scholarly journals Constraining the concentration of the hydroxyl radical in a stratocumulus-topped marine boundary layer from sea-to-air eddy covariance flux measurements of dimethylsulfide

2009 ◽  
Vol 9 (23) ◽  
pp. 9225-9236 ◽  
Author(s):  
M. Yang ◽  
B. W. Blomquist ◽  
B. J. Huebert
Keyword(s):  
Boundary Layer ◽  
Hydroxyl Radical ◽  
Eddy Covariance ◽  
Diurnal Cycle ◽  
Marine Boundary Layer ◽  
High Reactivity ◽  
Simple Method ◽  
Bromine Oxide ◽  
Dms Oxidation ◽  
Strong Inversion

Abstract. The hydroxyl radical (OH) is an important oxidant in the troposphere due to its high reactivity and relative abundance. Measuring the concentration of OH in situ, however, is technically challenging. Here we present a simple method of estimating an OH-equivalent oxidant concentration ("effective OH") in the marine boundary layer (MBL) from the mass balance of dimethylsulfide (DMS). We use shipboard eddy covariance measurements of the sea-to-air DMS flux from the Vamos Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in October and November of 2008. The persistent stratocumulus cloud-cover off the west coast of South America and the associated strong inversion between MBL and the free troposphere (FT) greatly simplify the dynamics in this region and make our budget estimate possible. From the observed diurnal cycle in DMS concentration, the nighttime entrainment velocity at the inversion is estimated to be 4 mm s−1. We calculate 1.4(±0.2)×106 OH molecules cm−3 from the DMS budget, which represents a monthly effective concentration and is well within the range of previous estimates. Furthermore, when linearly proportioned according to the intensity of solar flux, the resultant diel OH profile, together with DMS surface and entrainment fluxes, enables us to accurately replicate the observed diurnal cycle in DMS (correlation coefficient over 0.9). The nitrate radical (NO3) is found to have little contribution to DMS oxidation during VOCALS-REx. An upper limit estimate of 1 pptv of bromine oxide radical (BrO) would account for 30% of DMS oxidation and lower the OH concentration to 1.0)×106 OH molecules cm−3. Our effective OH estimate includes the oxidation of DMS by such radicals.

scholarly journals Constraining the concentration of the hydroxyl radical in a stratocumulus-topped marine boundary layer from sea-to-air eddy covariance flux measurements of dimethylsulfide

2009 ◽  
Vol 9 (4) ◽  
pp. 16267-16294
Author(s):  
M. Yang ◽  
B. W. Blomquist ◽  
B. J. Huebert
Keyword(s):  
Boundary Layer ◽  
Hydroxyl Radical ◽  
Eddy Covariance ◽  
Diurnal Cycle ◽  
Marine Boundary Layer ◽  
High Reactivity ◽  
Diel Variation ◽  
Measured Intensity ◽  
Simple Method ◽  
Strong Inversion

Abstract. The hydroxyl radical (OH) is an important oxidant in the troposphere due to its high reactivity and relative abundance. Measuring the concentration of OH in situ, however, is technically challenging. Here we present a robust yet simple method of estimating an OH-equivalent oxidant concentration ("effective OH") in the marine boundary layer (MBL) from the mass balance of dimethylsulfide (DMS). We use shipboard eddy covariance measurements of the sea-to-air DMS flux from the Vamos Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in October and November of 2008. The persistent stratocumulus cloud-cover off the west coast of South America and the associated strong inversion between MBL and the free troposphere (FT) greatly simplify the dynamics in this region and make our budget estimate possible. From the observed diurnal cycle in DMS concentration, the nighttime entrainment velocity at the inversion is estimated to be 4 mm s−1. We calculate 1.4×106 OH molecules cm−3 from the DMS budget, which represents a ~monthly effective OH concentration and is well within the range of previous estimates. Furthermore, when fitted to the measured intensity of solar flux, the resultant diel variation in OH concentration, together with the DMS surface and entrainment fluxes, enables us to accurately replicate the observed diurnal cycle in DMS (correlation coefficient exceeding 0.9). The nitrate radical is found to have little contribution to DMS oxidation during VOCALS-REx.

scholarly journals Evaluation of stratocumulus cloud prediction in the Met Office forecast model during VOCALS-REx

