scholarly journals Surface fluxes of bromoform and dibromomethane over the tropical western Pacific inferred from airborne in situ measurements

2017 ◽  
Author(s):  
Liang Feng ◽  
Paul I. Palmer ◽  
Robyn Butler ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Chemistry ◽  
Marine Boundary Layer ◽  
Current Knowledge ◽  
A Priori ◽  
Surface Fluxes ◽  
Western Pacific ◽  
Study Region ◽  
The Western Pacific ◽  
Aircraft Data

Abstract. We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from aircraft observations over the western Pacific using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a Maximum A Posteriori inverse model. The distribution of a priori ocean emissions of these gases are reasonably consistent with observed atmospheric mole fractions of CHBr3 (r = 0.62) and CH2Br2 (r = 0.38). These a priori emissions result in a positive model bias in CHBr3 peaking in the marine boundary layer, but capture observed values of CH2Br2 with no significant bias by virtue of its longer atmospheric lifetime. Using GEOS-Chem, we find that observed variations in atmospheric CHBr3 are determined equally by sources over the western Pacific and those outside the study region, but observed variations in CH2Br2 are determined mainly by sources outside the western Pacific. Numerical closed-loop experiments show that the spatial and temporal distribution of boundary layer aircraft data have the potential to substantially improve current knowledge of these fluxes, with improvements related to data density. Using the aircraft data, we estimate aggregated regional fluxes of 3.6 ± 0.3 × 108 g/month and 0.7 ± 0.1 × 108 g/month for CHBr3 and CH2Br2 over 130°–155° E and 0°–12° N, respectively, which represent reductions of 20–40 % and substantial spatial deviations from the a priori inventory. We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions, as used by previous studies.

scholarly journals Surface fluxes of bromoform and dibromomethane over the tropical western Pacific inferred from airborne in situ measurements

2018 ◽  
Vol 18 (20) ◽  
pp. 14787-14798
Author(s):  
Liang Feng ◽  
Paul I. Palmer ◽  
Robyn Butler ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Chemistry ◽  
Current Knowledge ◽  
A Priori ◽  
Surface Fluxes ◽  
Western Pacific ◽  
A Posteriori ◽  
Study Region ◽  
The Western Pacific ◽  
Aircraft Data

Abstract. We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from aircraft observations over the western Pacific using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a maximum a posteriori inverse model. Using GEOS-Chem (GC) as an intermediary, we find that the distribution of a priori ocean emissions of these gases are reasonably consistent with observed atmospheric mole fractions of CHBr3 (r=0.62) and CH2Br2 (r=0.38). These a priori emissions result in a positive model bias in CHBr3 peaking in the marine boundary layer, but reproduce observed values of CH2Br2 with no significant bias by virtue of its longer atmospheric lifetime. Using GEOS-Chem, we find that observed variations in atmospheric CHBr3 are determined equally by sources over the western Pacific and those outside the study region, but observed variations in CH2Br2 are determined mainly by sources outside the western Pacific. Numerical closed-loop experiments show that the spatial and temporal distribution of boundary layer aircraft data have the potential to substantially improve current knowledge of these fluxes, with improvements related to data density. Using the aircraft data, we estimate aggregated regional fluxes of 3.6±0.3×108 and 0.7±0.1×108 g month−1 for CHBr3 and CH2Br2 over 130–155∘E and 0–12∘ N, respectively, which represent reductions of 20 %–40 % of the prior inventories by Ordóñez et al. (2012) and substantial spatial deviations from different a priori inventories. We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions, as used by previous studies. We find that over regions with dense observation coverage, our choice of a priori inventory does not significantly impact our reported a posteriori flux estimates.

scholarly journals Quantifying the vertical transport of CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub> over the Western Pacific

2016 ◽  
Author(s):  
Robyn Butler ◽  
Paul I. Palmer ◽  
Liang Feng ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Open Ocean ◽  
Western Pacific ◽  
Study Region ◽  
Air Masses ◽  
Coastal Oceans ◽  
Geographical Regions ◽  
The Western Pacific

