scholarly journals Optimal estimation of the soil uptake rate of molecular hydrogen from the Advanced Global Atmospheric Gases Experiment and other measurements

Author(s):  
X. Xiao ◽  
R. G. Prinn ◽  
P. G. Simmonds ◽  
L. P. Steele ◽  
P. C. Novelli ◽  
...  
2011 ◽  
Vol 11 (2) ◽  
pp. 4059-4103 ◽  
Author(s):  
H. Yashiro ◽  
K. Sudo ◽  
S. Yonemura ◽  
M. Takigawa

Abstract. The molecular hydrogen (H2) in the troposphere is highly influenced by the strength of H2 uptake by the terrestrial soil surface. The global distribution of H2 and its uptake by the soil are simulated by using a model called CHemical AGCM for Study of Environment and Radiative forcing (CHASER), which incorporates a 2-layered soil diffusion/uptake process component. The simulated distribution of deposition velocity over land reflects regional climate and has a global average of 3.3 × 10−2 cm s−1. In the region north of 30° N, the amount of soil uptake increases, particularly in the summer. However, the increase in the uptake becomes smaller in the winter season due to snow cover and a reduction in the biological activity at low temperatures. In the temperate and humid regions in the mid- and low-latitudes, the uptake is mostly influenced by the soil air ratio, which controls the gas diffusivity in the soil. In the semi-arid region, water stress and high temperature contribute to the reduction of biological activity, as well as to the seasonal variation in the deposition velocity. The comparison with the observations shows that the model reproduces both the distribution and seasonal variation of H2 relatively well. The global burden and tropospheric lifetime are 150 Tg and 2.0 yr, respectively. The seasonal variation of H2 in the northern high latitude is mainly controlled by the large seasonal change in soil uptake. In the Southern Hemisphere, the seasonal change in the net chemical production and inter-hemispheric transport are the dominant cause of the seasonal cycle. Large biomass burning impacts the magnitude of seasonal variation mainly in the tropics and subtropics. Both observation and model show large inter-annual variation, especially for the period 1997–1998, associated with the large biomass burning in tropics and northern high-latitudes. The soil uptake shows relatively small inter-annual variability compared to the signal from biomass burning. We note that the thickness of biologically inactive layer near the soil surface and the uptake flux in semi-arid region is important for the current and future budget of atmospheric H2.


2018 ◽  
Author(s):  
Ronald G. Prinn ◽  
Ray F. Weiss ◽  
Jgor Arduini ◽  
Tim Arnold ◽  
H. Langley DeWitt ◽  
...  

Abstract. We present the organization, instrumentation, datasets, data interpretation, modeling, and accomplishments of the multinational, global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). AGAGE is distinguished by its capability to measure globally, at high frequency and multiple sites, all the important species in the Montreal Protocol and all the important non-carbon dioxide (CO2) gases assessed by the Intergovernmental Panel on Climate Change (CO2 is also measured at several sites). The scientific objectives of AGAGE are important in furthering understanding of global chemical and climatic phenomena. They are to: (1) measure accurately the temporal and spatial distributions of anthropogenic gases that contribute the majority of reactive halogen to the stratosphere and/or are strong infrared absorbers [chlorocarbons, chlorofluorocarbons (CFCs), bromocarbons, hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs) and polyfluorinated compounds (perfluorocarbons (PFCs), nitrogen trifluoride (NF3), sulfuryl fluoride (SO2F2), and sulfur hexafluoride (SF6)), and use these measurements to determine the global rates of their emission and/or destruction (i.e. lifetimes); (2) measure accurately the global distributions and temporal behaviors and determine sources and sinks of non-CO2 biogenic-anthropogenic gases important to climate change and/or ozone depletion [methane (CH4), nitrous oxide (N2O), carbon monoxide (CO), molecular hydrogen (H2), methyl chloride (CH3Cl) and methyl bromide (CH3Br); (3) identify new long-lived greenhouse and ozone-depleting gases [e.g. SO2F2, NF3, heavy PFCs (C4F10, C5F12, C6F14, C7F16, and C8F18) and hydrofluoro-olefins (HFOs, e.g. CH2 = CFCF3) have been identified in AGAGE], initiate real-time monitoring of these new gases, and reconstruct their past histories from AGAGE, air-archive and firn-air measurements; (4) determine the average concentrations and trends of tropospheric hydroxyl radicals (OH) from the rates of destruction of atmospheric trichloroethane (CH3CCl3), HFCs and HCFCs, and estimates of their emissions; (5) determine from atmospheric observations and estimates of their destruction rates, the magnitudes, and distributions by region of surface sources/sinks of all measured gases; (6) provide accurate data on the global accumulation of many of these trace gases, that are used to test the synoptic/regional/global-scale circulations predicted by three-dimensional models; and (7) provide global and regional measurements of methane, carbon monoxide and molecular hydrogen, and estimates of hydroxyl levels, to test primary atmospheric oxidation pathways at mid-latitudes and the tropics. Network Information and Data Repository: http://agage.mit.edu/data or http://cdiac.esd.ornl.gov/ndps/alegage.html


