Search

Ocean observational gridded products are vital for climate monitoring, ocean and climate research, model evaluation, and supporting climate mitigation and adaptation measures. This paper describes the 4th version of the Institute of Atmospheric Physics (IAPv4) ocean temperature and ocean heat content (OHC) objective analysis product. It accounts for recent developments in quality control (QC) procedures, climatology, bias correction, vertical and horizontal interpolation, and mapping and is available for the upper 6000 m (119 levels) since 1940 (more reliable after ∼ 1957) for monthly and 1°×1° temporal and spatial resolutions. IAPv4 is compared with the previous version, IAPv3, and with the other data products, sea surface temperatures (SSTs), and satellite observations. It has a slightly stronger long-term upper 2000 m OHC increase than IAPv3 for 1955–2023, mainly because of newly developed bias corrections. The IAPv4 0–2000 m OHC trend is also higher during 2005–2023 than IAPv3, mainly because of the QC process update. The uppermost level of IAPv4 is consistent with independent SST datasets. The month-to-month OHC variability for IAPv4 is desirably less than IAPv3 and the other OHC products investigated in this study, the trend of ocean warming rate (i.e., warming acceleration) is more consistent with the net energy imbalance at the top of the atmosphere than IAPv3, and the sea level budget can be closed within uncertainty. The gridded product is freely accessible at https://doi.org/10.12157/IOCAS.20240117.002 for temperature data (Cheng et al., 2024a) and at https://doi.org/10.12157/IOCAS.20240117.001 for ocean heat content data (Cheng et al., 2024b).

SUMMARY: An experiment was conducted to evaluate the effects of pure benzoic acid (PBA) or enteric-released benzoic acid (EBA) on performance, intestinal histology, apparent ileal digestibility (AID), cecal coliform and enterococci abundance, and litter moisture of broilers raised on used litter. Day-old male broiler chicks were assigned to control (Con), nontreated diet; positive control (BMD), Con + 50 ppm bacitracin methylene disalicylate; PBA, Con +1,000 ppm of PBA; EBA, Con +330 ppm of EBA. From 0 to 28 and 0 to 42 d, BMD outperformed the Con in either BW gain (BWG) or mortality corrected FCR (FCRm) (P ≤ 0.05). Over 0 to 28 d, EBA and PBA improved BWG and FCRm compared to the Con (P ≤ 0.05). When the entire 0 to 42 d period was considered, EBA improved both BWG and FCRm in comparison to Con (P ≤ 0.05). Supplementation with EBA and PBA resulted in inconsistent responses in duodenum and jejunum morphology; specifically, PBA decreased 28 d duodenal crypt depth and increased villus height to crypt depth ratio, while EBA decreased 28 d jejunum crypt depth (P ≤ 0.05). There were no differences in AID or cecal coliform counts (P > 0.05) due to treatment. However, PBA significantly reduced enterococcus counts at 42 d by 0.48 Log10 CFU/g compared to CON. These results suggest that EBA can increase BWG and decrease FCRm, while PBA performance was similar to CON. Additionally, benzoic acid decreased crypt depth, with the response being tissue-specific depending on the form of benzoic used.

Streamflow variability plays a crucial role in shaping the dynamics and sustainability of Earth's ecosystems, which can be simulated and projected by a river routing model coupled with a land surface model. However, the simulation of streamflow at large scales is subject to considerable uncertainties, primarily arising from two related processes: runoff generation (hydrological process) and river routing (hydraulic process). While both processes have impacts on streamflow variability, previous studies only calibrated one of the two processes to reduce biases in the simulated streamflow. Calibration focusing only on one process can result in unrealistic parameter values to compensate for the bias resulting from the other process; thus other water-related variables remain poorly simulated. In this study, we performed several experiments with the land and river components of the Energy Exascale Earth System Model (E3SM) over the Pantanal region to disentangle the hydrological and hydraulic controls on streamflow variability in coupled land–river simulations. Our results show that the generation of subsurface runoff is the most important factor for streamflow variability contributed by the runoff generation process, while floodplain storage effect and main-channel roughness have significant impacts on streamflow variability through the river routing process. We further propose a two-step procedure to robustly calibrate the two processes together. The impacts of runoff generation and river routing on streamflow are appropriately addressed with the two-step calibration, which may be adopted by developers of land surface and earth system models to improve the modeling of streamflow.

