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  1. ELM–Wet: Inclusion of a Wet–Landunit With Sub–Grid Representation of Eco–Hydrological Patches and Hydrological Forcing Improves Methane Emission Estimations in the E3SM Land Model (ELM)

    Wetlands are the largest emitters of biogenic methane (CH4) and represent the highest source of uncertainty in global CH4 budgets. Here, we aim to improve the realism of wetland representation in the U.S. Department of Energy's Exascale Earth System Model land surface model, ELM, thereby reducing uncertainty of CH4 flux predictions. We develop an updated version, ELM-Wet, where we activate a separate landunit for wetlands that handles multiple wetland-specific eco-hydrological patch functional types. We introduce more realistic hydrological forcing through prescribing site-level constraints on surface water elevation, which allows resolving different sustained inundation depth for different patches, and if data exists, prescribing inundation depth. We modified the calculation of aerenchyma transport diffusivity based on observed conductance per leaf area for different vegetation types. We use Bayesian Optimization to parameterize CO2 and CH4 fluxes in the developed wet-landunit. Site-level simulations of a coastal non-tidal freshwater wetland in Louisiana were performed with the updated model. Eddy covariance observations of CO2 and CH4 fluxes from 2012 to 2013 were used to train the model and data from 2021 were used for validation. Patch-specific chamber flux observations and observations of CH4 concentration profiles in the soil porewater from 2021 were used for evaluation of the model performance. Our results show that ELM-Wet reduces the model's CH4 emission root mean squared error by up to 33% and is able to represent inter-daily CO2 and CH4 flux variability across the wetland's eco-hydrological patches, including during periods of extreme dry or wet conditions.

  2. Molecular insights into the composition, sources, and aging of atmospheric brown carbon

    The light-absorbing chemical components of atmospheric organic aerosols are commonly referred to as Brown Carbon (BrC), reflecting the characteristic yellowish to brown appearance of aerosol. BrC is a highly complex mixture of organic compounds with diverse compositions and variable optical properties of its individual chromophores. BrC significantly influences the radiative budget of the climate and contributes to adverse air pollution effects such as reduced visibility and the presence of inhalable pollutants and irritants. However, a fundamental understanding of the sources, formation, and transformation (aging effects) of BrC remains incomplete. This gap in knowledge necessitates advanced chemical characterization of individual aerosol components and the correlation of their composition with optical properties. Over the past decade, a multi-modal analytical platform composed of high-performance liquid chromatography with a photodiode array UV-vis detector and high-resolution mass spectrometry has been extensively used for the untargeted analysis of BrC components in complex mixtures of atmospheric organic aerosols and their laboratory proxies. This method separates solvent-extractable BrC compounds into distinct fractions, each characterized by specific retention times, UV-vis absorption spectra, and elemental compositions, offering comprehensive molecular insights into BrC components. In this review, we highlight the application of this platform in analyzing both real-world aerosol samples and laboratory-generated proxies. These studies have identified composition-specific sources and transformations of BrC, advancing our understanding of these complex atmospheric mixtures. Atmospheric humic-like substances (HULIS), formed through cloud processing of wildfire smoke and the oligomerization of water-soluble organics, are key contributors to BrC. Additional HULIS originate from fossil fuel combustion, biogenic, and marine emissions. Key BrC chromophores include nitroaromatics, imidazoles, N-heterocycles, polyaromatic hydrocarbons, quinones, and others. Aging processes, including photolysis and multiphase reactions, can significantly alter BrC optical properties by generating new chromophores or degrading existing ones. The fundamental knowledge gained from these investigations is essential for assessing BrC optical properties. Additionally, it provides practical composition metrics necessary to inform and improve future atmospheric models, enabling more accurate predictions of BrC behavior and its impact on climate and air quality.

  3. Seasonal investigation of ultrafine-particle organic composition in an eastern Amazonian rainforest

    Reports on the composition of ultrafine particles (<100 nm in diameter) in the Amazon are scarce, due in part to the fact that new-particle formation has rarely been observed near ground level. Ultrafine particles near the surface have nevertheless been observed, leaving open questions regarding the sources and chemistry of their formation and growth, particularly as these vary across seasons. Here, we present measurements of the composition of ultrafine particles collected in the Tapajós National Forest (2.857°S, 54.959°W) during three different seasonal periods: 10–30 September 2016 (SEP), 18 November–23 December 2016 (DEC), and 22 May–21 June 2017 (JUN). Size-selected (5–70 nm) particles were collected daily (for 22 h each day) using an offline sampler. Samples collected during the three time periods were compiled and analyzed using liquid chromatography coupled with Orbitrap high-resolution mass spectrometry. Our findings suggest a sustained influence of isoprene organosulfate chemistry on ultrafine particles from the different periods. We present chemical evidence that indicates that biological-spore fragmentation impacted ultrafine-particle composition during the late wet season (JUN), while chemical markers for biomass burning and secondary chemistry peaked during the dry season (SEP and DEC). Higher oxidation states and degrees of unsaturation were observed for organics in the dry season (SEP and DEC), suggesting greater extents of aerosol aging. Finally, applying a volatility parameterization to the observed compounds suggests that organic sulfur species are likely key drivers of new-particle growth in the region due to their low volatility compared to other species.