Abstract. We use the GEOS-Chem global 3-D atmospheric chemistry transport model to interpret atmospheric observations of bromoform (CHBr3) and dibromomethane (CH2Br2) collected during the CAST and CONTRAST aircraft measurement campaigns over the Western Pacific, January–February, 2014. We use a new linearised, tagged version of CHBr3 and CH2Br2, allowing us to study the influence of emissions from specific geographical regions on observed atmospheric variations. The model describes 32 %–37 % of CHBr3 observed variability and 15 %–45 % of CH2Br2 observed variability during CAST and CONTRAST, reflecting errors in vertical model transport. The model has a mean positive bias of 30 % that is larger near the surface reflecting errors in the poorly constrained prior emission estimates. We find using the model that observed variability of CHBr3 and CH2Br2 is driven by ocean emissions, particularly by the open ocean above which there is deep convection. We find that contributions from coastal oceans and terrestrial sources over the Western Pacific are significant above altitudes > 6 km, but is still dominated by the open ocean emissions and by air masses transported over longer time lines than the campaign period. In the absence of reliable ocean emission estimates, we use a new physical age of air simulation to determine the relative abundance of halogens delivered by CHBr3 and CH2Br2 to the tropical transition layer (TTL). We find that 6 % (47 %) of air masses with halogen released by the ocean reach the TTL within two (three) atmospheric e-folding lifetimes of CHBr3 and almost all of them reach the TTL within one e-folding lifetime of CH2Br2. We find these gases are delivered to the TTL by a small number of rapid convection events during the study period. Over the duration of CAST and CONTRAST and over our study region, oceans delivered a mean (range) CHBr3 and CH2Br2 mole fraction of 0.46 (0.13–0.72) and 0.88 (0.71–1.01) pptv, respectively, to the TTL, and a mean (range) Bry mole fraction of 3.14 (1.81–4.18) pptv to the upper troposphere. Open ocean emissions are responsible for 75 % of these values, with only 8 % from coastal oceans.

scholarly journals Quantifying the vertical transport of CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub> over the western Pacific

2018 ◽  
Vol 18 (17) ◽  
pp. 13135-13153 ◽  
Author(s):  
Robyn Butler ◽  
Paul I. Palmer ◽  
Liang Feng ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Atmospheric Chemistry ◽  
Vertical Transport ◽  
Open Ocean ◽  
Western Pacific ◽  
Model Errors ◽  
Study Region ◽  
Air Masses ◽  
Geographical Regions ◽  
The Western Pacific

Abstract. We use the GEOS-Chem global 3-D atmospheric chemistry transport model to interpret atmospheric observations of bromoform (CHBr3) and dibromomethane (CH2Br2) collected during the CAST and CONTRAST aircraft measurement campaigns over the western Pacific, January–February 2014. We use a new linearized, tagged version of CHBr3 and CH2Br2, allowing us to study the influence of emissions from specific geographical regions on observed atmospheric variations. The model describes 32 %–37 % of CHBr3 and 15 %–45 % of CH2Br2 observed variability during CAST and CONTRAST, reflecting model errors in vertical transport. The model has a mean positive bias of 30 % that is larger near the surface, reflecting errors in the poorly constrained prior emission estimates. We find using the model that observed variability of CHBr3 and CH2Br2 is driven by open ocean emissions where there is deep convection. Atmospheric variability above 6 km includes a significant contribution from coastal oceans, but it is still dominated by emissions from the open ocean and by older air masses that originate upwind. In the absence of reliable ocean emission estimates, we use a new physical age-of-air simulation to determine the relative abundance of halogens delivered by CHBr3 and CH2Br2 to the tropical transition layer (TTL). We find that 76 % (92 %) of air masses that originate from the ocean reach the TTL within two (three) atmospheric e-folding lifetimes of CHBr3 and almost all of them reach the TTL within one e-folding lifetime of CH2Br2. Over the duration of CAST and CONTRAST, and over our study region, oceans delivered a mean (range) CHBr3 and CH2Br2 mole fraction of 0.46 (0.13–0.72) and 0.88 (0.71–1.01) pptv, respectively, to the TTL, and a mean (range) Bry mole fraction of 3.14 (1.81–4.18) pptv from source gases to the upper troposphere.

scholarly journals Iodine monoxide in the Western Pacific marine boundary layer

2013 ◽  
Vol 13 (6) ◽  
pp. 3363-3378 ◽  
Author(s):  
K. Großmann ◽  
U. Frieß ◽  
E. Peters ◽  
F. Wittrock ◽  
J. Lampel ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Western Pacific ◽  
Optical Absorption Spectroscopy ◽  
Mixing Ratios ◽  
Iodine Monoxide ◽  
German Research ◽  
Inorganic Iodine ◽  
The Tropics ◽  
The Western Pacific