HONO is an important precursor for OH radicals that impact secondary-pollutant production. However, there are still large uncertainties about different HONO sources which hinder accurate predictions of HONO concentration and hence atmospheric oxidation capacity. Here HONO was measured during the EXPLORE-YRD campaign (EXPeriment on the eLucidation of the atmospheric Oxidation capacity and aerosol foRmation and their Effects in the Yangtze River Delta), along with other important parameters, enabling us to comprehensively investigate HONO variation characteristics and evaluate the relative importance of different HONO sources by using a box model. HONO showed significant variations, ranging from several tens of parts per thousand to 4.4 ppb. The average diurnal pattern of HONO / NOx showed a maximum of 0.17 around noon and resembled that of j(O1D), indicating the existence of photo-induced sources. Modeling simulations with only the default HONO source (OH + NO) largely underestimated HONO concentrations, with the modeled-averaged noontime HONO concentration an order of magnitude lower than the observed concentration. The calculated strength of the unknown HONO source (Punknown) showed a nearly symmetrical diurnal profile with a maximum of 2.5 ppb h−1 around noon. The correlation analysis and sensitivity tests showed that the photo-induced NO2 conversion on the ground was able to explain Punknown. Additional HONO sources incorporated into the box model improved the model's performance in simulating HONO concentrations. The revised box model reproduced the nighttime HONO concentration well but still underestimated the daytime HONO concentration. Further sensitivity tests indicated the underestimation of daytime HONO was not due to uncertainties of photo-induced NO2 uptake coefficients on the ground or aerosol surfaces or the enhancement factor of nitrate photolysis but was more likely due to other sources that were not considered in the model. Among the incorporated HONO sources and the default gas-phase source, photo-induced NO2 conversion on the ground dominated the modeled HONO production during the daytime, accounting for 71 % of the total, followed by NO + OH, NO2 hydrolysis on the ground surface, vehicle emissions, photo-induced NO2 conversion on the aerosol surface, nitrate photolysis and NO2 hydrolysis on the aerosol surface. NO2 hydrolysis on the ground surface was the major source of nighttime HONO, contributing 55 % of total HONO production. HONO photolysis contributed 43 % of ROx production during the daytime, followed by O3 photolysis (17 %), HCHO photolysis (14 %), ozonolysis of alkenes (12 %) and carbonyl photolysis (10 %). With observed HONO as a model constraint, the average peak of net ozone production rate increased by 88 % to 12.6 ppb h−1 compared to that without observed HONO as a model constraint, indicating HONO evidently enhanced O3 production and hence aggravated O3 pollution in summer seasons. Our study emphasized the importance of heterogeneous NO2 conversion on the ground surface in HONO production and accurate parameterization of HONO sources in predicting secondary-pollutant production.

Compound flooding is a type of flood event caused by multiple flood drivers. The associated risk has usually been assessed using statistics-based analyses or hydrodynamics-based numerical models. This study proposes a compound flood (CF) risk assessment (CFRA) framework for coastal regions in the contiguous United States (CONUS). In this framework, a large-scale river model is coupled with a global ocean reanalysis dataset to (a) evaluate the CF exposure related to the coastal backwater effects on river basins, and (b) generate spatially distributed data for analyzing the CF hazard using a bivariate statistical model of river discharge and storm surge. The two kinds of risk are also combined to achieve a holistic understanding of the continental-scale CF risk. The estimated CF risk shows remarkable inter- and intra-basin variabilities along the CONUS coast with more variabilities in the CF hazard over the US west and Gulf coastal basins. Different risk assessment methods present significantly different patterns in a few key regions such as the San Francisco Bay area, the lower Mississippi River, and Puget Sound. Our results highlight the need to weigh different CF risk measures and avoid using single statistics-based or hydrodynamics-based CFRAs. Uncertainty sources in these CFRAs include the use of gauge observations, which cannot account for the flow physics or resolve the spatial variability of risks, and underestimations of the flood extremes and the dependence of CF drivers in large-scale models, highlighting the importance of understanding the CF risks for developing a more robust CFRA.

