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 ◽  
...  

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.

2012 ◽  
Vol 12 (17) ◽  
pp. 8095-8113 ◽  
Author(s):  
T. Umezawa ◽  
T. Machida ◽  
K. Ishijima ◽  
H. Matsueda ◽  
Y. Sawa ◽  
...  

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


2013 ◽  
Vol 141 (2) ◽  
pp. 690-706 ◽  
Author(s):  
Masaki Katsumata ◽  
Hiroyuki Yamada ◽  
Hisayuki Kubota ◽  
Qoosaku Moteki ◽  
Ryuichi Shirooka

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.


2009 ◽  
Vol 9 (1) ◽  
pp. 2165-2194 ◽  
Author(s):  
A. Lupu ◽  
J. W. Kaminski ◽  
L. Neary ◽  
J. C. McConnell ◽  
K. Toyota ◽  
...  

Abstract. We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the three-dimensional global multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004–2006 on a 1.5°×1.5° global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May–July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. Our model results show that in the upper troposphere GEM-AQ performs well globally for all seasons, except at Northern high and middle latitudes in summer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, including the interannual variations in the observed mixing ratio. The estimated average global emission equals 1.3 Tg N yr−1. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.


2021 ◽  
Author(s):  
Xiaoxuan Zhao ◽  
Buwen Dong ◽  
Riyu Lu

AbstractIn this study, the cross-equatorial flows (CEF) on both high and low level (HCEF/LCEF) troposphere over the Maritime Continent (MC) in boreal summer are found to have experienced an interdecadal weakening in the mid-1990s based on both JRA55 and NCEP reanalyses. The outputs of 8 coupled models in CMIP6 are used to investigate drivers and the corresponding mechanisms. Model results show that the role of external forcing is weak in the interdecadal weakening of CEF. By contrast, the observed interdecadal weakening of both HCEF and LCEF can be largely explained by internal variability associated with a negative phase of the interdecadal Pacific Oscillation (IPO). Associated with negative IPO are anomalous divergence (convergence), enhanced precipitation over MC and anomalous cyclonic (anticyclonic) circulations, reduced precipitation over western North Pacific (WNP) in the upper (lower) troposphere. Sensitivity experiments based on MetUM-GA6 further manifest that this IPO phase transition can lead to the interdecadal weakening of CEF, in which the central tropical Pacific (CTP) sea surface temperature (SST) anomalies play a dominant role. The cold SST anomalies in CTP lead to reduced local convection and trigger enhanced convection over MC through changes in the Walker circulation. The enhanced convection over MC leads to a change in local Hadley circulation over the western Pacific sector. This change is characterized by anomalous ascents over MC, southerlies in the upper troposphere, descents and reduced precipitation over WNP and northerlies in the lower troposphere, leading to the weakening of CEF. Meanwhile, positive SST anomalies over MC associated with negative IPO also make a contribution to the weakening of CEF by inducing a change in the Hadley circulation in the western Pacific sector through similar processes.


2009 ◽  
Vol 9 (13) ◽  
pp. 4301-4313 ◽  
Author(s):  
A. Lupu ◽  
J. W. Kaminski ◽  
L. Neary ◽  
J. C. McConnell ◽  
K. Toyota ◽  
...  

Abstract. We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the three-dimensional global multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004–2006 on a 1.5°×1.5° global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May–July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. The comparison with the satellite data shows that in the upper troposphere GEM-AQ performs well globally for all seasons, except at northern high and middle latitudes in summer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, including the interannual variations in the observed mixing ratio. A complementary comparison with daily total columns of HCN from two middle latitude ground-based stations in Northern Japan for the same simulation period shows that the model captures the observed seasonal variation and also points to an underestimation of model emissions in the Northern Hemisphere in the summer. The estimated average global emission equals 1.3 Tg N yr−1. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.


2017 ◽  
Author(s):  
Liang Feng ◽  
Paul I. Palmer ◽  
Robyn Butler ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  

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.


2016 ◽  
Vol 29 (18) ◽  
pp. 6597-6616 ◽  
Author(s):  
Sho Tanaka ◽  
Kazuaki Nishii ◽  
Hisashi Nakamura

