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188 records · Page 11

Atmospheric Trace Gas Abundances and Stable Isotope Ratios via IR-LIF

We propose to develop new technologies with support provided by PIDDP that will enable the in situ measurements of abundances and stable isotope ratios in important radiatively and biogenically active gases such as carbon dioxide, carbon monoxide, water, methane, nitrous oxide, and hydrogen sulfide to very high precision (0.1 per mil or better for the isotopic ratios, for example). Such measurements, impossible at present, could provide pivotal new constraints on the global (bio)geochemical budgets of these critical species, and could also be used to examine the dynamics of atmospheric transport on Mars, Titan, and other solar system bodies. We believe the combination of solid state light sources with imaging of the IR laser induced fluorescence (IR-LIF) via newly available detector arrays will make such in situ measurements possible for the first time. Even under ambient terrestrial conditions, the LIF yield from vibrational excitation of species such as water and carbon dioxide should produce emission measures well in excess of ten billion photons/sec from samples volumes of order 1 c.c. These count rates can, in principle, yield detection limits into the sub-ppt range that are required for the in situ isotopic study of atmospheric trace gases. While promising, such technologies are relatively immature, but developing rapidly, and there are a great many uncertainties regarding their applicability to in situ IR-LIF planetary studies. We therefore feel PIDDP support will be critical to developing these new tools, and propose a three-year program to combine microchip near-IR lasers with low background detection axes and state-of-the-art HgCdTe detectors developed for astronomical spectroscopy to investigate the sensitivity of IR-LIF under realistic planetary conditions, to optimize the optical pumping and filtering schemes for important species, and to apply the spectrometer to the non-destructive measurement of stable isotopes in a variety of test samples. These studies form the necessary precursors to the development of compact, lightweight stable isotope/trace gas sensors for future planetary missions.

Blake, Geoffrey A.↗

Permafrost Region Greenhouse Gas Budgets Suggest a Weak CO 2 Sink and CH 4 and N 2 O Sources, But Magnitudes Differ Between Top-Down and Bottom-Up Methods

Large stocks of soil carbon (C) and nitrogen (N) in northern permafrost soils are vulnerable to remobilization under climate change. However, there are large uncertainties in present-day greenhouse gas (GHG) budgets. We compare bottom-up (data-driven upscaling and process-based models) and top-down (atmospheric inversion models) budgets of carbon dioxide (CO 2 ), methane (CH 4 ) and nitrous oxide (N 2 O) as well as lateral fluxes of C and N across the region over 2000–2020. Bottom-up approaches estimate higher land-to-atmosphere fluxes for all GHGs. Both bottom-up and top-down approaches show a sink of CO 2 in natural ecosystems (bottom-up: -29 (-709, 455), top-down: -587 (-862, -312) Tg CO 2 -C yr -1 ) and sources of CH 4 (bottom-up: 38 (22, 53), top-down: 15 (11, 18) Tg CH 4 -C y -1 ) and N 2 O (bottom-up: 0.7 (0.1, 1.3), top-down: 0.09 (-0.19, 0.37) Tg N 2 O-N yr -1 ). The combined global warming potential of all three gases (GWP-100) cannot be distinguished from neutral. Over shorter timescales (GWP-20), the region is a net GHG source because CH 4 dominates the total forcing. The net CO 2 sink in Boreal forests and wetlands is largely offset by fires and inland water CO 2 emissions as well as CH 4 emissions from wetlands and inland waters, with a smaller contribution from N 2 O emissions. Priorities for future research include the representation of inland waters in process-based models and the compilation of process-model ensembles for CH 4 and N 2 O. Discrepancies between bottom-up and top-down methods call for analyses of how prior flux ensembles impact inversion budgets, more and well-distributed in situ GHG measurements and improved resolution in upscaling techniques.

54 ENVIRONMENTAL SCIENCES↗

Genome-Resolved Metaproteomics Decodes the Microbial and Viral Contributions to Coupled Carbon and Nitrogen Cycling in River Sediments

Rivers have a significant role in global carbon and nitrogen cycles, serving as a nexus for nutrient transport between terrestrial and marine ecosystems. Although rivers have a small global surface area, they contribute substantially to worldwide greenhouse gas emissions through microbially mediated processes within the river hyporheic zone. Despite this importance, research linking microbial and viral communities to specific biogeochemical reactions is still nascent in these sediment environments. To survey the metabolic potential and gene expression underpinning carbon and nitrogen biogeochemical cycling in river sediments, we collected an integrated data set of 33 metagenomes, metaproteomes, and paired metabolomes. We reconstructed over 500 microbial metagenome-assembled genomes (MAGs), which we dereplicated into 55 unique, nearly complete medium- and high-quality MAGs spanning 12 bacterial and archaeal phyla. We also reconstructed 2,482 viral genomic contigs, which were dereplicated into 111 viral MAGs (vMAGs) of >10 kb in size. As a result of integrating gene expression data with geochemical and metabolite data, we created a conceptual model that uncovered new roles for microorganisms in organic matter decomposition, carbon sequestration, nitrogen mineralization, nitrification, and denitrification. We show how these metabolic pathways, integrated through shared resource pools of ammonium, carbon dioxide, and inorganic nitrogen, could ultimately contribute to carbon dioxide and nitrous oxide fluxes from hyporheic sediments. Further, by linking viral MAGs to these active microbial hosts, we provide some of the first insights into viral modulation of river sediment carbon and nitrogen cycling.