Carbonyl sulfide (OCS), the most abundant sulfur gas in the Earth's atmosphere, is a greenhouse gas, a precursor to stratospheric sulfate aerosol, and a proxy for terrestrial CO2 uptake. Estimates of important OCS sources and sinks still have significant uncertainties and the global budget is not considered closed. One particularly uncertain source term, the OCS production during the atmospheric oxidation of dimethyl sulfide (DMS) emitted by the oceans, is addressed by a series of experiments in the atmospheric simulation chamber SAPHIR in conditions comparable to the remote marine atmosphere. DMS oxidation was initiated with OH and/or Cl radicals and DMS, OCS, and several oxidation products and intermediates were measured, including hydroperoxymethyl thioformate (HPMTF), which was recently found to play a key role in DMS oxidation in the marine atmosphere. One important finding is that the onset of HPMTF and OCS formation occurred faster than expected from the current chemical mechanisms. In agreement with other recent studies, OCS yields between 9 % and 12 % were observed in our experiments. Such yields are substantially higher than the 0.7 % yield measured in laboratory experiments in the 1990s, which is generally used to estimate the indirect OCS source from DMS in global budget estimates. However, we do not expect the higher yields found in our experiments to directly translate into a substantially higher OCS source from DMS oxidation in the real atmosphere, where conditions are highly variable, and, as pointed out in recent work, heterogeneous HPMTF loss is expected to effectively limit OCS production via this pathway. Together with other experimental studies, our results will be helpful to further elucidate the DMS oxidation chemical mechanism and in particular the paths leading to OCS formation.

Land–atmosphere (L–A) interactions encompass the co-evolution of the land surface and overlying planetary boundary layer, primarily during daylight hours. However, many studies have been conducted using monthly or entire-day mean time series due to the lack of subdaily data. It is unclear whether the inclusion of nighttime data alters the assessment of L–A coupling or obscures L–A interactive processes. To address this question, we generate monthly (M), entire-day mean (E), and daytime-only mean (D) data based on the ERA5 (5th European Centre for Medium-Range Weather Forecasts reanalysis) product and evaluate the strength of L–A coupling through two-legged metrics, which partition the impact of the land states on surface fluxes (the land leg) from the impact of surface fluxes on the atmospheric states (the atmospheric leg). Here we show that the spatial patterns of strong L–A coupling regions among the M-, D-, and E-based diagnoses can differ by more than 80 %. The signal loss from E- to M-based diagnoses is determined by the memory of local L–A states. The differences between E- and D-based diagnoses can be driven by physical mechanisms or averaging algorithms. To improve understanding of L–A interactions, we call attention to the urgent need for more high-frequency data from both simulations and observations for relevant diagnoses. Regarding model outputs, two approaches are proposed to resolve the storage dilemma for high-frequency data: (1) integration of L–A metrics within Earth system models, and (2) producing alternative daily datasets based on different averaging algorithms.

Photochemical processes in ambient air were studied using the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich, Germany. Ambient air was continuously drawn into the chamber through a 50 m high inlet line and passed through the chamber for 1 month in each season throughout 2019. The residence time of the air inside the chamber was about 1 h. As the research center is surrounded by a mixed deciduous forest and is located close to the city Jülich, the sampled air was influenced by both anthropogenic and biogenic emissions. Measurements of hydroxyl (OH), hydroperoxyl (HO2), and organic peroxy (RO2) radicals were achieved by a laser-induced fluorescence instrument. The radical measurements together with measurements of OH reactivity (kOH, the inverse of the OH lifetime) and a comprehensive set of trace gas concentrations and aerosol properties allowed for the investigation of the seasonal and diurnal variation of radical production and destruction pathways. In spring and summer periods, median OH concentrations reached 6 × 106 cm−3 at noon, and median concentrations of both HO2 and RO2 radicals were 3 × 108 cm−3. The measured OH reactivity was between 4 and 18 s−1 in both seasons. The total reaction rate of peroxy radicals with NO was found to be consistent with production rates of odd oxygen (Ox= NO2 + O3) determined from NO2 and O3 concentration measurements. The chemical budgets of radicals were analyzed for the spring and summer seasons, when peroxy radical concentrations were above the detection limit. For most conditions, the concentrations of radicals were mainly sustained by the regeneration of OH via reactions of HO2 and RO2 radicals with nitric oxide (NO). The median diurnal profiles of the total radical production and destruction rates showed maxima between 3 and 6 ppbv h−1 for OH, HO2, and RO2. Total ROX (OH, HO2, and RO2) initiation and termination rates were below 3 ppbv h−1. The highest OH radical turnover rate of 13 ppbv h−1 was observed during a high-temperature (max. 40 ∘C) period in August. In this period, the highest HO2, RO2, and ROX turnover rates were around 11, 10, and 4 ppbv h−1, respectively. When NO mixing ratios were between 1 and 3 ppbv, OH and HO2 production and destruction rates were balanced, but unexplained RO2 and ROX production reactions with median rates of 2 and 0.4 ppbv h−1, respectively, were required to balance their destruction. For NO mixing ratios above 3 ppbv, the peroxy radical reaction rates with NO were highly uncertain due to the low peroxy radical concentrations close to the limit of NO interferences in the HO2 and RO2 measurements. For NO mixing ratios below 1 ppbv, a missing source for OH and a missing sink for HO2 were found with maximum rates of 3.0 and 2.0 ppbv h−1, respectively. The missing OH source likely consisted of a combination of a missing inter-radical HO2 to OH conversion reaction (up to 2 ppbv h−1) and a missing primary radical source (0.5–1.4 ppbv h−1). The dataset collected in this campaign allowed analyzing the potential impact of OH regeneration from RO2 isomerization reactions from isoprene, HO2 uptake on aerosol, and RO2 production from chlorine chemistry on radical production and destruction rates. These processes were negligible for the chemical conditions encountered in this study.