2010 ◽  
Vol 10 (21) ◽  
pp. 10541-10559 ◽  
Author(s):  
S. J. Abel ◽  
D. N. Walters ◽  
G. Allen
Keyword(s):  
Boundary Layer ◽  
Diurnal Cycle ◽  
Liquid Water ◽  
Large Scale ◽  
Marine Boundary Layer ◽  
Coastal Region ◽  
Forecast Model ◽  
Good Representation ◽  
Liquid Water Path ◽  
Water Path

Abstract. Observations in the subtropical southeast Pacific obtained during the VOCALS-REx field experiment are used to evaluate the representation of stratocumulus cloud in the Met Office forecast model and to identify key areas where model biases exist. Marked variations in the large scale structure of the cloud field were observed during the experiment on both day-to-day and on diurnal timescales. In the remote maritime region the model is shown to have a good representation of synoptically induced variability in both cloud cover and marine boundary layer depth. Satellite observations show a strong diurnal cycle in cloud fraction and liquid water path in the stratocumulus with enhanced clearances of the cloud deck along the Chilean and Peruvian coasts on certain days. The model accurately simulates the phase of the diurnal cycle but is unable to capture the coastal clearing of cloud. Observations along the 20° S latitude line show a gradual increase in the depth of the boundary layer away from the coast. This trend is well captured by the model (typical low bias of 200 m) although significant errors exist at the coast where the model marine boundary layer is too shallow and moist. Drizzle in the model responds to changes in liquid water path in a manner that is consistent with previous ship-borne observations in the region although the intensity of this drizzle is likely to be too high, particularly in the more polluted coastal region where higher cloud droplet number concentrations are typical. Another mode of variability in the cloud field that the model is unable to capture are regions of pockets of open cellular convection embedded in the overcast stratocumulus deck and an example of such a feature that was sampled during VOCALS-REx is shown.

scholarly journals Measurements of diurnal variations and eddy covariance (EC) fluxes of glyoxal in the tropical marine boundary layer: description of the Fast LED-CE-DOAS instrument

2014 ◽  
Vol 7 (10) ◽  
pp. 3579-3595 ◽  
Author(s):  
S. Coburn ◽  
I. Ortega ◽  
R. Thalman ◽  
B. Blomquist ◽  
C. W. Fairall ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Eddy Covariance ◽  
Marine Boundary Layer ◽  
Light Emitting Diode ◽  
Chemical Properties ◽  
Diurnal Variations ◽  
Optical Absorption Spectroscopy ◽  
Tropical Ocean ◽  
Mixing Ratios ◽  
Fast Light

Abstract. Here we present first eddy covariance (EC) measurements of fluxes of glyoxal, the smallest α-dicarbonyl product of hydrocarbon oxidation, and a precursor for secondary organic aerosol (SOA). The unique physical and chemical properties of glyoxal – i.e., high solubility in water (effective Henry's law constant, KH = 4.2 × 105 M atm−1) and short atmospheric lifetime (~2 h at solar noon) – make it a unique indicator species for organic carbon oxidation in the marine atmosphere. Previous reports of elevated glyoxal over oceans remain unexplained by atmospheric models. Here we describe a Fast Light-Emitting Diode Cavity-Enhanced Differential Optical Absorption Spectroscopy (Fast LED-CE-DOAS) instrument to measure diurnal variations and EC fluxes of glyoxal and inform about its unknown sources. The fast in situ sensor is described, and first results are presented from a cruise deployment over the eastern tropical Pacific Ocean (20° N to 10° S; 133 to 85° W) as part of the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO) field experiment (January to March 2012). The Fast LED-CE-DOAS is a multispectral sensor that selectively and simultaneously measures glyoxal (CHOCHO), nitrogen dioxide (NO2), oxygen dimers (O4), and water vapor (H2O) with ~2 Hz time resolution (Nyquist frequency ~1 Hz) and a precision of ~40 pptv Hz−0.5 for glyoxal. The instrument is demonstrated to be a "white-noise" sensor suitable for EC flux measurements. Fluxes of glyoxal are calculated, along with fluxes of NO2, H2O, and O4, which are used to aid the interpretation of the glyoxal fluxes. Further, highly sensitive and inherently calibrated glyoxal measurements are obtained from temporal averaging of data (e.g., detection limit smaller than 2.5 pptv in an hour). The campaign average mixing ratio in the Southern Hemisphere (SH) is found to be 43 ± 9 pptv glyoxal, which is higher than the Northern Hemisphere (NH) average of 32 ± 6 pptv (error reflects variability over multiple days). The diurnal variation of glyoxal in the marine boundary layer (MBL) is measured for the first time, and mixing ratios vary by ~8 pptv (NH) and ~12 pptv (SH) over the course of 24 h. Consistently, maxima are observed at sunrise (NH: 35 ± 5 pptv; SH: 47 ± 7 pptv), and minima at dusk (NH: 27 ± 5 pptv; SH: 35 ± 8 pptv). In both hemispheres, the daytime flux was directed from the atmosphere into the ocean, indicating that the ocean is a net sink for glyoxal during the day. After sunset the ocean was a source for glyoxal to the atmosphere (positive flux) in the SH; this primary ocean source was operative throughout the night. In the NH, the nighttime flux was positive only shortly after sunset and negative during most of the night. Positive EC fluxes of soluble glyoxal over oceans indicate the presence of an ocean surface organic microlayer (SML) and locate a glyoxal source within the SML. The origin of most atmospheric glyoxal, and possibly other oxygenated hydrocarbons over tropical oceans, remains unexplained and warrants further investigation.

