scholarly journals Emission of atmospherically significant halocarbons by naturally occurring and farmed tropical macroalgae

2013 ◽  
Vol 10 (1) ◽  
pp. 483-528 ◽  
Author(s):  
E. C. Leedham ◽  
C. Hughes ◽  
F. S. L. Keng ◽  
S.-M. Phang ◽  
G. Malin ◽  
...  

Abstract. Current estimates of global halocarbon emissions highlight the tropical coastal environment as an important source of very short-lived (VSL) biogenic halocarbons to the troposphere and stratosphere. This is due to a combination of assumed high primary productivity in tropical coastal waters and the prevalence of deep convective transport potentially capable of rapidly lifting surface emissions to the upper troposphere/lower stratosphere. However, despite this perceived importance direct measurements of tropical coastal biogenic halocarbon emissions, notably from macroalgae (seaweeds), have not been made. In light of this, we provide the first dedicated study of halocarbon production by a range of 15 common tropical macroalgal species and compare these results to those from previous studies of polar and temperate macroalgae. Variation between species was substantial; CHBr3 measured at the end of a 24 h incubation varied from 1.4 to 1129 pmol g FW−1 h−1 (FW = fresh weight of sample). We used our laboratory-determined emission rates to estimate emissions of CHBr3 and CH2Br2 (the two dominant VSL precursors of stratospheric bromine) from the coastlines of Malaysia and South East Asia. We compare these values to previous top-down model estimates of emissions from these regions, and conclude that the contribution of coastal CHBr3 emissions is likely to be lower than previously assumed. The contribution of tropical aquaculture to current emission budgets is also considered. Whilst the current aquaculture contribution to halocarbon emissions in this regional is small, the potential exists for substantial increases in aquaculture to make a significant contribution to regional halocarbon budgets.

2013 ◽  
Vol 10 (6) ◽  
pp. 3615-3633 ◽  
Author(s):  
E. C. Leedham ◽  
C. Hughes ◽  
F. S. L. Keng ◽  
S.-M. Phang ◽  
G. Malin ◽  
...  

Abstract. Current estimates of global halocarbon emissions highlight the tropical coastal environment as an important source of very short-lived (VSL) biogenic halocarbons to the troposphere and stratosphere, due to a combination of assumed high primary productivity in tropical coastal waters and the prevalence of deep convective transport, potentially capable of rapidly lifting surface emissions to the upper troposphere/lower stratosphere. However, despite this perceived importance, direct measurements of tropical coastal biogenic halocarbon emissions, notably from macroalgae (seaweeds), have not been made. In light of this, we provide the first dedicated study of halocarbon production by a range of 15 common tropical macroalgal species and compare these results to those from previous studies of polar and temperate macroalgae. Variation between species was substantial; CHBr3 production rates, measured at the end of a 24 h incubation, varied from 1.4 to 1129 pmol g FW−1 h−1 (FW = fresh weight of sample). We used our laboratory-determined emission rates to estimate emissions of CHBr3 and CH2Br2 (the two dominant VSL precursors of stratospheric bromine) from the coastlines of Malaysia and elsewhere in South East Asia (SEA). We compare these values to previous top-down model estimates of emissions from these regions and, by using several emission scenarios, we calculate an annual CHBr3 emission of 40 (6–224 Mmol Br−1 yr), a value that is lower than previous estimates. The contribution of tropical aquaculture to current emission budgets is also considered. Whilst the current aquaculture contribution to halocarbon emissions in this regional is small, the potential exists for substantial increases in aquaculture to make a significant contribution to regional halocarbon budgets.


2020 ◽  
Vol 20 (2) ◽  
pp. 1163-1181
Author(s):  
Michal T. Filus ◽  
Elliot L. Atlas ◽  
Maria A. Navarro ◽  
Elena Meneguz ◽  
David Thomson ◽  
...  

Abstract. The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important uncertainty in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the western Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model. This methodology benefits from an updated convection scheme that improves simulation of the effect of deep convective motions on particle distribution within the tropical troposphere. We find that the observed CH3I, CHBr3 and CH2Br2 mixing ratios in the tropical tropopause layer (TTL) are consistent with those in the boundary layer when the new convection scheme is used to account for convective transport. More specifically, comparisons between modelled estimates and observations of short-lived CH3I indicate that the updated convection scheme is realistic up to the lower TTL but is less good at reproducing the small number of extreme convective events in the upper TTL. This study consolidates our understanding of the transport of short-lived halocarbons to the upper troposphere and lower stratosphere by using improved model calculations to confirm consistency between observations in the boundary layer, observations in the TTL and atmospheric transport processes. Our results support recent estimates of the contribution of short-lived bromocarbons to the stratospheric bromine budget.