Coastal backwater effects are caused by the downstream water level increase as a result of elevated sea level, high river discharge and their compounding influence. Such effects have crucial impacts on floods in densely populated regions but have not been well represented in large-scale river models used in Earth system models (ESMs), partly due to model mesh deficiency and oversimplifications of river hydrodynamics. Using two mid-Atlantic river basins as a testbed, we perform the first attempt to simulate the backwater effects comprehensively over a coastal region using the MOSART river transport model under an ESM framework, i.e., Energy Exascale Earth System Model (E3SM) configured on a regionally refined unstructured mesh, with a focus on understanding the backwater drivers and their long-term variations. By including sea level variations at the river downstream boundary, the model performance in capturing backwaters is greatly improved. We also propose a new flood event selection scheme to facilitate the decomposition of backwater drivers into different components. Our results show that while storm surge is a key driver, the influence of extreme discharge cannot be neglected, particularly when the river drains to a narrow river-like estuary. Compound flooding, while not necessarily increasing the flood peaks, exacerbates the flood risk by extending the duration of multiple coastal and fluvial processes. Furthermore, our simulations and analysis highlight the increasing strength of backwater effects due to sea level rise and more frequent storm surge during 1990–2019. Thus, backwaters need to be properly represented in ESMs to improve the predictive understanding of coastal flooding.

Ambient measurements of nitryl chloride (ClNO2) were performed at a rural site in Germany, covering three periods in winter, summer, and autumn 2019, as part of the JULIAC campaign (Jülich Atmospheric Chemistry Project) that aimed to understand the photochemical processes in air masses typical of midwestern Europe. Measurements were conducted at 50 m aboveground, which was mainly located in the nocturnal boundary layer and thus uncoupled from local surface emissions. ClNO2 is produced at night by the heterogeneous reaction of dinitrogen pentoxide (N2O5) on chloride (Cl−) that contains aerosol. Its photolysis during the day is of general interest, as it produces chlorine (Cl) atoms that react with different atmospheric trace gases to form radicals. The highest-observed ClNO2 mixing ratio was 1.6 ppbv (parts per billion by volume; 15 min average) during the night of 20 September. Air masses reaching the measurement site either originated from long-range transport from the southwest and had an oceanic influence or circulated in the nearby region and were influenced by anthropogenic activities. Nocturnal maximum ClNO2 mixing ratios were around 0.2 ppbv if originating from long-range transport in nearly all seasons, while the values were higher, ranging from 0.4 to 0.6 ppbv for regionally influenced air. The chemical composition of long-range transported air was similar in all investigated seasons, while the regional air exhibited larger differences between the seasons. The N2O5 necessary for ClNO2 formation comes from the reaction of nitrate radicals (NO3) with nitrogen dioxide (NO2), where NO3 itself is formed by a reaction of NO2 with ozone (O3). Measured concentrations of ClNO2, NO2, and O3 were used to quantify ClNO2 production efficiencies, i.e., the yield of ClNO2 formation per NO3 radical formed, and a box model was used to examine the idealized dependence of ClNO2 on the observed nocturnal O3 and NO2 concentrations. Results indicate that ClNO2 production efficiency was most sensitive to the availability of NO2 rather than that of O3 and increased with decreasing temperature. The average ClNO2 production efficiency was highest in February and September, with values of 18 %, and was lowest in December, with values of 3 %. The average ClNO2 production efficiencies were in the range of 3 % and 6 % from August to November for air masses originating from long-range transportation. These numbers are at the high end of values reported in the literature, indicating the importance of ClNO2 chemistry in rural environments in midwestern Europe.

