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  • 1
    Publication Date: 2019-12-20
    Description: Although most field and modeling studies of river corridor exchange have been conducted at scales ranging from tens to hundreds of meters, results of these studies are used to predict their ecological and hydrological influences at the scale of river networks. Further complicating prediction, exchanges are expected to vary with hydrologic forcing and the local geomorphic setting. While we desire predictive power, we lack a complete spatiotemporal relationship relating discharge to the variation in geologic setting and hydrologic forcing that is expected across a river basin. Indeed, the conceptual model of Wondzell (2011) predicts systematic variation in river corridor exchange as a function of (1) variation in baseflow over time at a fixed location, (2) variation in discharge with location in the river network, and (3) local geomorphic setting. To test this conceptual model we conducted more than 60 solute tracer studies including a synoptic campaign in the 5th-order river network of the H. J. Andrews Experimental Forest (Oregon, USA) and replicate-in-time experiments in four watersheds. We interpret the data using a series of metrics describing river corridor exchange and solute transport, testing for consistent direction and magnitude of relationships relating these metrics to discharge and local geomorphic setting. We confirmed systematic decrease in river corridor exchange space through the river networks, from headwaters to the larger main stem. However, we did not find systematic variation with changes in discharge through time or with local geomorphic setting. While interpretation of our results is complicated by problems with the analytical methods, the results are sufficiently robust for us to conclude that space-for-time and time-for-space substitutions are not appropriate in our study system. Finally, we suggest two strategies that will improve the interpretability of tracer test results and help the hyporheic community develop robust datasets that will enable comparisons across multiple sites and/or discharge conditions.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 2
    Publication Date: 2019-03-01
    Description: Nitrous oxide (N2O) is an important greenhouse gas and it can also generate nitric oxide, which depletes ozone in the stratosphere. It is a common target species of ground-based Fourier transform infrared (FTIR) near-infrared (TCCON) and mid-infrared (NDACC) measurements. Both TCCON and NDACC networks provide a long-term global distribution of atmospheric N2O mole fraction. In this study, the dry-air column-averaged mole fractions of N2O (XN2O) from the TCCON and NDACC measurements are compared against each other at seven sites around the world (Ny-Ålesund, Sodankylä, Bremen, Izaña, Réunion, Wollongong, Lauder) in the time period of 2007–2017. The mean differences in XN2O between TCCON and NDACC (NDACC–TCCON) at these sites are between −3.32 and 1.37 ppb (−1.1 %–0.5 %) with standard deviations between 1.69 and 5.01 ppb (0.5 %–1.6 %), which are within the uncertainties of the two datasets. The NDACC N2O retrieval has good sensitivity throughout the troposphere and stratosphere, while the TCCON retrieval underestimates a deviation from the a priori in the troposphere and overestimates it in the stratosphere. As a result, the TCCON XN2O measurement is strongly affected by its a priori profile. Trends and seasonal cycles of XN2O are derived from the TCCON and NDACC measurements and the nearby surface flask sample measurements and compared with the results from GEOS-Chem model a priori and a posteriori simulations. The trends and seasonal cycles from FTIR measurement at Ny-Ålesund and Sodankylä are strongly affected by the polar winter and the polar vortex. The a posteriori N2O fluxes in the model are optimized based on surface N2O measurements with a 4D-Var inversion method. The XN2O trends from the GEOS-Chem a posteriori simulation (0.97±0.02 (1σ) ppb yr−1) are close to those from the NDACC (0.93±0.04 ppb yr−1) and the surface flask sample measurements (0.93±0.02 ppb yr−1). The XN2O trend from the TCCON measurements is slightly lower (0.81±0.04 ppb yr−1) due to the underestimation of the trend in TCCON a priori simulation. The XN2O trends from the GEOS-Chem a priori simulation are about 1.25 ppb yr−1, and our study confirms that the N2O fluxes from the a priori inventories are overestimated. The seasonal cycles of XN2O from the FTIR measurements and the model simulations are close to each other in the Northern Hemisphere with a maximum in August–October and a minimum in February–April. However, in the Southern Hemisphere, the modeled XN2O values show a minimum in February–April while the FTIR XN2O retrievals show different patterns. By comparing the partial column-averaged N2O from the model and NDACC for three vertical ranges (surface–8, 8–17, 17–50 km), we find that the discrepancy in the XN2O seasonal cycle between the model simulations and the FTIR measurements in the Southern Hemisphere is mainly due to their stratospheric differences.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2018-01-22