Abstract The western Pacific (WP) pattern, characterized by north–south dipolar anomalies in pressure over the Far East and western North Pacific, is known as one of the dominant teleconnection patterns in the wintertime Northern Hemisphere. Composite analysis reveals that monthly height anomalies exhibit baroclinic structure with their phase lines tilting southwestward with height in the lower troposphere. The anomalies can thus yield not only a poleward heat flux across the climatological thermal gradient across the strong Pacific jet but also a westward heat flux across the climatological thermal gradient between the North Pacific and the cooler Asian continent. The resultant baroclinic conversion of available potential energy (APE) from the climatological-mean flow contributes most efficiently to the APE maintenance of the monthly WP pattern, acting against strong thermal damping effects by anomalous heat exchanges with the underlying ocean and anomalous precipitation in the subtropics and by the effect of anomalous eddy heat flux under modulated storm-track activity. Kinetic energy (KE) of the pattern is maintained through barotropic feedback forcing associated with modulated activity of transient eddies and the conversion from the climatological-mean westerlies, both of which act against frictional damping. The net feedback forcing by transient eddies is therefore not particularly efficient. The present study suggests that the WP pattern has a characteristic of a dynamical mode that can maintain itself through efficient energy conversion from the climatological-mean fields even without external forcing, including remote influence from the tropics.


Atmosphere ◽  
2020 ◽  
Vol 11 (10) ◽  
pp. 1049
Author(s):  
Xin Li ◽  
Ming Yin ◽  
Xiong Chen ◽  
Minghao Yang ◽  
Fei Xia ◽  
...  

Based on the observation and reanalysis data, the relationship between the Madden–Julian Oscillation (MJO) over the Maritime Continent (MC) and the tropical Pacific–Indian Ocean associated mode was analyzed. The results showed that the MJO over the MC region (95°–150° E, 10° S–10° N) (referred to as the MC–MJO) possesses prominent interannual and interdecadal variations and seasonally “phase-locked” features. MC–MJO is strongest in the boreal winter and weakest in the boreal summer. Winter MC–MJO kinetic energy variation has significant relationships with the El Niño–Southern Oscillation (ENSO) in winter and the Indian Ocean Dipole (IOD) in autumn, but it correlates better with the tropical Pacific–Indian Ocean associated mode (PIOAM). The correlation coefficient between the winter MC–MJO kinetic energy index and the autumn PIOAM index is as high as −0.5. This means that when the positive (negative) autumn PIOAM anomaly strengthens, the MJO kinetic energy over the winter MC region weakens (strengthens). However, the correlation between the MC–MJO convection and PIOAM in winter is significantly weaker. The propagation of MJO over the Maritime Continent differs significantly in the contrast phases of PIOAM. During the positive phase of the PIOAM, the eastward propagation of the winter MJO kinetic energy always fails to move across the MC region and cannot enter the western Pacific. However, during the negative phase of the PIOAM, the anomalies of MJO kinetic energy over the MC is not significantly weakened, and MJO can propagate farther eastward and enter the western Pacific. It should be noted that MJO convection is more likely to extend to the western Pacific in the positive phases of PIOAM than in the negative phases. This is significant different with the propagation of the MJO kinetic energy.


2018 ◽  
Vol 18 (20) ◽  
pp. 14787-14798
Author(s):  
Liang Feng ◽  
Paul I. Palmer ◽  
Robyn Butler ◽  
Stephen J. Andrews ◽  
Elliot L. Atlas ◽  
...  

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.


2013 ◽  
Vol 6 (5) ◽  
pp. 1413-1423 ◽  
Author(s):  
W. W. Verstraeten ◽  
K. F. Boersma ◽  
J. Zörner ◽  
M. A. F. Allaart ◽  
K. W. Bowman ◽  
...  

Abstract. In this analysis, Tropospheric Emission Spectrometer (TES) V004 nadir ozone (O3) profiles are validated with more than 4400 coinciding ozonesonde measurements taken across the world from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) during the period 2005–2010. The TES observation operator was applied to the sonde data to ensure a consistent comparison between TES and ozonesonde data, i.e. without the influence of the a priori O3 profile needed to regulate the retrieval. Generally, TES V004 O3 retrievals are biased high by 2–7 ppbv (7–15%) in the troposphere, consistent with validation results from earlier studies. Because of two degrees of freedom for signal in the troposphere, we can distinguish between upper and lower troposphere mean biases, respectively ranging from −0.4 to +13.3 ppbv for the upper troposphere and +3.9 to +6.0 ppbv for the lower troposphere. Focusing on the 464 hPa retrieval level, broadly representative of the free tropospheric O3, we find differences in the TES biases for the tropics (+3 ppbv, +7%), sub-tropics (+5 ppbv, +11%), and northern (+7 ppbv, +13%) and southern mid-latitudes (+4 ppbv, +10%). The relatively long-term record (6 yr) of TES–ozonesonde comparisons allowed us to quantify temporal variations in TES biases at 464 hPa. We find that there are no discernable biases in each of these latitudinal bands; temporal variations in the bias are typically within the uncertainty of the difference between TES and ozonesondes. Establishing these bias patterns is important in order to make meaningful use of TES O3 data in applications such as model evaluation, trend analysis, or data assimilation.


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