54 ENVIRONMENTAL SCIENCES↗

Isotopically Tracking Nitrogen Oxides, Nitrous Acid, And Nitric Acid, Particulate Nitrate from Wildfire During FIREX-AQ

Wildfires are an important source of reactive nitrogen species including nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO), as well as products such as nitric acid (HNO3) and particulate nitrate (p-NO3-). These species have strongly influence air quality and climate. In summer of 2019 (July 25 —August 21), as part of the FIREX-AQ ground mission, we drove ~3000 miles and sampled smoke of different ages in both daytime and nighttime from 5 different wildfires in the western US. Using recently developed methods that have been validated in both laboratory and field settings, we conducted high time resolution collection of NOx, NO2, HONO, HNO3, and p-NO3- for off-line characterization of isotopic composition δ15N, δ18O and Δ17O (=δ17O−0.52 δ18O). δ15N serves as a potential tracer for tracking sources and reactive nitrogen cycling pathways, δ18O and Δ17O provide key information about oxidation pathways (i.e. O3 versus RO2). Our measured δ15N for HONO ranges from -4.9‰ to +5.2‰ and -8‰ to +5.2‰ respectively, in the majority overlapping with our prior lab controlled burning results, which suggests the capability of δ15N for tracing the biomass burning emissions against other sources including vehicular emissions and soil emissions. In addition, our measurements show δ18O and Δ17O for NO2 and HONO vary significantly day vs night, as well as in young smoke vs aged smoke, likely reflecting different oxidizing mechanisms under different smoke conditions. Preliminary results of isotopic signatures of all the above reactive nitrogen species will be presented, and their relationships will be explored to identify wildfire derived reactive nitrogen source signatures and to constrain atmospheric processing pathways (e.g. secondary formation of HONO) for different fires under various smoke conditions depending on fuel types, fire conditions and meteorological conditions.

Jiajue Chai↗

Restoring wetlands on intensive agricultural lands modifies nitrogen cycling microbial communities and reduces N 2 O production potential

The concentration of nitrous oxide (N 2 O), an ozone-depleting greenhouse gas, is rapidly increasing in the atmosphere. Most atmospheric N 2 O originates in terrestrial ecosystems, of which the majority can be attributed to microbial cycling of nitrogen in agricultural soils. Here, in this study, we demonstrate how the abundance of nitrogen cycling genes vary across intensively managed agricultural fields and adjacent restored wetlands in the Sacramento-San Joaquin Delta in California, USA. We found that the abundances of nirS and nirK genes were highest at the intensively managed organic-rich cornfield and significantly outnumber any other gene abundances, suggesting very high N 2 O production potential. The quantity of nitrogen transforming genes, particularly those responsible for denitrification, nitrification and DNRA, were highest in the agricultural sites, whereas nitrogen fixation and ANAMMOX was strongly associated with the wetland sites. Although the abundance of nosZ genes was also high at the agricultural sites, the ratio of nosZ genes to nir genes was significantly higher in wetland sites indicating that these sites could act as a sink of N 2 O. These findings suggest that wetland restoration could be a promising natural climate solution not only for carbon sequestration but also for reduced N 2 O emissions.