    Description: We present top-down constraints on global monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies include (1) a standard 4D-Var inversion at native model resolution (4° × 5°), (2) an inversion for six continental and three ocean regions, and (3) a fast 4D-Var inversion based on a novel dimension reduction technique employing randomized singular value decomposition (SVD). The optimized global flux ranges from 15.9 Tg N yr−1 (SVD-based inversion) to 17.5–17.7 Tg N yr−1 (continental-scale, standard 4D-Var inversions), with the former better capturing the extratropical N2O background measured during the HIAPER Pole-to-Pole Observations (HIPPO) airborne campaigns. We find that the tropics provide a greater contribution to the global N2O flux than is predicted by the prior bottom-up inventories, likely due to underestimated agricultural and oceanic emissions. We infer an overestimate of natural soil emissions in the extratropics and find that predicted emissions are seasonally biased in northern midlatitudes. Here, optimized fluxes exhibit a springtime peak consistent with the timing of spring fertilizer and manure application, soil thawing, and elevated soil moisture. Finally, the inversions reveal a major emission underestimate in the US Corn Belt in the bottom-up inventory used here. We extensively test the impact of initial conditions on the analysis and recommend formally optimizing the initial N2O distribution to avoid biasing the inferred fluxes. We find that the SVD-based approach provides a powerful framework for deriving emission information from N2O observations: by defining the optimal resolution of the solution based on the information content of the inversion, it provides spatial information that is lost when aggregating to political or geographic regions, while also providing more temporal information than a standard 4D-Var inversion.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2018-09-12
    Description: GHOST is a novel, compact shortwave-infrared grating spectrometer, designed for remote sensing of tropospheric columns of greenhouse gases (GHGs) from an airborne platform. It observes solar radiation at medium to high spectral resolution (better than 0.3 nm), which has been reflected by the Earth's surface using similar methods to those used by polar-orbiting satellites such as the JAXA GOSAT mission, NASA's OCO-2, and the Copernicus Sentinel-5 Precursor. By using an original design comprising optical fibre inputs along with a single diffraction grating and detector array, GHOST is able to observe CO2 absorption bands centred around 1.61 and 2.06 µm (the same wavelength regions used by OCO-2 and GOSAT) whilst simultaneously measuring CH4 absorption at 1.65 µm (also observed by GOSAT) and CH4 and CO at 2.30 µm (observed by Sentinel-5P). With emissions expected to become more concentrated towards city sources as the global population residing in urban areas increases, there emerges a clear requirement to bridge the spatial scale gap between small-scale urban emission sources and global-scale GHG variations. In addition to the benefits achieved in spatial coverage through being able to remotely sense GHG tropospheric columns from an aircraft, the overlapping spectral ranges and comparable spectral resolutions mean that GHOST has unique potential for providing validation opportunities for these platforms, particularly over the ocean, where ground-based validation measurements are not available. In this paper we provide an overview of the GHOST instrument, calibration, and data processing, demonstrating the instrument's performance and suitability for GHG remote sensing. We also report on the first GHG observations made by GHOST during its maiden science flights on board the NASA Global Hawk unmanned aerial vehicle, which took place over the eastern Pacific Ocean in March 2015 as part of the CAST/ATTREX joint Global Hawk flight campaign.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2012-09-12
    Description: We present a detailed description of the TES methanol (CH3OH) retrieval algorithm, along with initial global results showing the seasonal and spatial distribution of methanol in the lower troposphere. The full development of the TES methanol retrieval is described, including microwindow selection, error analysis, and the utilization of a priori and initial guess information provided by the GEOS-Chem chemical transport model. Retrieval simulations and a sensitivity analysis using the developed retrieval strategy show that TES: (i) generally provides less than 1.0 piece of information, (ii) is sensitive in the lower troposphere with peak sensitivity typically occurring between ~900–700 hPa (~1–3 km) at a vertical resolution of ~5 km, (iii) has a limit of detectability between 0.5 and 1.0 ppbv Representative Volume Mixing Ratio (RVMR) depending on the atmospheric conditions, corresponding roughly to a profile with a maximum concentration of at least 1 to 2 ppbv, and (iv) in a simulation environment has a mean bias of 0.16 ppbv with a standard deviation of 0.34 ppbv. Applying the newly derived TES retrieval globally and comparing the results with corresponding GEOS-Chem output, we find generally consistent large-scale patterns between the two. However, TES often reveals higher methanol concentrations than simulated in the Northern Hemisphere spring, summer and fall. In the Southern Hemisphere, the TES methanol observations indicate a model overestimate over the bulk of South America from December through July, and a model underestimate during the biomass burning season.