The ambient radical concentrations were measured continuously by laser-induced fluorescence during the STORM (STudy of the Ozone foRmation Mechanism) campaign at the Shenzhen site, located in the Pearl River Delta in China, in the autumn of 2018. The diurnal maxima were 4.5×106 cm−3 for OH radicals and 4.2×108 cm−3 for HO2 radicals (including an estimated interference of 23 %–28 % from RO2 radicals during the daytime), respectively. The state-of-the-art chemical mechanism underestimated the observed OH concentration, similar to the other warm-season campaigns in China. The OH underestimation was attributable to the missing OH sources, which can be explained by the X mechanism. Good agreement between the observed and modeled OH concentrations was achieved when an additional numerical X equivalent to 0.1 ppb NO concentrations was added into the base model. The isomerization mechanism of RO2 derived from isoprene contributed approximately 7 % to the missing OH production rate, and the oxidation of isoprene oxidation products (MACR and MVK) had no significant impact on the missing OH sources, demonstrating further exploration of unknown OH sources is necessary. A significant HO2 heterogeneous uptake was found in this study, with an effective uptake coefficient of 0.3. The model with the HO2 heterogeneous uptake can simultaneously reproduce the OH and HO2 concentrations when the amount of X changed from 0.1 to 0.25 ppb. The ROx primary production rate was dominated by photolysis reactions, in which the HONO, O3, HCHO, and carbonyls photolysis accounted for 29 %, 16 %, 16 %, and 11 % during the daytime, respectively. The ROx termination rate was dominated by the reaction of OH+NO2 in the morning, and thereafter the radical self-combination gradually became the major sink of ROx in the afternoon. As the sum of the respective oxidation rates of the pollutants via reactions with oxidants, the atmospheric oxidation capacity was evaluated, with a peak of 11.8 ppb h−1 around noontime. The ratio of P(O3)net to AOCVOCs, which indicates the yield of net ozone production from VOC oxidation, trended to increase and then decrease as the NO concentration increased. The median ratios ranged within 1.0–4.5, with the maximum existing when the NO concentration was approximately 1 ppb. The nonlinear relationship between the yield of net ozone production from VOC oxidation and NO concentrations demonstrated that optimizing the NOx and VOC control strategies is critical to controlling ozone pollution effectively in the future.

Empirical evidence demonstrates that lakes and reservoirs are warming across the globe. Consequently, there is an increased need to project future changes in lake thermal structure and resulting changes in lake biogeochemistry in order to plan for the likely impacts. Previous studies of the impacts of climate change on lakes have often relied on a single model forced with limited scenario-driven projections of future climate for a relatively small number of lakes. As a result, our understanding of the effects of climate change on lakes is fragmentary, based on scattered studies using different data sources and modelling protocols, and mainly focused on individual lakes or lake regions. This has precluded identification of the main impacts of climate change on lakes at global and regional scales and has likely contributed to the lack of lake water quality considerations in policy-relevant documents, such as the Assessment Reports of the Intergovernmental Panel on Climate Change (IPCC). Here, we describe a simulation protocol developed by the Lake Sector of the Inter-Sectoral Impact Model Intercomparison Project (ISIMIP) for simulating climate change impacts on lakes using an ensemble of lake models and climate change scenarios for ISIMIP phases 2 and 3. The protocol prescribes lake simulations driven by climate forcing from gridded observations and different Earth system models under various representative greenhouse gas concentration pathways (RCPs), all consistently bias-corrected on a 0.5∘ × 0.5∘ global grid. In ISIMIP phase 2, 11 lake models were forced with these data to project the thermal structure of 62 well-studied lakes where data were available for calibration under historical conditions, and using uncalibrated models for 17 500 lakes defined for all global grid cells containing lakes. In ISIMIP phase 3, this approach was expanded to consider more lakes, more models, and more processes. The ISIMIP Lake Sector is the largest international effort to project future water temperature, thermal structure, and ice phenology of lakes at local and global scales and paves the way for future simulations of the impacts of climate change on water quality and biogeochemistry in lakes.

