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 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 Carbon and hydrogen isotopic ratios of atmospheric methane in the upper troposphere over the Western Pacific

2012 ◽  
Vol 12 (17) ◽  
pp. 8095-8113 ◽  
Author(s):  
T. Umezawa ◽  
T. Machida ◽  
K. Ishijima ◽  
H. Matsueda ◽  
Y. Sawa ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Isotopic Ratio ◽  
Lower Troposphere ◽  
Western Pacific ◽  
Boreal Summer ◽  
Additional Contribution ◽  
Mixing Ratio ◽  
Upper Troposphere ◽  
The Western Pacific

Abstract. We present the mixing ratio, δ13C and δD of atmospheric CH4 using commercial aircraft in the upper troposphere (UT) over the Western Pacific for the period December 2005–September 2010. The observed results were compared with those obtained using commercial container ships in the lower troposphere (LT) over the same region. In the Northern Hemisphere (NH), the UT CH4 mixing ratio shows high values in the boreal summer–autumn, when the LT CH4 mixing ratio reaches a seasonal minimum. From tagged tracer experiments made using an atmospheric chemistry transport model, we found that such high CH4 values are due to rapid transport of air masses influenced by CH4 sources in South Asia and East Asia. The observed isotopic ratio data imply that these areas have CH4 sources with relatively low δ13C and δD signatures such as biogenic sources. Latitudinal distributions of the annual average UT and LT CH4 mixing ratio intersect each other in the tropics; the mixing ratio value is lower in the UT than in the LT in the NH and the situation is reversed in the Southern Hemisphere (SH), due mainly to the NH air intrusion into the SH through the UT. Such intersection of the latitudinal distributions is observable in δD but not in δ13C, implying an additional contribution from reaction of CH4 with active chlorine in the marine boundary layer. δ13C and δD show low values in the NH and high values in the SH both in the UT and in the LT. We also observed an increase in the CH4 mixing ratio and decreases in δ13C and δ

scholarly journals Estimating surface CO<sub>2</sub> fluxes from space-borne CO<sub>2</sub> dry air mole fraction observations using an ensemble Kalman Filter

2009 ◽  
Vol 9 (8) ◽  
pp. 2619-2633 ◽  
Author(s):  
L. Feng ◽  
P. I. Palmer ◽  
H. Bösch ◽  
S. Dance
Keyword(s):  
Kalman Filter ◽  
Mole Fraction ◽  
Ensemble Kalman Filter ◽  
Transport Model ◽  
Co2 Flux ◽  
Surface Flux ◽  
Surface Fluxes ◽  
Co2 Fluxes ◽  
Dry Air ◽  
Geographical Regions

Abstract. We have developed an ensemble Kalman Filter (EnKF) to estimate 8-day regional surface fluxes of CO2 from space-borne CO2 dry-air mole fraction observations (XCO2) and evaluate the approach using a series of synthetic experiments, in preparation for data from the NASA Orbiting Carbon Observatory (OCO). The 32-day duty cycle of OCO alternates every 16 days between nadir and glint measurements of backscattered solar radiation at short-wave infrared wavelengths. The EnKF uses an ensemble of states to represent the error covariances to estimate 8-day CO2 surface fluxes over 144 geographical regions. We use a 12×8-day lag window, recognising that XCO2 measurements include surface flux information from prior time windows. The observation operator that relates surface CO2 fluxes to atmospheric distributions of XCO2 includes: a) the GEOS-Chem transport model that relates surface fluxes to global 3-D distributions of CO2 concentrations, which are sampled at the time and location of OCO measurements that are cloud-free and have aerosol optical depths <0.3; and b) scene-dependent averaging kernels that relate the CO2 profiles to XCO2, accounting for differences between nadir and glint measurements, and the associated scene-dependent observation errors. We show that OCO XCO2 measurements significantly reduce the uncertainties of surface CO2 flux estimates. Glint measurements are generally better at constraining ocean CO2 flux estimates. Nadir XCO2 measurements over the terrestrial tropics are sparse throughout the year because of either clouds or smoke. Glint measurements provide the most effective constraint for estimating tropical terrestrial CO2 fluxes by accurately sampling fresh continental outflow over neighbouring oceans. We also present results from sensitivity experiments that investigate how flux estimates change with 1) bias and unbiased errors, 2) alternative duty cycles, 3) measurement density and correlations, 4) the spatial resolution of estimated flux estimates, and 5) reducing the length of the lag window and the size of the ensemble. At the revision stage of this manuscript, the OCO instrument failed to reach its orbit after it was launched on 24 February 2009. The EnKF formulation presented here is also applicable to GOSAT measurements of CO2 and CH4.

scholarly journals Detecting changes in Arctic methane emissions: limitations of the inter-polar difference of atmospheric mole fractions