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2012-07-12
    Description: Methanol retrievals from nadir-viewing space-based sensors offer powerful new information for quantifying methanol emissions on a global scale. Here we apply an ensemble of aircraft observations over North America to evaluate new methanol measurements from the Tropospheric Emission Spectrometer (TES) on the Aura satellite, and combine the TES data with observations from the Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp-A satellite to investigate the seasonality of methanol emissions from northern midlatitude ecosystems. Using the GEOS-Chem chemical transport model as an intercomparison platform, we find that the TES retrieval performs well when the degrees of freedom for signal (DOFS) are above 0.5, in which case the model:TES regressions are generally consistent with the model:aircraft comparisons. Including retrievals with DOFS below 0.5 degrades the comparisons, as these are excessively influenced by the a priori. The comparisons suggest DOFS 〉0.5 as a minimum threshold for interpreting retrievals of trace gases with a weak tropospheric signal. We analyze one full year of satellite observations and find that GEOS-Chem, driven with MEGANv2.1 biogenic emissions, underestimates observed methanol concentrations throughout the midlatitudes in springtime, with the timing of the seasonal peak in model emissions 1–2 months too late. We attribute this discrepancy to an underestimate of emissions from new leaves in MEGAN, and apply the satellite data to better quantify the seasonal change in methanol emissions for midlatitude ecosystems. The derived parameters (relative emission factors of 11.0, 0.26, 0.12 and 3.0 for new, growing, mature, and old leaves, respectively, plus a leaf area index activity factor of 0.5 for expanding canopies with leaf area index
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2011-11-10
    Description: We present over one year (January 2010–February 2011) of continuous atmospheric methanol measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), and interpret the dataset in terms of constraints on regional methanol sources and seasonality. The seasonal cycle of methanol concentrations observed at the KCMP tall tower is generally similar to that simulated by a global 3-D chemical transport model (GEOS-Chem, driven with MEGANv2.0 biogenic emissions) except the seasonal peak occurs ~1 month earlier in the observations, apparently reflecting a model underestimate of emission rates for younger versus older leaves. Based on a source tracer approach, which we evaluate using GEOS-Chem and with multiple tracers, we estimate that anthropogenic emissions account for approximately 40% of ambient methanol abundance during winter and 10% during summer. During daytime in summer, methanol concentrations increase exponentially with temperature, reflecting the temperature sensitivity of the biogenic source, and the observed temperature dependence is statistically consistent with that in the model. Nevertheless, summertime concentrations are underestimated by on average 35% in the model for this region. The seasonal importance of methanol as a source of formaldehyde (HCHO) and carbon monoxide (CO) is highest in spring through early summer, when biogenic methanol emissions are high but isoprene emissions are still relatively low. During that time observed methanol concentrations account for on average 20% of the total CO and HCHO production rates as simulated by GEOS-Chem, compared to 12% later in the summer and 12% on an annual average basis. The biased seasonality in the model means that the photochemical role for methanol early in the growing season is presently underestimated.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2013-03-25