Abstract. A latitudinal cross-section and vertical profiles of iodine monoxide (IO) are reported from the marine boundary layer of the Western Pacific. The measurements were taken using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) during the TransBrom cruise of the German research vessel Sonne, which led from Tomakomai, Japan (42° N, 141° E) through the Western Pacific to Townsville, Australia (19° S, 146° E) in October 2009. In the marine boundary layer within the tropics (between 20° N and 5° S), IO mixing ratios ranged between 1 and 2.2 ppt, whereas in the subtropics and at mid-latitudes typical IO mixing ratios were around 1 ppt in the daytime. The profile retrieval reveals that the bulk of the IO was located in the lower part of the marine boundary layer. Photochemical simulations indicate that the organic iodine precursors observed during the cruise (CH3I, CH2I2, CH2ClI, CH2BrI) are not sufficient to explain the measured IO mixing ratios. Reasonable agreement between measured and modelled IO can only be achieved if an additional sea-air flux of inorganic iodine (e.g., I2) is assumed in the model. Our observations add further evidence to previous studies that reactive iodine is an important oxidant in the marine boundary layer.

scholarly journals Iodine monoxide in the Western Pacific marine boundary layer

2012 ◽  
Vol 12 (10) ◽  
pp. 27475-27519 ◽  
Author(s):  
K. Großmann ◽  
U. Frieß ◽  
E. Peters ◽  
F. Wittrock ◽  
J. Lampel ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Western Pacific ◽  
Optical Absorption Spectroscopy ◽  
Mixing Ratios ◽  
Iodine Monoxide ◽  
German Research ◽  
Inorganic Iodine ◽  
The Tropics ◽  
The Western Pacific

Abstract. A latitudinal cross-section and vertical profiles of iodine monoxide (IO) are reported from the marine boundary layer of the Western Pacific. The measurements were taken using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) during the TransBrom cruise of the German research vessel Sonne, which led from Tomakomai, Japan (42° N, 141° E) through the Western Pacific to Townsville, Australia (19° S, 146° E) in October 2009. In the marine boundary layer within the tropics (between 20° N and 5° S), IO mixing ratios ranged between 1 and 2.2 ppt, whereas in the subtropics and at mid-latitudes typical IO mixing ratios were around 1 ppt in the daytime. The profile retrieval reveals that the bulk of the IO was located in the lower part of the marine boundary layer. Photochemical simulations indicate that the organic iodine precursors observed during the cruise (CH3I, CH2I2, CH2ClI, CH2BrI) are not sufficient to explain the measured IO mixing ratios. Reasonable agreement between measured and modelled IO can only be achieved, if an additional sea-air flux of inorganic iodine (e.g. I2) is assumed in the model. Our observations add further evidence to previous studies that reactive iodine is an important oxidant in the marine boundary layer.

Cold Pools and Their Influence on the Tropical Marine Boundary Layer

2017 ◽  
Vol 74 (4) ◽  
pp. 1149-1168 ◽  
Author(s):  
Simon P. de Szoeke ◽  
Eric D. Skyllingstad ◽  
Paquita Zuidema ◽  
Arunchandra S. Chandra
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Sensible Heat Flux ◽  
Surface Flux ◽  
Active Phase ◽  
Surface Fluxes ◽  
Cold Pool ◽  
Madden Julian Oscillation ◽  
Cold Pools ◽  
Central Indian Ocean

Abstract Cold pools dominate the surface temperature variability observed over the central Indian Ocean (0°, 80°E) for 2 months of research cruise observations in the Dynamics of the Madden–Julian Oscillation (DYNAMO) experiment in October–December 2011. Cold pool fronts are identified by a rapid drop of temperature. Air in cold pools is slightly drier than the boundary layer (BL). Consistent with previous studies, cold pools attain wet-bulb potential temperatures representative of saturated downdrafts originating from the lower midtroposphere. Wind and surface fluxes increase, and rain is most likely within the ~20-min cold pool front. Greatest integrated water vapor and liquid follow the front. Temperature and velocity fluctuations shorter than 6 min achieve 90% of the surface latent and sensible heat flux in cold pools. The temperature of the cold pools recovers in about 20 min, chiefly by mixing at the top of the shallow cold wake layer, rather than by surface flux. Analysis of conserved variables shows mean BL air is composed of 51% air entrained from the BL top (800 m), 22% saturated downdrafts, and 27% air at equilibrium with the ocean surface. The number of cold pools, and their contribution to the BL heat and moisture, nearly doubles in the convectively active phase compared to the suppressed phase of the Madden–Julian oscillation.

