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Creators/Authors contains: "Chen, Ning"

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  1. Abstract Microbial processes are crucial in producing and oxidizing biological methane (CH4) in natural wetlands. Therefore, modeling methanogenesis and methanotrophy is advantageous for accurately projecting CH4cycling. Utilizing the CLM‐Microbe model, which explicitly represents the growth and death of methanogens and methanotrophs, we demonstrate that genome‐enabled model parameterization improves model performance in four natural wetlands. Compared to the default model parameterization against CH4flux, genomic‐enabled model parameterization added another contain on microbial biomass, notably enhancing the precision of simulated CH4flux. Specifically, the coefficient of determination (R2) increased from 0.45 to 0.74 for Sanjiang Plain, from 0.78 to 0.89 for Changbai Mountain, and from 0.35 to 0.54 for Sallie's Fen, respectively. A drop inR2was observed for the Dajiuhu nature wetland, primarily caused by scatter data points. Theil's coefficient (U) and model efficiency (ME) confirmed the model performance from default parameterization to genome‐enabled model parameterization. Compared with the model solely calibrated to surface CH4flux, additional constraints of functional gene data led to better CH4seasonality; meanwhile, genome‐enabled model parameterization established more robust associations between simulated CH4production rates and environmental factors. Sensitivity analysis underscored the pivotal role of microbial physiology in governing CH4flux. This genome‐enabled model parameterization offers a valuable promise to integrate fast‐cumulating genomic data with CH4models to better understand microbial roles in CH4in the era of climate change. 
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  2. Abstract Recent studies have reported worldwide vegetation suppression in response to increasing atmospheric vapor pressure deficit (VPD). Here, we integrate multisource datasets to show that increasing VPD caused by warming alone does not suppress vegetation growth in northern peatlands. A site-level manipulation experiment and a multiple-site synthesis find a neutral impact of rising VPD on vegetation growth; regional analysis manifests a strong declining gradient of VPD suppression impacts from sparsely distributed peatland to densely distributed peatland. The major mechanism adopted by plants in response to rising VPD is the “open” water-use strategy, where stomatal regulation is relaxed to maximize carbon uptake. These unique surface characteristics evolve in the wet soil‒air environment in the northern peatlands. The neutral VPD impacts observed in northern peatlands contrast with the vegetation suppression reported in global nonpeatland areas under rising VPD caused by concurrent warming and decreasing relative humidity, suggesting model improvement for representing VPD impacts in northern peatlands remains necessary. 
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  3. Abstract Actinide diatomic molecules are ideal models to study elusive actinide multiple bonds, but most of these diatomic molecules have so far only been studied in solid inert gas matrices. Herein, we report a charged U≡N diatomic species captured in fullerene cages and stabilized by the U-fullerene coordination interaction. Two diatomic clusterfullerenes, viz. UN@Cs(6)-C82and UN@C2(5)-C82, were successfully synthesized and characterized. Crystallographic analysis reveals U-N bond lengths of 1.760(7) and 1.760(20) Å in UN@Cs(6)-C82and UN@C2(5)-C82. Moreover, U≡N was found to be immobilized and coordinated to the fullerene cages at 100 K but it rotates inside the cage at 273 K. Quantum-chemical calculations show a (UN)2+@(C82)2−electronic structure with formal +5 oxidation state (f1) of U and unambiguously demonstrate the presence of a U≡N bond in the clusterfullerenes. This study constitutes an approach to stabilize fundamentally important actinide multiply bonded species. 
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  4. Context.The methyl cation (CH3+) has recently been discovered in the interstellar medium through the detection of 7 μm (1400 cm−1) features toward the d203-506 protoplanetary disk by the JWST. Line-by-line spectroscopic assignments of these features, however, were unsuccessful due to complex intramolecular perturbations preventing a determination of the excitation and abundance of the species in that source. Aims.Comprehensive rovibrational assignments guided by theoretical and experimental laboratory techniques provide insight into the excitation mechanisms and chemistry of CH3+in d203-506. Methods.The rovibrational structure of CH3+was studied theoretically by a combination of coupled-cluster electronic structure theory and (quasi-)variational nuclear motion calculations. Two experimental techniques were used to confirm the rovibrational structure of CH3+:(1) infrared leak-out spectroscopy of the methyl cation, and (2) rotationally resolved photoelectron spectroscopy of the methyl radical (CH3). In (1), CH3+ions, produced by the electron impact dissociative ionization of methane, were injected into a 22-pole ion trap where they were probed by the pulses of infrared radiation from the FELIX free electron laser. In (2), neutral CH3, produced by CH3NO2pyrolysis in a molecular beam, was probed by pulsed-field ionization zero-kinetic-energy photoelectron spectroscopy. Results.The quantum chemical calculations performed in this study have enabled a comprehensive spectroscopic assignment of thev2+andv4+bands of CH3+detected by the JWST. The resulting spectroscopic constants and derived EinsteinAcoefficients fully reproduce both the infrared and photoelectron spectra and permit the rotational temperature of CH3+(T= 660 ± 80 K) in d203-506 to be derived. A beam-averaged column density of CH3+in this protoplanetary disk is also estimated. 
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