  4. Cloud radiative effect dominates variabilities of surface energy budget in the dark Arctic

    Climate models simulate a wide range of temperatures in the Arctic. Here we investigate one of the main drivers of changes in surface temperature: the net surface heat flux in the models. We show that in the winter months of the dark Arctic, there is a more than two-fold difference in the net surface heat fluxes among the models, and this difference is dominated by the downward infrared radiation from clouds. Owing to the small amount of water vapor in the winter Arctic, infrared radiation from clouds transmits more easily to the surface in the Arctic than at other latitudes, resulting in large cloud radiative effect at the surface. The dominant role of the cloud effect is also found in the transient variability of the net surface heat flux. Results demonstrate that accurate simulation of clouds is crucial for determining the net surface heat flux, which in turn affects surface temperature and sea ice properties in the Arctic.

  5. Measurement report: A comparative analysis of an intensive incursion of fluorescing African dust particles over Puerto Rico and another over Spain

    Measurements during episodes of African dust, made with two wideband integrated bioaerosol spectrometers (WIBSs), one on the northeastern coast of Puerto Rico and the other in the city of León, Spain, show unmistakable, bioaerosol-like fluorescing aerosol particles (FAPs) that can be associated with these dust episodes. The Puerto Rico event occurred during a major incursion of African dust during June 2020. The León event occurred in the late winter and spring of 2022, when widespread, elevated layers of dust inundated the Iberian Peninsula. Satellite and back-trajectory analyses confirm that dust from northern Africa was the source of the particles during both events. The WIBSs measure the size of individual particles in the range from 0.5 to 30 µm, derive a shape factor, and classify seven types of fluorescence from the FAPs. In general, it is not possible to directly determine the specific biological identity from fluorescence signatures; however, measurements of these types of bioaerosols in laboratory studies allow us to compare ambient fluorescence patterns with whole microbial cells measured under controlled conditions. Here we introduce some new metrics that offer a more quantitative approach for comparing FAP characteristics derived from particles measured under different environmental conditions. The analysis highlights the similarities and differences at the two locations and reveals differences that can be attributed to the age and history of the dust plumes, e.g., the amount of time that the air masses were in the mixed layer and the frequency of precipitation along the air mass trajectory.

  6. Exploring Causal Relationships and Adjustment Timescales of Aerosol-Cloud Interactions in Geostationary Satellite Observations and CAM6 Using Wavelet Phase Coherence Analysis

    We present for the first time within the cloud physics context, the application of wavelet phase coherence analysis to disentangle counteracting physical processes associated with the lead-lag phase difference between cloud-proxy liquid water path (LWP) and aerosol-proxy cloud droplet number concentration (Nd) in an Eulerian framework using satellite-based observations and climate model outputs. This approach allows us to identify the causality and dominant adjustment timescales governing the correlation between LWP and Nd. Satellite observations indicate a more prevalent positive correlation between daytime LWP and Nd regardless of whether LWP leads or lags Nd. The positive cloud water response, associated with precipitation processes, typically occurs within 1 hr, while the negative response resulting from entrainment drying, usually takes 2–4 hr. CAM6 displays excessively rapid negative responses along with overly strong negative cloud water response and insufficient positive response, leading to a more negative correlation between LWP and Nd compared to observations.

  7. Systematic characterization of unknown compounds via dimensionality reduction of time series

    Analysis of ambient aerosols provides valuable insight into particle sources and formation chemistry. However, due to the complexity of atmospheric data and the dynamic nature of aerosol composition, a substantial fraction of data often become discarded by conventional analysis methods. Furthermore, a large fraction of chemical species within those data are unidentifiable due to a lack of matching spectral information, resulting in suboptimal characterization of chemical composition. Previous work has demonstrated techniques for cataloging analytes in a chromatographic dataset by deconvolution of mass spectra, but integration of these analytes throughout a large dataset remains time consuming. We present a method to automatically identify an ion for quantitation for single-ion chromatogram based peak fitting and integration, enabling comprehensive integration of analytes with minimal user interaction. The resulting time series are clustered with a machine-learning based dimensionality reduction technique to systematically investigate the underlying characteristics of the categorized analytes and gain new insights into the chemical composition and physicochemical properties of the unidentifiable analytes. We apply these methods to existing atmospheric datasets collected in Manacapuru, Brazil during the GoAmazon2014/5 campaign to identify new analytes and interpret their variability and transformations in the atmosphere. The analysis results generate 408 time series from cataloged analytes of interest, and the clustering of those time series with spherical k-means results in 8 distinct clusters. We find the analytes form clusters based on their distinct physicochemical properties, demonstrating the method’s ability to systematically identify and selectively filter contaminants and instrumental analytes and characterize the unidentifiable analytes.