2018 ◽  
Vol 18 (24) ◽  
pp. 17895-17907 ◽  
Author(s):  
Oscar B. Dimdore-Miles ◽  
Paul I. Palmer ◽  
Lori P. Bruhwiler
Keyword(s):  
Mole Fraction ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Random Noise ◽  
The Arctic ◽  
Polar Regions ◽  
Annual Growth Rate ◽  
Continuous Version ◽  
The Antarctic

Abstract. We consider the utility of the annual inter-polar difference (IPD) as a metric for changes in Arctic emissions of methane (CH4). The IPD has been previously defined as the difference between weighted annual means of CH4 mole fraction data collected at stations from the two polar regions (defined as latitudes poleward of 53∘ N and 53∘ S, respectively). This subtraction approach (IPD) implicitly assumes that extra-polar CH4 emissions arrive within the same calendar year at both poles. We show using a continuous version of the IPD that the metric includes not only changes in Arctic emissions but also terms that represent atmospheric transport of air masses from lower latitudes to the polar regions. We show the importance of these atmospheric transport terms in understanding the IPD using idealized numerical experiments with the TM5 global 3-D atmospheric chemistry transport model that is run from 1980 to 2010. A northern mid-latitude pulse in January 1990, which increases prior emission distributions, arrives at the Arctic with a higher mole fraction and ≃12 months earlier than at the Antarctic. The perturbation at the poles subsequently decays with an e-folding lifetime of ≃4 years. A similarly timed pulse emitted from the tropics arrives with a higher value at the Antarctic ≃11 months earlier than at the Arctic. This perturbation decays with an e-folding lifetime of ≃7 years. These simulations demonstrate that the assumption of symmetric transport of extra-polar emissions to the poles is not realistic, resulting in considerable IPD variations due to variations in emissions and atmospheric transport. We assess how well the annual IPD can detect a constant annual growth rate of Arctic emissions for three scenarios, 0.5 %, 1 %, and 2 %, superimposed on signals from lower latitudes, including random noise. We find that it can take up to 16 years to detect the smallest prescribed trend in Arctic emissions at the 95 % confidence level. Scenarios with higher, but likely unrealistic, growth in Arctic emissions are detected in less than a decade. We argue that a more reliable measurement-driven approach would require data collected from all latitudes, emphasizing the importance of maintaining a global monitoring network to observe decadal changes in atmospheric greenhouse gases.

scholarly journals Global carbon budgets estimated from atmospheric O<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub> observations in the western Pacific region over a 15-year period

2019 ◽  
Author(s):  
Yasunori Tohjima ◽  
Hitoshi Mukai ◽  
Toshinobu Machida ◽  
Yu Hoshina ◽  
Shin-Ichiro Nakaoka
Keyword(s):  
Mole Fraction ◽  
Temporal Trends ◽  
Heat Content ◽  
Western Pacific ◽  
Global Ocean ◽  
Carbon Sinks ◽  
Increasing Trend ◽  
Carbon Project ◽  
Global Carbon ◽  
The Western Pacific

Abstract. Time series of atmospheric O2/N2 ratio and CO2 mole fraction of flask samples obtained from NIES’s flask sampling network are presented. The network includes two ground sites, Hateruma Island (HAT, 24.05 °N, 123.81 °E) and Cape Ochiishi (COI, 43.17 °N, 145.50 °E), and cargo ships regularly sailing in the western Pacific. Based on temporal changes in fossil fuel-derived CO2 emissions, global atmospheric CO2 burden, and atmospheric potential oxygen (APO), which were calculated from the observed O2/N2 ratio and CO2 mole fraction according to APO = O2 + 1.1 × CO2, we estimated the global carbon sinks of the ocean and land biosphere for a period of more than 15 years. In this carbon budget calculation, we adopted a correction for the time-varying ocean O2 outgassing effect with an average of 0.43 PgC yr−1 for 2000–2016. The outgassing effect, attributed to global ocean warming, was evaluated under the assumption that the net ocean gas flux is proportional to the change in the ocean heat content for the 0–2000 m layer. The resulting oceanic and land biotic carbon sinks were 2.5 ± 0.6 PgC yr−1 and 1.6 ± 0.8 PgC yr−1, respectively, for a 17-year period (2000–2016) and 2.3 ± 0.6 PgC yr−1 and 2.0 ± 0.8 PgC yr−1, respectively, for a 14-year period (2003–2016). Despite the independent approaches, these sink values of this study agreed with those estimated by the Global Carbon Project (GCP) within a difference of about ±0.3 PgC yr−1. We examined the carbon sinks for an interval of five years to assess the temporal trends. The pentad (5-year) ocean sinks showed an increasing trend at a rate of 0.09 ± 0.02 PgC yr−2 during 2001–2014, while the pentad land sinks showed an increasing trend at a rate of 0.23 ± 0.03 PgC yr−2 for 2001–2009 and a decreasing trend at a rate of − 0.23 ± 0.05 PgC yr−2 during 2009–2014. Although there is good agreement in the trends of the pentad sinks between this study and that of GCP, the increasing rate of the pentad ocean sinks of this study was about two times larger than that of GCP.

