15, 100,and 235 μmol photons m−2 s−1). No clear pattern was observed for I2 or aerosol parameters as a function of light levels. Aerosol mass fluxes and particle number concentrations,were, however, correlated with I2 mixing ratios for low O3mixing ratios of <3 ppbv (R2 = 0.7 and 0.83, respectively for low light levels, and R2 = 0.95 and 0.98, respectively for medium lightlevels). Additional experiments into particle production as a function of laboratory-generated I2, over a mixing ratio range of 1−8ppbv, were conducted under moderate O3 mixing ratios (∼24 ppbv) where a clear, 100-fold or greater, increase in the aeroso lnumber concentrations and mass fluxes was observed compared to the low O3 experiments. A linear relationship between particle concentration and I2 was found, in reasonable agreement with previous studies. Scaling the laboratory relationship to aerosol concentrations typical of the coastal boundary layer suggests a I2 mixing ratio range of 6−93 pptv can account for the observed particle production events. Aerosol number concentration produced from I2 is more than a factor of 10 higher than thatproduced from CH2I2 for the same mixing ratios

New particle formation from photooxidation of diiodomethane (CH_2I_2)

Photolysis of CH_2I_2 in the presence of O_3 has been proposed as a mechanism leading to intense new particle formation in coastal areas. We report here a comprehensive laboratory chamber study of this system. Rapid homogeneous nucleation was observed over three orders of magnitude in CH_2I_2 mixing ratio, down to a level of 15 ppt (∼4 × 10^8 molec. cm^(−3)) comparable to the directly measured total gas-phase iodine species concentrations in coastal areas. After the nucleation burst, the observed aerosol dynamics in the chamber was dominated by condensation of additional vapors onto existing particles and particle coagulation. Particles formed under dry conditions are fractal agglomerates with mass fractal dimension, D_f ∼ 1.8–2.5. Higher relative humidity (65%) does not change the nucleation or growth behavior from that under dry conditions, but results in more compact and dense particles (D_f ∼ 2.7). On the basis of the known gas-phase chemistry, OIO is the most likely gas-phase species to produce the observed nucleation and aerosol growth; however, the current understanding of this chemistry is very likely incomplete. Chemical analysis of the aerosol using an Aerodyne Aerosol Mass Spectrometer reveals that the particles are composed mainly of iodine oxides but also contain water and/or iodine oxyacids. The system studied here can produce nucleation events as intense as those observed in coastal areas. On the basis of comparison between the particle composition, hygroscopicity, and nucleation and growth rates observed in coastal nucleation and in the experiments reported here, it is likely that photooxidation of CH_2I_2, probably aided by other organic iodine compounds, is the mechanism leading to the observed new particle formation in the west coast of Ireland

Coastal iodine emissions. 1. Release of I2 by Laminaria digitata in chamber experiments

Tidally exposed macroalgae emit large amounts of I2 and iodocarbons that produce hotspots of iodine chemistry and intense particle nucleation events in the coastal marine boundary layer. Current emission rates are poorly characterized, however,with reported emission rates varying by 3 orders of magnitude. In this study, I2 emissions from 25 Laminaria digitata samples were investigated in a simulation chamber using incoherent broadbandcavity-enhanced absorption spectroscopy (IBBCEAS). The chamber design allowed gradual extraction of seawater to simulate tidal emersion of algae. Samples were exposed to air with or without O3 and to varying irradiances. Emission of I2 occurred in four distinct stages: (1) moderate emissions from partially submerged samples;(2) a strong release by fully emerged samples; (3) slowing or stopping of I2 release; and (4) later pulses of I2 evident in some samples. Emission rates were highly variable and ranged from 7to 616 pmol min−1 gFW−1 in ozone-free air, with a median value of 55 pmol min−1 gFW−1 for 20 samples