2009 ◽  
Vol 137 (8) ◽  
pp. 2493-2514 ◽  
Author(s):  
Charles Chemel ◽  
Maria R. Russo ◽  
John A. Pyle ◽  
Ranjeet S. Sokhi ◽  
Cornelius Schiller

Abstract The development of a severe Hector thunderstorm that formed over the Tiwi Islands, north of Australia, during the Aerosol and Chemical Transport in Tropical Convection/Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere (ACTIVE/SCOUT-O3) field campaign in late 2005, is simulated by the Advanced Research Weather Research and Forecasting (ARW) model and the Met Office Unified Model (UM). The general aim of this paper is to investigate the role of isolated deep convection over the tropics in regulating the water content in the upper troposphere/lower stratosphere (UT/LS). Using a horizontal resolution as fine as 1 km, the numerical simulations reproduce the timing, structure, and strength of Hector fairly well when compared with field campaign observations. The sensitivity of results from ARW to horizontal resolution is investigated by running the model in a large-eddy simulation mode with a horizontal resolution of 250 m. While refining the horizontal resolution to 250 m leads to a better representation of convection with respect to rainfall, the characteristics of the Hector thunderstorm are basically similar in space and time to those obtained in the 1-km-horizontal-resolution simulations. Several overshooting updrafts penetrating the tropopause are produced in the simulations during the mature stage of Hector. The penetration of rising towering cumulus clouds into the LS maintains the entrainment of air at the interface between the UT and the LS. Vertical exchanges resulting from this entrainment process have a significant impact on the redistribution of atmospheric constituents within the UT/LS region at the scale of the islands. In particular, a large amount of water is injected in the LS. The fate of the ice particles as Hector develops drives the water vapor mixing ratio to saturation by sublimation of the injected ice particles, moistening the air in the LS. The moistening was found to be fairly significant above 380 K and averaged about 0.06 ppmv in the range 380–420 K for ARW. As for UM, the moistening was found to be much larger (about 2.24 ppmv in the range of 380–420 K) than for ARW. This result confirms that convective transport can play an important role in regulating the water vapor mixing ratio in the LS.


2005 ◽  
Vol 5 (4) ◽  
pp. 5325-5372 ◽  
Author(s):  
D. B. Considine ◽  
D. J. Bergmann ◽  
H. Liu

Abstract. We have used the Global Modeling Initiative chemistry and transport model to simulate the radionuclides radon-222 and lead-210 using three different sets of input meteorological information: 1. Output from the Goddard Space Flight Center Global Modeling and Assimilation Office GEOS-STRAT assimilation; 2. Output from the Goddard Institute for Space Studies GISS II′ general circulation model; and 3. Output from the National Center for Atmospheric Research MACCM3 general circulation model. We intercompare these simulations with observations to determine the variability resulting from the different meteorological data used to drive the model, and to assess the agreement of the simulations with observations at the surface and in the upper troposphere/lower stratosphere region. The observational datasets we use are primarily climatologies developed from multiple years of observations. In the upper troposphere/lower stratosphere region, climatological distributions of lead-210 were constructed from ~25 years of aircraft and balloon observations compiled into the US Environmental Measurements Laboratory RANDAB database. Taken as a whole, no simulation stands out as superior to the others. However, the simulation driven by the NCAR MACCM3 meteorological data compares better with lead-210 observations in the upper troposphere/lower stratosphere region. Comparisons of simulations made with and without convection show that the role played by convective transport and scavenging in the three simulations differs substantially. These differences may have implications for evaluation of the importance of very short-lived halogen-containing species on stratospheric halogen budgets.


2005 ◽  
Vol 5 (12) ◽  
pp. 3389-3406 ◽  
Author(s):  
D. B. Considine ◽  
D. J. Bergmann ◽  
H. Liu