The first OH and HO2 radical observation in Yangtze River Delta, one of the four major urban agglomerations in China, was carried out at a suburban site (Taizhou) in summer 2018 from May to June, aiming to elucidate the atmospheric oxidation capacity in this region. The maximum diurnal averaged OH and HO2 concentrations were 1.0×107 and 1.1×109 cm−3, respectively, which were the second highest HOx (sum of OH and HO2) radical concentrations observed in China. HONO photolysis was the dominant radical primary source, accounting for 42 % of the total radical initiation rate. Other contributions were from carbonyl photolysis (including HCHO, 24 %), O3 photolysis (17 %), alkene ozonolysis (14 %), and NO3 oxidation (3 %). A chemical box model based on the RACM2-LIM1 mechanism could generally reproduce the observed HOx radicals, but systematic discrepancy remained in the afternoon for the OH radical, when the NO mixing ratio was less than 0.3 ppb. An additional recycling mechanism equivalent to 100 ppt NO was capable to fill the gap. The sum of monoterpenes was on average up to 0.4 ppb during daytime, which was all allocated to α-pinene in the base model. A sensitivity test without monoterpene input showed the modeled OH and HO2 concentrations would increase by 7 % and 4 %, respectively, but modeled RO2 concentration would significantly decrease by 23 %, indicating that monoterpene was an important precursor of RO2 radicals in this study. Consequently, the daily integrated net ozone production would reduce by 6.3 ppb without monoterpene input, proving the significant role of monoterpene in the photochemical O3 production in this study. In addition, the generally good agreement between observed and modeled HOx concentrations suggested no significant HO2 heterogeneous uptake process during this campaign. Incorporation of HO2 heterogeneous uptake process would worsen the agreement between HOx radical observation and simulation, and the discrepancy would be beyond the combined measurement–model uncertainties using an effective uptake coefficient of 0.2. Finally, the ozone production efficiency (OPE) was only 1.7 in this study, a few folds lower than other studies in (sub)urban environments. The low OPE indicated a slow radical propagation rate and short chain length. As a consequence, ozone formation was suppressed by the low NO concentration in this study.

Sedimentary charcoal records are widely used to reconstruct regional changes in fire regimes through time in the geological past. Existing global compilations are not geographically comprehensive and do not provide consistent metadata for all sites. Furthermore, the age models provided for these records are not harmonised and many are based on older calibrations of the radiocarbon ages. These issues limit the use of existing compilations for research into past fire regimes. Here, we present an expanded database of charcoal records, accompanied by new age models based on recalibration of radiocarbon ages using IntCal20 and Bayesian age-modelling software. We document the structure and contents of the database, the construction of the age models, and the quality control measures applied. We also record the expansion of geographical coverage relative to previous charcoal compilations and the expansion of metadata that can be used to inform analyses. This first version of the Reading Palaeofire Database contains 1676 records (entities) from 1480 sites worldwide. The database (RPDv1b – Harrison et al., 2021) is available at https://doi.org/10.17864/1947.000345.

Suspended sediment plays a vital role in the regional and global cycling of carbon and nutrients by carrying carbon and nutrients from headwaters into lowland rivers and the oceans. Sediment transport through river systems is often fundamentally modified by human activities such as reservoir management. However, a physically based representation of sediment transport is still missing in most existing Earth system models (ESMs), which are essential tools for modeling and predicting Earth system changes. Here, we introduce a multi-process river sediment module for ESMs, which includes (1) hillslope soil erosion and sediment discharge into streams, (2) sediment transport processes through river networks, (3) reservoir operation based on the inflows from upstream areas and water demand from downstream areas, and (4) sediment trapping by reservoirs. All model parameters are estimated a priori without calibration. We apply this new sediment modeling framework to the contiguous United States and validate it against historical observations of monthly streamflow and sediment discharges at 35 river gauges. The model reasonably well captures the long-term balance and seasonal variations of suspended sediment in large river systems. Furthermore, our model results show that suspended sediment discharge in managed rivers is affected more by reservoirs' direct trapping of sediment particles than by their flow regulation. This new sediment module enables future modeling of the transportation and transformation of carbon and nutrients carried by the fine sediment along the river–ocean continuum to close the global carbon and nutrient cycles.