59 BASIC BIOLOGICAL SCIENCES↗

Remote sounding of tropospheric minor constituents

The etalon interferometer, or Fabry-Perot interferometer (FPI), with its high throughput and high spectral resolution was widely used in the remote-sensing measurements of the earth's atmospheric composition, winds, and temperatures. The most recent satellite instruments include the Fabry-Perot interferometer flown on the Dynamics Explorer-2 (DE-2) and the High Resolution Doppler Imager (HRDI) to be flown on the Upper Atmosphere Research Satellite (UARS). These instruments measure the Doppler line profiles of the emission and absorption of certain atmospheric species (such as atomic oxygen) in the visible spectral region. The successful space flight of DE-FPI and the test and delivery of UARS-HRDI demonstrated the extremely high spectral resolution and ruggedness of the etalon system for the remote sensing of earth and planetary atmospheres. Recently, an innovative FPI focal plane detection technique called the Circle-to-Line Interferometer Optical (CLIO) system was invented at the Space Physics Research Laboratory (SPRL). The CLIO simplifies the FPI focal plane detection process by converting the circular rings or fringes into a linear pattern similar to that produced by a conventional spectrometer, while retaining the throughput advantage of the etalon interferometer. CLIO makes the use of linear array detectors more practical and efficient with FPI, the combination of FPI and CLIO represents a very promising new technique for the remote sensing of the lower atmospheres of Earth, Mars, Venus, Neptune, and other planets. The Multiorder Etalon Spectrometer (MOES), as a combination of the rugged etalon and the CLIO, compares very favorably to other spaceborne optical instruments in terms of performance versus complexity. The feasibility of an advanced etalon spectrometer for the remote sensing of tropospheric trace species, particularly carbon monoxide (CO), nitrous oxide (N2O), and methane (CH4) was discussed. The etalon atmospheric spectroscopy techniques are described, instrument design and related technical issues are discussed. The primary objective is to establish the concept of atmospheric spectroscopy with the CLIO and etalon system and its applications for the measurements of tropospheric trace species analyze system requirements and performance, determine the feasibility of components and subsystem implementation with available technology, and develop inversion algorithm for retrieval simulation and data analysis.

Drayson, S. Roland↗

A novel bacterial protein family that catalyses nitrous oxide reduction

Nitrous oxide (N 2 O), a driver of global warming and climate change, has reached unprecedented concentrations in Earth’s atmosphere. Current N 2 O sources outpace N 2 O sinks, emphasizing the need for comprehensive understanding of processes that consume N 2 O. Microbes that express the enzyme N 2 O reductase (N 2 OR) convert N 2 O to climate change-neutral dinitrogen (N 2 ). Known N 2 ORs belong to the canonical clade I and clade II NosZ reductases and are considered key enzymes for N 2 O reduction. Here we report a previously unrecognized protein family with a role in N 2 O reduction, clade III lactonase-type N 2 OR (L-N 2 OR), which diverges in sequence from canonical NosZ but conserves three-dimensional protein structural features. Integrated physiological, metagenomic, proteomic and structural modelling studies demonstrate that L-N 2 ORs catalyse N 2 O reduction. L-N 2 OR genes occur in several phyla, predominantly in uncultured taxa with broad geographic distribution. Our findings expand the known diversity of N 2 ORs and implicate previously unrecognized taxa (for example, Nitrospinota) in N 2 O consumption. In conclusion, the expansion of N 2 OR diversity and the identification of a novel type of catalyst for N 2 O reduction advances the understanding of N 2 O sinks, has implications for greenhouse gas emission and climate change modelling, and expands opportunities for innovative biotechnologies aimed at curbing N 2 O emissions.

He, Guang 何广 [Univ. of Tennessee, Knoxville, TN (U↗

A scalable framework for quantifying field-level agricultural carbon outcomes

Agriculture contributes nearly a quarter of global greenhouse gas (GHG) emissions, which is motivating interest in adopting certain farming practices that have the potential to reduce GHG emissions or sequester carbon in soil. The related GHG emission (including N 2 O and CH 4 ) and changes in soil carbon stock are defined here as “agricultural carbon outcomes”. Accurate quantification of agricultural carbon outcomes is the basis for achieving emission reductions for agriculture, but existing approaches for measuring carbon outcomes (including direct measurements, emission factors, and process-based modeling) fall short of achieving the required accuracy and scalability necessary to support credible, verifiable, and cost-effective measurement and improvement of these carbon outcomes. Here we propose a foundational and scalable framework to quantify field-level carbon outcomes for farmland, which is based on the holistic carbon balance of the agroecosystem: Agroecosystem Carbon Outcomes = Environment (E) × Management (M) × Crop (C). Following a comprehensive review of the scientific challenges associated with existing approaches, as well as their tradeoffs between cost and accuracy, we propose that the most viable path for the quantification of field-level carbon outcomes in agricultural land is through an effective integration of various approaches (e.g. diverse observations, sensor/in-situ data, and modeling), defined as the “System-of-Systems” solution. Such a “System-of-Systems” solution should simultaneously comprise the following components: (1) scalable collection of ground truth data and cross-scale sensing of environment variables (E), management practices (M), and crop conditions (C) at the local field level; (2) advanced modeling with necessary processes to support the quantification of carbon outcomes; (3) systematic Model-Data Fusion (MDF), i.e. robust and efficient methods to integrate sensing data and models at each local farmland level; (4) high computation efficiency and artificial intelligence (AI) to scale to millions of individual fields with low cost; and (5) robust and multi-tier validation systems and infrastructures to ensure solution fidelity and true scalability, i.e. the ability of a solution to perform robustly with accepted accuracy on all targeted fields. In this regard, we provide here the detailed scientific rationale, current progress, and future research and development (R&D) priorities to achieve different components of the “System-of-Systems” solution, thus accomplishing the Environment×Management×Crop framework to quantify field-level agricultural carbon outcomes.

54 ENVIRONMENTAL SCIENCES↗