2011 ◽  
Vol 11 (7) ◽  
pp. 3375-3392 ◽  
Author(s):  
C. E. Yver ◽  
I. C. Pison ◽  
A. Fortems-Cheiney ◽  
M. Schmidt ◽  
F. Chevallier ◽  
...  

Abstract. This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and +8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is −59±9 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks.


2011 ◽  
Vol 11 (13) ◽  
pp. 6701-6719 ◽  
Author(s):  
H. Yashiro ◽  
K. Sudo ◽  
S. Yonemura ◽  
M. Takigawa

Abstract. The global tropospheric distribution of molecular hydrogen (H2) and its uptake by the soil are simulated using a model called CHemical AGCM (atmospheric general circulation model) for the Study of the Environment and Radiative forcing (CHASER), which incorporates a two-layered soil diffusion/uptake process component. The simulated distribution of deposition velocity over land is influenced by regional climate, and has a global average of 3.3×10−2 cm s−1. In the region north of 30° N, the amount of soil uptake shows a large seasonal variation corresponding to change in biological activity due to soil temperature and change in diffusion suppression by snow cover. In the temperate and humid regions in the mid- to low- latitudes, the uptake is mostly influenced by the soil air ratio, which controls the gas diffusivity in the soil. In the semi-arid regions, water stress and high temperatures contribute to the reduction of biological activity, as well as to the seasonal variation in the deposition velocity. A comparison with the observations shows that the model reproduces both the distribution and seasonal variation of H2 relatively well. The global burden and tropospheric lifetime of H2 are 150 Tg and 2.0 yr, respectively. The seasonal variation in H2 mixing ratios at the northern high latitudes is mainly controlled by a large seasonal change in the soil uptake. In the Southern Hemisphere, seasonal change in net chemical production and inter-hemispheric transport are the dominant causes of the seasonal cycle, while large biomass burning contributes significantly to the seasonal variation in the tropics and subtropics. Both observations and the model show large inter-annual variations, especially for the period 1997–1998, associated with large biomass burning in the tropics and at Northern Hemisphere high latitudes. The soil uptake shows relatively small inter-annual variability compared with the biomass burning signal. Given that the thickness of biologically inactive layer plays an important role in the soil uptake of H2, its value in the model is chosen to achieve agreement with the observed H2 trends. Uncertainty of the estimated soil uptake flux in the semi-arid region is still large, reflecting the discrepancy in the observed and modeled seasonal variations.


2018 ◽  
Vol 10 (2) ◽  
pp. 985-1018 ◽  
Author(s):  
Ronald G. Prinn ◽  
Ray F. Weiss ◽  
Jgor Arduini ◽  
Tim Arnold ◽  
H. Langley DeWitt ◽  
...  