Developing a big data analytics framework for generating the Long-term Gap-free High-resolution Air Pollutant concentration dataset (abbreviated as LGHAP) is of great significance for environmental management and Earth system science analysis. By synergistically integrating multimodal aerosol data acquired from diverse sources via a tensor-flow-based data fusion method, a gap-free aerosol optical depth (AOD) dataset with a daily 1 km resolution covering the period of 2000–2020 in China was generated. Specifically, data gaps in daily AOD imageries from the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard Terra were reconstructed based on a set of AOD data tensors acquired from diverse satellites, numerical analysis, and in situ air quality measurements via integrative efforts of spatial pattern recognition for high-dimensional gridded image analysis and knowledge transfer in statistical data mining. To our knowledge, this is the first long-term gap-free high-resolution AOD dataset in China, from which spatially contiguous PM2.5 and PM10 concentrations were then estimated using an ensemble learning approach. Ground validation results indicate that the LGHAP AOD data are in good agreement with in situ AOD observations from the Aerosol Robotic Network (AERONET), with an R of 0.91 and RMSE equaling 0.21. Meanwhile, PM2.5 and PM10 estimations also agreed well with ground measurements, with R values of 0.95 and 0.94 and RMSEs of 12.03 and 19.56 µg m−3, respectively. The LGHAP provides a suite of long-term gap-free gridded maps with a high resolution to better examine aerosol changes in China over the past 2 decades, from which three major variation periods of haze pollution in China were revealed. Additionally, the proportion of the population exposed to unhealthy PM2.5 increased from 50.60 % in 2000 to 63.81 % in 2014 across China, which was then reduced drastically to 34.03 % in 2020. Overall, the generated LGHAP dataset has great potential to trigger multidisciplinary applications in Earth observations, climate change, public health, ecosystem assessment, and environmental management. The daily resolution AOD, PM2.5, and PM10 datasets are publicly available at https://doi.org/10.5281/zenodo.5652257 (Bai et al., 2021a), https://doi.org/10.5281/zenodo.5652265 (Bai et al., 2021b), and https://doi.org/10.5281/zenodo.5652263 (Bai et al., 2021c), respectively. Monthly and annual datasets can be acquired from https://doi.org/10.5281/zenodo.5655797 (Bai et al., 2021d) and https://doi.org/10.5281/zenodo.5655807 (Bai et al., 2021e), respectively. Python, MATLAB, R, and IDL codes are also provided to help users read and visualize these data.

Bed-material sediment particle size data, particularly the median sediment particle size (D50), are critical for understanding and modeling riverine sediment transport. However, sediment particle size observations are primarily available at individual sites. Large-scale modeling and assessment of riverine sediment transport are limited by the lack of continuous regional maps of bed-material sediment particle size. We hence present a map of D50 over the contiguous US in a vector format that corresponds to approximately 2.7 million river segments (i.e., flowlines) in the National Hydrography Dataset Plus (NHDPlus) dataset. We develop the map in four steps: (1) collect and process the observed D50 data from 2577 U.S. Geological Survey stations or U.S. Army Corps of Engineers sampling locations; (2) collocate these data with the NHDPlus flowlines based on their geographic locations, resulting in 1691 flowlines with collocated D50 values; (3) develop a predictive model using the eXtreme Gradient Boosting (XGBoost) machine learning method based on the observed D50 data and the corresponding climate, hydrology, geology, and other attributes retrieved from the NHDPlus dataset; and (4) estimate the D50 values for flowlines without observations using the XGBoost predictive model. We expect this map to be useful for various purposes, such as research in large-scale river sediment transport using model- and data-driven approaches, teaching environmental and earth system sciences, planning and managing floodplain zones, etc. The map is available at https://doi.org/10.5281/zenodo.4921987 (Li et al., 2021a).