scholarly journals Measurements and modelling of I<sub>2</sub>, IO, OIO, BrO and NO<sub>3</sub> in the mid-latitude marine boundary layer

2005 ◽  
Vol 5 (5) ◽  
pp. 9731-9767 ◽  
Author(s):  
A. Saiz-Lopez ◽  
J. A. Shillito ◽  
H. Coe ◽  
J. M. C. Plane
Keyword(s):  
Boundary Layer ◽  
Time Series ◽  
West Coast ◽  
Marine Boundary Layer ◽  
Molecular Iodine ◽  
Nitrate Radical ◽  
The West ◽  
Bromine Oxide ◽  
Coastal Marine ◽  
Iodine Oxides

Abstract. Time series observations of molecular iodine (I2), iodine oxides (IO, OIO), bromine oxide (BrO), and the nitrate radical (NO3) in the mid-latitude coastal marine boundary layer (MBL) are reported. Measurements were made using a new long-path DOAS instrument during a summertime campaign at Mace Head on the west coast of Ireland. I

An Unusual Aerial Photograph of an Eddy Circulation in Marine Stratocumulus Clouds

2015 ◽  
Vol 143 (2) ◽  
pp. 419-432 ◽  
Author(s):  
Bradley M. Muller ◽  
Christopher G. Herbster ◽  
Frederick R. Mosher
Keyword(s):  
Boundary Layer ◽  
Aerial Photograph ◽  
Marine Boundary Layer ◽  
Model Simulation ◽  
Surface Wind ◽  
Formation Mechanisms ◽  
Marine Stratocumulus ◽  
Surface Evolution ◽  
Strong Inversion ◽  
Stratocumulus Clouds

Abstract An aerial photograph of a cyclonic, von Kármán–like vortex in the marine stratocumulus clouds off the California coast, taken by a commercial pilot near Grover Beach, is presented. It is believed that this is the first photograph of such an eddy, taken from an airplane, to appear in publication. The eddy occurred with a strong inversion above a shallow marine boundary layer, in the lee of high, inversion-penetrating terrain. Tower and surface wind measurements plotted on satellite imagery demonstrate that the Grover Beach eddy was not just a cloud-level feature, but extended through the marine atmospheric boundary layer (MABL) to the surface. Evolution of the flow during the formation of the eddy appears similar to idealized numerical simulations of blocked MABL flow from the literature. The tower measurements sampled the northern part of the eddy circulation during its formation just offshore. The 2°–3°C temperature increases and then decreases during and after the eddy passage may be indicative of warmer air, from sheltered locations to the southeast, and/or downslope flow, being advected by and included into the eddy circulation. Satellite data compared with sequences of wind reversals at two different levels of the meteorological tower suggest that the eddy is tilted with height, at least during its formation stage. Formation mechanisms are discussed, but the subsynoptic observations are inadequate to resolve basic questions about the flow; ultimately a high-resolution model simulation is needed.

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