scholarly journals Oxidation photochemistry in the Southern Atlantic boundary layer: unexpected deviations of photochemical steady state

2011 ◽  
Vol 11 (3) ◽  
pp. 7045-7093 ◽  
Author(s):  
Z. Hosaynali Beygi ◽  
H. Fischer ◽  
H. D. Harder ◽  
M. Martinez ◽  
R. Sander ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Steady State ◽  
Atlantic Ocean ◽  
Atmospheric Chemistry ◽  
Marine Boundary Layer ◽  
Air Pollutant ◽  
Photochemical Oxidant ◽  
Important Region ◽  
Atmospheric Observations ◽  
Oxidation Efficiency

Abstract. Ozone (O3) is a photochemical oxidant, an air pollutant and a greenhouse gas. As the main precursor of the hydroxyl radical (OH) it strongly affects the oxidation power of the atmosphere. The remote marine boundary layer (MBL) is considered an important region in terms of chemical O3 loss; however surface-based atmospheric observations are sparse and the photochemical processes are not well understood. To investigate the photochemistry under the clean background conditions of the Southern Atlantic Ocean, ship measurements of NO, NO2, O3, JNO2, J(O1D), HO2, OH, ROx and a range of meteorological parameters were carried out. The concentrations of NO and NO2 measured on board the French research vessel Marion-Dufresne (28° S–57° S, 46° W–34° E) in March 2007, are among the lowest yet observed. The data is evaluated for consistency with photochemical steady state (PSS) conditions, and the calculations indicate substantial deviations from PSS (Φ>1). The deviations observed under low NOx conditions (5–25 pptv) demonstrate a remarkable upward tendency in the Leighton ratio (used to characterize PSS) with increasing NOx mixing ratio and JNO2 intensity. It is a paradigm in atmospheric chemistry that OH largely controls the oxidation efficiency of the atmosphere. However, evidence is growing that for unpolluted low-NOx (NO + NO2) conditions the atmospheric oxidant budget is poorly understood. Nevertheless, for the very cleanest conditions, typical for the remote marine boundary layer, good model agreement with measured OH and HO2 radicals has been interpreted as accurate understanding of baseline photochemistry. Here we show that such agreement can be deceptive and that a yet unidentified oxidant is needed to explain the photochemical conditions observed at 40°–60° S over the Atlantic Ocean.

scholarly journals Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

2016 ◽  
Author(s):  
Yuzo Miyazaki ◽  
Sean Coburn ◽  
Kaori Ono ◽  
David T. Ho ◽  
R. Bradley Pierce ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Organic Carbon ◽  
Marine Boundary Layer ◽  
Organic Aerosols ◽  
Equatorial Pacific ◽  
Water Soluble ◽  
Total Carbon ◽  
Stable Carbon ◽  
Study Region ◽  
Eastern Equatorial Pacific

Abstract. Stable carbon isotopic compositions of water-soluble organic carbon (WSOC) and organic molecular markers were measured to investigate the relative contributions of the sea-surface sources to the water-soluble fraction of submicron organic aerosols collected over the eastern equatorial Pacific during the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO)/KA-12-01 cruise. On average, the water-soluble organic fraction of the total carbon (TC) mass in submicron aerosols was ~ 30–35 % in the open oceans, whereas it was ~ 60 % in the coastal oceans. The average stable carbon isotope ratio of WSOC (δ13CWSOC) was −19.8 ± 2.0 ‰, which was systematically higher than that of TC (δ13CTC) (−21.8 ± 1.4 ‰). We found that in both coastal and open oceans, the δ13CWSOC was close to the typical values of δ13C for dissolved organic carbon (DOC), ranging from −22 ‰ to −20 ‰ in surface seawater of tropical Pacific oceans. This suggests an enrichment of marine biological products in WSOC aerosols in the study region regardless of the oceanic area. In particular, enhanced levels of WSOC and biogenic organic marker compounds together with high values of WSOC/TC (~ 60 %) and δ13CWSOC were observed over upwelling areas and phytoplankton blooms, which was attributed to planktonic tissues being more enriched in δ13C. The δ13C analysis estimated that on average, marine sources contribute ~ 90 ± 25 % of the aerosol carbon, indicating the predominance of marine-derived carbon in the submicron WSOC. This conclusion is supported by Lagrangian trajectory analysis, which suggests that the majority of the sampling points on the ship had been exposed to marine boundary layer air for more than 80 % of the time during the previous 7 days. The combined analysis of the δ13C and monosaccharides, such as glucose and fructose, indicated that DOC concentration was the major factor controlling the concentration levels of the submicron WSOC regardless of the oceanic areas over the study region.