scholarly journals Carbon and hydrogen isotopic ratios of atmospheric methane in the upper troposphere over the Western Pacific

2012 ◽  
Vol 12 (4) ◽  
pp. 9035-9077 ◽  
Author(s):  
T. Umezawa ◽  
T. Machida ◽  
K. Ishijima ◽  
H. Matsueda ◽  
Y. Sawa ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Isotopic Ratio ◽  
Lower Troposphere ◽  
Western Pacific ◽  
Boreal Summer ◽  
Additional Contribution ◽  
Mixing Ratio ◽  
Upper Troposphere ◽  
The Tropics ◽  
The Western Pacific

Abstract. We present the mixing ratio, δ13C and δD of atmospheric CH4 using commercial aircraft in the upper troposphere (UT) over the Western Pacific for the period December 2005–September 2010. The observed results were compared with those obtained using commercial container ships in the lower troposphere (LT) over the same region. In the Northern Hemisphere (NH), the UT CH4 mixing ratio shows high values in the boreal summer–autumn, when the LT CH4 mixing ratio reaches a seasonal minimum. From tagged tracer experiments made using an atmospheric chemistry transport model, we found that such high CH4 values are due to rapid transport of air masses influenced by CH4 sources in South Asia and East Asia. The observed isotopic ratio data suggest that CH4 sources in these areas have relatively low δ13C and δD signatures, implying biogenic sources. Latitudinal distributions of the annual average UT and LT CH4 mixing ratio intersect each other in the tropics; the mixing ratio value is lower in the UT than in the LT in the NH and the situation is reversed in the Southern Hemisphere (SH), due mainly to the NH air intrusion into the SH through the UT. Such intersection of the latitudinal distributions is observable in δD but not in δ13C, implying additional contribution of a reaction of CH4 with active chlorine in the marine boundary layer. δ13C and δD show low values in the NH and high values in the SH both in the UT and in the LT. We also observed an increase in the CH4 mixing ratio and decreases in δ13C and δD during 2007–2008 in the UT and LT over the Western Pacific, possibly due to enhanced biogenic emissions in the tropics and NH.

scholarly journals Aerial observations of air masses transported from East Asia to the Western Pacific: Vertical structure of polluted air masses

2014 ◽  
Vol 97 ◽  
pp. 456-461 ◽  
Author(s):  
Shiro Hatakeyama ◽  
Keisuke Ikeda ◽  
Sayuri Hanaoka ◽  
Izumi Watanabe ◽  
Takemitsu Arakaki ◽  
...  
Keyword(s):  
East Asia ◽  
Vertical Structure ◽  
Western Pacific ◽  
Air Masses ◽  
The Western Pacific

scholarly journals Sea ice as a source of sea salt aerosol to Greenland ice cores: a model-based study

2017 ◽  
Vol 17 (15) ◽  
pp. 9417-9433 ◽  
Author(s):  
Rachael H. Rhodes ◽  
Xin Yang ◽  
Eric W. Wolff ◽  
Joseph R. McConnell ◽  
Markus M. Frey
Keyword(s):  
Sea Ice ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Ice Core ◽  
Ice Cores ◽  
Open Ocean ◽  
Sea Salt ◽  
The Arctic ◽  
Sea Salt Aerosol ◽  
Annual Variability

Abstract. Growing evidence suggests that the sea ice surface is an important source of sea salt aerosol and this has significant implications for polar climate and atmospheric chemistry. It also suggests the potential to use ice core sea salt records as proxies for past sea ice extent. To explore this possibility in the Arctic region, we use a chemical transport model to track the emission, transport, and deposition of sea salt from both the open ocean and the sea ice, allowing us to assess the relative importance of each. Our results confirm the importance of sea ice sea salt (SISS) to the winter Arctic aerosol burden. For the first time, we explicitly simulate the sea salt concentrations of Greenland snow, achieving values within a factor of two of Greenland ice core records. Our simulations suggest that SISS contributes to the winter maxima in sea salt characteristic of ice cores across Greenland. However, a north–south gradient in the contribution of SISS relative to open-ocean sea salt (OOSS) exists across Greenland, with 50 % of winter sea salt being SISS at northern sites such as NEEM (77° N), while only 10 % of winter sea salt is SISS at southern locations such as ACT10C (66° N). Our model shows some skill at reproducing the inter-annual variability in sea salt concentrations for 1991–1999, particularly at Summit where up to 62 % of the variability is explained. Future work will involve constraining what is driving this inter-annual variability and operating the model under different palaeoclimatic conditions.

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