Abstract. We have used the Global Modeling Initiative chemistry and transport model to simulate the radionuclides radon-222 and lead-210 using three different sets of input meteorological information: 1. Output from the Goddard Space Flight Center Global Modeling and Assimilation Office GEOS-STRAT assimilation; 2. Output from the Goddard Institute for Space Studies GISS II' general circulation model; and 3. Output from the National Center for Atmospheric Research MACCM3 general circulation model. We intercompare these simulations with observations to determine the variability resulting from the different meteorological data used to drive the model, and to assess the agreement of the simulations with observations at the surface and in the upper troposphere/lower stratosphere region. The observational datasets we use are primarily climatologies developed from multiple years of observations. In the upper troposphere/lower stratosphere region, climatological distributions of lead-210 were constructed from ~25 years of aircraft and balloon observations compiled into the US Environmental Measurements Laboratory RANDAB database. Taken as a whole, no simulation stands out as superior to the others. However, the simulation driven by the NCAR MACCM3 meteorological data compares better with lead-210 observations in the upper troposphere/lower stratosphere region. Comparisons of simulations made with and without convection show that the role played by convective transport and scavenging in the three simulations differs substantially. These differences may have implications for evaluation of the importance of very short-lived halogen-containing species on stratospheric halogen budgets.


2014 ◽  
Vol 14 (14) ◽  
pp. 20159-20195 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
M. G. Schultz ◽  
A. Mahajan ◽  
L. Pozzoli ◽  
...  

Abstract. The Asian summer monsoon involves complex transport patterns with large scale redistribution of trace gases in the upper troposphere and lower stratosphere (UTLS). We employ the global chemistry–climate model ECHAM5-HAMMOZ in order to evaluate the transport pathways and the contributions of nitrogen oxide reservoir species PAN, NOx, and HNO3 from various monsoon regions, to the UTLS over Southern Asia and vice versa. The model is evaluated with trace gas retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-E) and aircraft campaigns during the monsoon season (June–September). There are three regions which contribute substantial pollution to the UTLS during the monsoon: the Asian summer monsoon (ASM), the North American Monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection is deeper into the UTLS as compared to NAM and WAM outflow. The circulation in these monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere. Remote transport also occurs in the extratropical upper troposphere where westerly winds drive North American and European pollutants eastward to partly merge with the ASM plume. Strong ASM convection transports these remote and regional pollutants into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. The intense convective activity in the monsoon regions is associated with lightning generation and thereby the emission of NOy species. This will affect the distribution of PAN in the UTLS. The estimates of lightning produced PAN, HNO3, NOx and ozone obtained from control and lightning-off simulations shows high percentage changes over the regions of convective transport especially equatorial Africa and America and comparatively less over the ASM. This indicates higher anthropogenic pollution transport from the ASM region into the UTLS.


2016 ◽  
Author(s):  
Chaitri Roy ◽  
Suvarna Fadnavis ◽  
Rolf Müller ◽  
Ayantika Dey Chaudhary ◽  
Felix Ploeger

Abstract. Asian summer monsoon convection plays an important role in efficient vertical transport from the surface to the anticyclone. In this paper we investigate the potential impact of convectively transported anthropogenic nitrogen oxides (NOx) on the distribution of ozone in the Upper Troposphere and Lower Stratosphere (UTLS) from simulations with the fully-coupled aerosol chemistry climate model, ECHAM5-HAMMOZ. We performed anthropogenic NOx emission sensitivity experiments over India and China. In these simulations, anthropogenic NOx emissions for the period 2000–2010 have been increased by 38 % over India and by 73 % over China in accordance with satellite observed trends over India of 3.8 % per year and China of 7.3 % per year. These NOx emission sensitivity simulations show that strong convection over the Bay of Bengal and the Southern slopes of the Himalayas transports Indian emissions into the UTLS. Convective transport from the South China Sea injects Chinese emissions into the lower stratosphere. Indian and Chinese emissions are partially transported over the Arabian Sea and west Asia by the tropical easterly jet. Enhanced NOx emissions over India and China increase the ozone radiative forcing over India by 0.112 W/m2 and 0.121 W/m2 respectively. These elevated emissions produces significant warming over the Tibetan Plateau and increase precipitation over India due to a strengthening of the monsoon Hadley circulation. However doubling of NOx emissions over India (73 %); equal to China, produced high ozone in the lower troposphere. It induced a reverse monsoon Hadley circulation and negative precipitation anomalies over India. The associated subsidence suppressed vertical transport of NOx and ozone into the anticyclone.