scholarly journals Observationally constrained analysis of sea salt aerosol in the marine atmosphere

2019 ◽  
Author(s):  
Huisheng Bian ◽  
Karl Froyd ◽  
Daniel M. Murphy ◽  
Jack Dibb ◽  
Mian Chin ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Chemistry ◽  
Marine Boundary Layer ◽  
Model Simulation ◽  
In Situ Measurements ◽  
Sea Salt ◽  
Boreal Summer ◽  
Integrated Analysis ◽  
Marine Atmosphere

Abstract. Atmospheric sea salt plays important roles in marine cloud formation and atmospheric chemistry. We performed an integrated analysis of NASA GEOS model simulations run with the GOCART aerosol module, in situ measurements from the PALMS and SAGA instruments obtained during the NASA ATom campaign, and aerosol optical depth (AOD) measurements from AERONET Marine Aerosol Network (MAN) sun photometers and from MODIS satellite observations to better constrain sea salt in the marine atmosphere. ATom measurements and GEOS model simulation both show that sea salt concentrations over the Pacific and Atlantic oceans have a strong vertical gradient, varying up to four orders of magnitude from the marine boundary layer to free troposphere. The modeled residence times suggest that the lifetime of sea salt particles with dry diameter less than 3 μm is largely controlled by wet removal, followed next by turbulent process. During both boreal summer and winter, the GEOS simulated sea salt mass mixing ratios agree with SAGA measurements in the marine boundary layer (MBL) and with PALMS measurements above the MBL. However, comparison of AOD from GEOS with AERONET/MAN and MODIS aerosol retrievals indicated that the model underestimated AOD over the oceans where sea salt dominates. The apparent discrepancy of slightly overpredicted concentration and large underpredicted AOD could not be explained by biases in the model RH, which was found to be comparable to or larger than the in-situ measurements. This conundrum is at least partially explained by the sea salt size distribution; where the GEOS simulation has much less sea salt percentage-wise in the smaller particles than was observed by PALMS. Model sensitivity experiments indicated that the simulated sea salt is better correlated with measurements when the sea salt emission is calculated based on the friction velocity and with consideration of sea surface temperature dependence than that parameterized with the 10-m winds.

scholarly journals Observed Evolution of Northward-Propagating Intraseasonal Variation over the Western Pacific: A Case Study in Boreal Early Summer

2013 ◽  
Vol 141 (2) ◽  
pp. 690-706 ◽  
Author(s):  
Masaki Katsumata ◽  
Hiroyuki Yamada ◽  
Hisayuki Kubota ◽  
Qoosaku Moteki ◽  
Ryuichi Shirooka
Keyword(s):  
Boundary Layer ◽  
Large Scale ◽  
Lower Troposphere ◽  
Western Pacific ◽  
Boreal Summer ◽  
Intraseasonal Variation ◽  
Middle Troposphere ◽  
Inactive Period ◽  
The Western Pacific

Abstract This report describes the in situ observed evolution of the atmospheric profile during an event of the boreal summer intraseasonal variation (BSISV) in the tropical western Pacific Ocean. The convectively active region of the BSISV proceeded northward over the sounding and radar network. Over the array, the situation changed from a convectively inactive period to an active period. Inspection of the sounding data revealed the gradual moistening of the lower troposphere during the convectively inactive period. The sounding-derived heat and moisture budget analyses indicated that both the convective- and large-scale processes caused moistening of the lower and middle troposphere where the radar echo tops were observed most frequently. This study is the first to identify such a “preconditioning” process for the BSISV in the western Pacific using detailed in situ observational data. During the preconditioning, an increase in CAPE was observed, as in previous studies of the MJO. An increase of moisture in the boundary layer was responsible for the increase of CAPE. The large-scale horizontal convergence in the boundary layer may be a key factor to moisten the boundary layer through the convective-scale processes, as well as through the large-scale processes to moisten the lower and middle troposphere.

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