| 1. |
- Guo, Hao, et al.
(author)
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Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected
- 2023
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:1, s. 99-117
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Journal article (peer-reviewed)abstract
- The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation.
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| 2. |
- Guo, Hao, et al.
(author)
-
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
- 2021
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:18, s. 13729-13746
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Journal article (peer-reviewed)abstract
- The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (21(m) merged and gap-filled observations of the key reactive species driving the chemical budgets of O-3 and CH4 (O-3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O-3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %-90 % of the total reactivity lies in the top 50 % of the parcels and 25 %-35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. In other words, accurate simulation of the least reactive 50 % of the troposphere is unimportant for global budgets. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find excellent agreement with the loss of O-3 and CH4 but sharp disagreement with production of O-3. The models sharply underestimate O-3 production below 4 km in both Pacific and Atlantic basins, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-towhat-matters, set of metrics for model evaluation.
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| 3. |
- Zona, Donatella, et al.
(author)
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Earlier snowmelt may lead to late season declines in plant productivity and carbon sequestration in Arctic tundra ecosystems
- 2022
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In: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 12:1
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Journal article (peer-reviewed)abstract
- Arctic warming is affecting snow cover and soil hydrology, with consequences for carbon sequestration in tundra ecosystems. The scarcity of observations in the Arctic has limited our understanding of the impact of covarying environmental drivers on the carbon balance of tundra ecosystems. In this study, we address some of these uncertainties through a novel record of 119 site-years of summer data from eddy covariance towers representing dominant tundra vegetation types located on continuous permafrost in the Arctic. Here we found that earlier snowmelt was associated with more tundra net CO2 sequestration and higher gross primary productivity (GPP) only in June and July, but with lower net carbon sequestration and lower GPP in August. Although higher evapotranspiration (ET) can result in soil drying with the progression of the summer, we did not find significantly lower soil moisture with earlier snowmelt, nor evidence that water stress affected GPP in the late growing season. Our results suggest that the expected increased CO2 sequestration arising from Arctic warming and the associated increase in growing season length may not materialize if tundra ecosystems are not able to continue sequestering CO2 later in the season.
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| 4. |
- Santoni, Gregory W., et al.
(author)
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Mass fluxes and isofluxes of methane (ch4) at a new hampshire fen measured by a continuous wave quantum cascade laser spectrometer
- 2012
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In: Journal of Geophysical Research. - 0148-0227 .- 2156-2202. ; 117, s. D10301-
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Journal article (peer-reviewed)abstract
- We have developed a mid-infrared continuous-wave quantum cascade laser direct-absorption spectrometer (QCLS) capable of high frequency (>= 1 Hz) measurements of (CH4)-C-12 and (CH4)-C-13 isotopologues of methane (CH4) with in situ 1-s RMS delta C-13(CH4) precision of 1.5 parts per thousand and Allan-minimum precision of 0.2 parts per thousand. We deployed this QCLS in a well-studied New Hampshire fen to compare measurements of CH4 isoflux by eddy covariance (EC) to Keeling regressions of data from automated flux chamber sampling. Mean CH4 fluxes of 6.5 +/- 0.7 mg CH4 m(-2) hr(-1) over two days of EC sampling in July, 2009 were indistinguishable from mean autochamber CH4 fluxes (6.6 +/- 0.8 mgCH(4) m(-2) hr(-1)) over the same period. Mean delta C-13(CH4) composition of emitted CH4 calculated using EC isoflux methods was -71 +/- 8 parts per thousand (95% C.I.) while Keeling regressions of 332 chamber closing events over 8 days yielded a corresponding value of -64.5 +/- 0.8 parts per thousand Ebullitive fluxes, representing similar to 10% of total CH4 fluxes at this site, were on average 1.2 parts per thousand enriched in C-13 compared to diffusive fluxes. CH4 isoflux time series have the potential to improve process-based understanding of methanogenesis, fully characterize source isotopic distributions, and serve as additional constraints for both regional and global CH4 modeling analysis.
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