2021 ◽  
Vol 13 (9) ◽  
pp. 1677
Author(s):  
Dmitry A. Belikov ◽  
Naoko Saitoh ◽  
Prabir K. Patra ◽  
Naveen Chandra

We examined methane (CH4) variability over different regions of India and the surrounding oceans derived from thermal infrared (TIR) band observations (TIR CH4) by the Thermal and Near-infrared Sensor for carbon Observation—Fourier Transform Spectrometer (TANSO-FTS) onboard the Greenhouse gases Observation SATellite (GOSAT) for the period 2009–2014. This study attempts to understand the sensitivity of the vertical profile retrievals at different layers of the troposphere and lower stratosphere, on the basis of the averaging kernel (AK) functions and a priori assumptions, as applied to the simulated concentrations by the MIROC4.0-based Atmospheric Chemistry-Transport Model (MIROC4-ACTM). We stress that this is of particular importance when the satellite-derived products are analyzed using different ACTMs other than those used as retrieved a priori. A comparison of modeled and retrieved CH4 vertical profiles shows that the GOSAT/TANSO-FTS TIR instrument has sufficient sensitivity to provide critical information about the transport of CH4 from the top of the boundary layer to the upper troposphere. The mean mismatch between TIR CH4 and model is within 50 ppb, except for the altitude range above 150 hPa, where the sensitivity of TIR CH4 observations becomes very low. Convolved model profiles with TIR CH4 AK reduces the mismatch to less than the retrieval uncertainty. Distinct seasonal variations of CH4 have been observed near the atmospheric boundary layer (800 hPa), free troposphere (500 hPa), and upper troposphere (300 hPa) over the northern and southern regions of India, corresponding to the southwest monsoon (July–September) and post-monsoon (October–December) seasons. Analysis of the transport and emission contributions to CH4 suggests that the CH4 seasonal cycle over the Indian subcontinent is governed by both the heterogeneous distributions of surface emissions and the influence of the global monsoon divergent wind circulations. The major contrast between monsoon, and pre- and post-monsoon profiles of CH4 over Indian regions are noticed near the boundary layer heights, which is mainly caused by seasonal change in local emission strength with a peak during summer due to increased emissions from the paddy fields and wetlands. A strong difference between seasons in the middle and upper troposphere is caused by convective transport of the emission signals from the surface and redistribution in the monsoon anticyclone of upper troposphere. TIR CH4 observations provide additional information on CH4 in the region compared to what is known from in situ data and total-column (XCH4) measurements. Based on two emission sensitivity simulations compared to TIR CH4 observations, we suggest that the emissions of CH4 from the India region were 51.2 ± 4.6 Tg year−1 during the period 2009–2014. Our results suggest that improvements in the a priori profile shape in the upper troposphere and lower stratosphere (UT/LS) region would help better interpretation of CH4 cycling in the earth’s environment.


2019 ◽  
Vol 19 (15) ◽  
pp. 9989-10008 ◽  
Author(s):  
Suvarna Fadnavis ◽  
Rolf Müller ◽  
Gayatry Kalita ◽  
Matthew Rowlinson ◽  
Alexandru Rap ◽  
...  

Abstract. Convective transport plays a key role in aerosol enhancement in the upper troposphere and lower stratosphere (UTLS) over the Asian monsoon region where low-level convective instability persists throughout the year. We use the state-of-the-art ECHAM6–HAMMOZ global chemistry–climate model to investigate the seasonal transport of anthropogenic Asian sulfate aerosols and their impact on the UTLS. Sensitivity simulations for SO2 emission perturbation over India (48 % increase) and China (70 % decrease) are performed based on the Ozone Monitoring Instrument (OMI) satellite-observed trend, rising over India by ∼4.8 % per year and decreasing over China by ∼7.0 % per year during 2006–2017. The enhanced Indian emissions result in an increase in aerosol optical depth (AOD) loading in the UTLS by 0.61 to 4.17 % over India. These aerosols are transported to the Arctic during all seasons by the lower branch of the Brewer–Dobson circulation enhancing AOD by 0.017 % to 4.8 %. Interestingly, a reduction in SO2 emission over China inhibits the transport of Indian sulfate aerosols to the Arctic in summer-monsoon and post-monsoon seasons due to subsidence over northern India. The region of sulfate aerosol enhancement shows significant warming in the UTLS over northern India, south China (0.2±0.15 to 0.8±0.72 K) and the Arctic (∼1±0.62 to 1.6±1.07 K). The estimated seasonal mean direct radiative forcing at the top of the atmosphere (TOA) induced by the increase in Indian SO2 emission is −0.2 to −1.5 W m−2 over northern India. The Chinese SO2 emission reduction leads to a positive radiative forcing of ∼0.6 to 6 W m−2 over China. The decrease in vertical velocity and the associated enhanced stability of the upper troposphere in response to increased Indian SO2 emissions will likely decrease rainfall over India.


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