    Description: We apply a full year of continuous atmospheric acetone measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), with a 0.5° × 0.667° GEOS-Chem nested grid simulation to develop quantitative new constraints on seasonal acetone sources over North America. Biogenic acetone emissions in the model are computed based on the MEGANv2.1 inventory. An inverse analysis of the tall tower observations implies a 37% underestimate of emissions from broadleaf trees, shrubs, and herbaceous plants, and an offsetting 40% overestimate of emissions from needleleaf trees plus secondary production from biogenic precursors. The overall result is a small (16%) model underestimate of the total primary + secondary biogenic acetone source in North America. Our analysis shows that North American primary + secondary anthropogenic acetone sources in the model (based on the EPA NEI 2005 inventory) are accurate to within approximately 20%. An optimized GEOS-Chem simulation incorporating the above findings captures 70% of the variance (R = 0.83) in the hourly measurements at the KCMP tall tower, with minimal bias. The resulting North American acetone source is 11 Tg a−1, including both primary emissions (5.5 Tg a−1) and secondary production (5.5 Tg a−1), and with roughly equal contributions from anthropogenic and biogenic sources. The North American acetone source alone is nearly as large as the total continental volatile organic compound (VOC) source from fossil fuel combustion. Using our optimized source estimates as a baseline, we evaluate the sensitivity of atmospheric acetone and peroxyacetyl nitrate (PAN) to shifts in natural and anthropogenic acetone sources over North America. Increased biogenic acetone emissions due to surface warming are likely to provide a significant offset to any future decrease in anthropogenic acetone emissions, particularly during summer.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2012-11-30
    Description: We apply a full year of continuous atmospheric acetone measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), with a 0.5° × 0.667° GEOS-Chem nested grid simulation to develop quantitative new constraints on seasonal acetone sources over North America, and assess the corresponding impacts on atmospheric chemistry. Biogenic acetone emissions in the model are computed based on the MEGANv2.1 inventory. An inverse analysis of the tall tower observations implies a 37% underestimate of emissions from broadleaf trees, shrubs, and herbaceous plants, and an offsetting 40% overestimate of emissions from needleleaf trees plus secondary production from biogenic precursors. The overall result is a small (16%) model underestimate of the total primary + secondary biogenic acetone source in North America. Our analysis shows that North American primary + secondary anthropogenic acetone sources in the model (based on the EPA NEI 2005 inventory) are accurate to within approximately 20%. An optimized GEOS-Chem simulation incorporating the above findings captures 70% of the variance (R=0.83) in the hourly measurements at the KCMP tall tower, with minimal bias. The resulting North American acetone source is 10.9 Tg a−1, including both primary emissions (5.5 Tg a−1) and secondary production (5.5 Tg a−1), and with roughly equal contributions from anthropogenic and biogenic sources. The North American acetone source alone is nearly as large as the total continental volatile organic compound (VOC) source from fossil fuel combustion. Using our optimized source estimates as a baseline, we evaluate the atmospheric impact of some potential future shifts in acetone sources over North America. Increased biogenic acetone emissions due to surface warming are likely to provide a significant offset to any future decrease in anthropogenic acetone emissions, particularly during summer.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2012-05-08
    Description: We present a detailed description of the TES methanol (CH3OH) retrieval algorithm, along with initial global results showing the seasonal and spatial distribution of methanol in the lower troposphere. The full development of the TES methanol retrieval is described, including microwindow selection, error analysis, and the utilization of a priori and initial guess information provided by the GEOS-Chem chemical transport model. Retrieval simulations and a sensitivity analysis using the developed retrieval strategy show that TES: (i) generally provides between 0.5 and 1.0 pieces of information, (ii) is sensitive in the lower troposphere with peak sensitivity typically occurring between ~900–700 hPa (~1–3 km) at a vertical resolution of ~5 km, (iii) has a limit of detectability between 0.5 and 1.0 ppbv Representative Volume Mixing Ratio (RVMR) depending on the atmospheric conditions, corresponding roughly to a profile with a maximum concentration of at least 1 to 2 ppbv, and (iv) in a simulation environment has a mean bias of 0.16 ppbv and a standard deviation of 0.34 ppbv. Applying the newly-derived TES retrieval globally and comparing the results with corresponding GEOS-Chem output, we find generally consistent large-scale patterns between the two. However, TES often reveals higher methanol concentrations than predicted in the Northern Hemisphere spring, summer and fall. In the Southern Hemisphere, the TES methanol observations indicate a model overestimate over the bulk of South America from December through July, and a model underestimate during the biomass burning season.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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