Abstract. We present the organization, instrumentation, datasets, data interpretation, modeling, and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). AGAGE is distinguished by its capability to measure globally, at high frequency, and at multiple sites all the important species in the Montreal Protocol and all the important non-carbon-dioxide (non-CO2) gases assessed by the Intergovernmental Panel on Climate Change (CO2 is also measured at several sites). The scientific objectives of AGAGE are important in furthering our understanding of global chemical and climatic phenomena. They are the following: (1) to accurately measure the temporal and spatial distributions of anthropogenic gases that contribute the majority of reactive halogen to the stratosphere and/or are strong infrared absorbers (chlorocarbons, chlorofluorocarbons – CFCs, bromocarbons, hydrochlorofluorocarbons – HCFCs, hydrofluorocarbons – HFCs and polyfluorinated compounds (perfluorocarbons – PFCs), nitrogen trifluoride – NF3, sulfuryl fluoride – SO2F2, and sulfur hexafluoride – SF6) and use these measurements to determine the global rates of their emission and/or destruction (i.e., lifetimes); (2) to accurately measure the global distributions and temporal behaviors and determine the sources and sinks of non-CO2 biogenic–anthropogenic gases important to climate change and/or ozone depletion (methane – CH4, nitrous oxide – N2O, carbon monoxide – CO, molecular hydrogen – H2, methyl chloride – CH3Cl, and methyl bromide – CH3Br); (3) to identify new long-lived greenhouse and ozone-depleting gases (e.g., SO2F2, NF3, heavy PFCs (C4F10, C5F12, C6F14, C7F16, and C8F18) and hydrofluoroolefins (HFOs; e.g., CH2 = CFCF3) have been identified in AGAGE), initiate the real-time monitoring of these new gases, and reconstruct their past histories from AGAGE, air archive, and firn air measurements; (4) to determine the average concentrations and trends of tropospheric hydroxyl radicals (OH) from the rates of destruction of atmospheric trichloroethane (CH3CCl3), HFCs, and HCFCs and estimates of their emissions; (5) to determine from atmospheric observations and estimates of their destruction rates the magnitudes and distributions by region of surface sources and sinks of all measured gases; (6) to provide accurate data on the global accumulation of many of these trace gases that are used to test the synoptic-, regional-, and global-scale circulations predicted by three-dimensional models; and (7) to provide global and regional measurements of methane, carbon monoxide, and molecular hydrogen and estimates of hydroxyl levels to test primary atmospheric oxidation pathways at midlatitudes and the tropics. Network Information and Data Repository: http://agage.mit.edu/data or http://cdiac.ess-dive.lbl.gov/ndps/alegage.html (https://doi.org/10.3334/CDIAC/atg.db1001).


2010 ◽  
Vol 10 (11) ◽  
pp. 28963-29005 ◽  
Author(s):  
C. Yver ◽  
I. Pison ◽  
A. Fortems-Cheiney ◽  
M. Schmidt ◽  
P. Bousquet ◽  
...  

Abstract. This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, soil uptake distinct from surface emissions and finally, soil uptake, biomass burning, anthropogenic emissions and N2 fixation-related emissions separately were inverted in several scenarios. The various inversions generate an estimate for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and 8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on soil uptake measurements. Our estimate of global H2 soil uptake is −59 ± 4.0 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions considering their respective uncertainties. To constrain a more robust partition of H2 sources and sinks would need additional constraints, such as isotopic measurements.


2010 ◽  
Vol 12 (3) ◽  
pp. 821-829 ◽  
Author(s):  
Philippe Constant ◽  
Soumitra Paul Chowdhury ◽  
Jennifer Pratscher ◽  
Ralf Conrad

2020 ◽  
Vol 8 ◽  
Author(s):  
Ilya V. Baimler ◽  
Andrey B. Lisitsyn ◽  
Sergey V. Gudkov

The paper investigates the effect of gases dissolved in water on the processes occurring during the laser breakdown of colloidal solutions of nanoparticles. The dynamics of the dependences of the plasma luminosity and acoustic signals on the concentration of nanoparticles under irradiation of colloids of nanoparticles saturated with air, argon, and molecular hydrogen has been studied. It is shown that irradiation of colloids saturated with molecular hydrogen and argon leads to an increase in the integral luminosity and integral acoustic signals in comparison with the control sample saturated with atmospheric gases, which indicates the obvious presence of the influence of gases dissolved in the liquid on the optical breakdown process. The most intense acoustic signals, as well as the brightest breakdowns, were observed when the colloidal solution was saturated with molecular hydrogen.


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