  8. Air temperature and precipitation constraining the modelled wetland methane emissions in a boreal region in northern Europe

    Wetland methane responses to temperature and precipitation are studied in a boreal wetland-rich region in northern Europe using ecosystem process models. Six ecosystem models (JSBACH-HIMMELI, LPX-Bern, LPJ-GUESS, JULES, CLM4.5, and CLM5) are compared to multi-model means of ecosystem models and atmospheric inversions from the Global Carbon Project and upscaled eddy covariance flux results for their temperature and precipitation responses and seasonal cycles of the regional fluxes. Two models with contrasting response patterns, LPX-Bern and JSBACH-HIMMELI, are used as priors in atmospheric inversions with Carbon Tracker Europe–CH4 (CTE-CH4) in order to find out how the assimilation of atmospheric concentration data changes the flux estimates and how this alters the interpretation of the flux responses to temperature and precipitation. Inversion moves wetland emissions of both models towards co-limitation by temperature and precipitation. Between 2000 and 2018, periods of high temperature and/or high precipitation often resulted in increased emissions. However, the dry summer of 2018 did not result in increased emissions despite the high temperatures. The process models show strong temperature and strong precipitation responses for the region (51 %–91 % of the variance explained by both). The month with the highest emissions varies from May to September among the models. However, multi-model means, inversions, and upscaled eddy covariance flux observations agree on the month of maximum emissions and are co-limited by temperature and precipitation. The setup of different emission components (peatland emissions, mineral land fluxes) has an important role in building up the response patterns. Considering the significant differences among the models, it is essential to pay more attention to the regional representation of wet and dry mineral soils and periodic flooding which contribute to the seasonality and magnitude of methane fluxes. The realistic representation of temperature dependence of the peat soil fluxes is also important. Furthermore, it is important to use process-based descriptions for both mineral and peat soil fluxes to simulate the flux responses to climate drivers.

  9. Atmospheric River Frequency-Category Characteristics Shape U.S. West Coast Runoff

    Abstractrunoff response to atmospheric rivers (ARs) over the U.S. West Coast. We focused on runoff time series variations impacted by AR characteristics (e.g., category and frequency) and land preconditions during Northern Hemisphere cool seasons in the period of 1940–2023. Results show that high-category ARs significantly increase local runoff with higher hourly precipitation rates leading to a greater incremental rate and peak runoff. Extreme runoff increases greatly with the AR category with an increase rate up to 12.5 times stronger than non-extreme runoff. Besides the AR category, land preconditions such as soil moisture and snowpack also play crucial roles in modulating runoff response. We found that runoff induced by weak-category ARs is more sensitive to land preconditions than high-category ARs, with high peak runoff occurring when soil is nearly saturated. Additionally, more than 50% of high-peak-runoff events in snow-covered grid cells are associated with rain-on-snow events particularly for the events associated with weaker ARs. Regression analysis reveals that AR precipitation and land preconditions jointly influence runoff, emphasizing the importance of including soil moisture and snowpack levels in AR impact assessments. The study also highlights the intensified runoff response to back-to-back ARs with short intervals, which may become more frequent with climate warming, posing increased flood risks via facilitating wet soil conditions. Our findings have significant implications for AR risk predictions and the development of prediction models for AR-induced runoff.

  10. Soil moisture controls over carbon sequestration and greenhouse gas emissions: a review

    This literature review synthesizes the role of soil moisture in regulating carbon sequestration and greenhouse gas emissions (CS-GHG). Soil moisture directly affects photosynthesis, respiration, microbial activity, and soil organic matter dynamics, with optimal levels enhancing carbon storage while extremes, such as drought and flooding, disrupt these processes. A quantitative analysis is provided on the effects of soil moisture on CS-GHG across various ecosystems and climatic conditions, highlighting a “Peak and Decline” pattern for CO2 emissions at 40% water-filled pore space (WFPS), while CH4 and N2O emissions peak at higher levels (60–80% and around 80% WFPS, respectively). The review also examines ecosystem models, discussing how soil moisture dynamics are incorporated to simulate photosynthesis, microbial activity, and nutrient cycling. Sustainable soil moisture management practices, including conservation agriculture, agroforestry, and optimized water management, prove effective in enhancing carbon sequestration and mitigating GHG emissions by maintaining ideal soil moisture levels. The review further emphasizes the importance of advancing multiscale observations and feedback modeling through high-resolution remote sensing and ground-based data integration, as well as hybrid modeling frameworks. The interactive model-experiment framework emerges as a promising approach for linking experimental data with model refinement, enabling continuous improvement of CS-GHG predictions. From a policy perspective, shifting focus from short-term agricultural productivity to long-term carbon sequestration is crucial. Achieving this shift will require financial incentives, robust monitoring systems, and collaboration among stakeholders to ensure sustainable practices effectively contribute to climate mitigation goals.


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