The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a Large Reaction Chamber). The chemical structure of myrcene consists of one moiety that is a conjugated π system (similar to isoprene) and another moiety that is a triple-substituted olefinic unit (similar to 2-methyl-2-butene). Hydrogen shift reactions of organic peroxy radicals (RO2) formed in the reaction of isoprene with atmospheric OH radicals are known to be of importance for the regeneration of OH. Structure–activity relationships (SARs) suggest that similar hydrogen shift reactions like in isoprene may apply to the isoprenyl part of RO2 radicals formed during the OH oxidation of myrcene. In addition, SAR predicts further isomerization reactions that would be competitive with bimolecular RO2 reactions for chemical conditions that are typical for forested environments with low concentrations of nitric oxide. Assuming that OH peroxy radicals can rapidly interconvert by addition and elimination of O2 like in isoprene, bulk isomerization rate constants of 0.21 and 0.097 s−1 (T=298 K) for the three isomers resulting from the 3′-OH and 1-OH addition, respectively, can be derived from SAR. Measurements of radicals and trace gases in the experiments allowed us to calculate radical production and destruction rates, which are expected to be balanced. The largest discrepancies between production and destruction rates were found for RO2. Additional loss of organic peroxy radicals due to isomerization reactions could explain the observed discrepancies. The uncertainty of the total radical (ROx=OH+HO2+RO2) production rates was high due to the uncertainty in the yield of radicals from myrcene ozonolysis. However, results indicate that radical production can only be balanced if the reaction rate constant of the reaction between hydroperoxy (HO2) and RO2 radicals derived from myrcene is lower (0.9 to 1.6×10-11 cm3 s−1) than predicted by SAR. Another explanation of the discrepancies would be that a significant fraction of products (yield: 0.3 to 0.6) from these reactions include OH and HO2 radicals instead of radical-terminating organic peroxides. Experiments also allowed us to determine the yields of organic oxidation products acetone (yield: 0.45±0.08) and formaldehyde (yield: 0.35±0.08). Acetone and formaldehyde are produced from different oxidation pathways, so that yields of these compounds reflect the branching ratios of the initial OH addition to myrcene. Yields determined in the experiments are consistent with branching ratios expected from SAR. The yield of organic nitrate was determined from the gas-phase budget analysis of reactive oxidized nitrogen in the chamber, giving a value of 0.13±0.03. In addition, the reaction rate constant for myrcene + OH was determined from the measured myrcene concentration, yielding a value of (2.3±0.3)×10-10 cm3 s−1.

Heterogeneous uptake of hydroperoxyl radicals (HO2) onto aerosols has been proposed to be a significant sink of HOx, hence impacting the atmospheric oxidation capacity. Accurate calculation of the HO2 uptake coefficient γHO2 is key to quantifying the potential impact of this atmospheric process. Laboratory studies show that γHO2 can vary by orders of magnitude due to changes in aerosol properties, especially aerosol soluble copper (Cu) concentration and aerosol liquid water content (ALWC). In this study we present a state-of-the-art model called MARK to simulate both gas- and aerosol-phase chemistry for the uptake of HO2 onto Cu-doped aerosols. Moreover, a novel parameterization of HO2 uptake was developed that considers changes in relative humidity (RH) and condensed-phase Cu ion concentrations and which is based on a model optimization using previously published and new laboratory data included in this work. This new parameterization will be applicable to wet aerosols, and it will complement current IUPAC recommendations. The new parameterization is as follows (the explanations for symbols are in the Appendix): 1γHO2=1αHO2+3×υHO24×106×RdHcorrRT×(5.87+3.2×ln⁡(ALWC/[PM]+0.067))×[PM]-0.2×Cu2+eff0.65+υHO2l4RTHorgDorgε. All parameters used in the paper are summarized in Table A1. Using this new equation, field data from a field campaign were used to evaluate the impact of the HO2 uptake onto aerosols on the ROx (= OH + HO2 + RO2) budget. Highly variable values for HO2 uptake were obtained for the North China Plain (median value < 0.1).

High concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 µm) in China have caused severe visibility degradation. Accurate simulations of PM2.5 and its chemical components are essential for evaluating the effectiveness of pollution control strategies and the health and climate impacts of air pollution. In this study, we compared the GEOS-Chem model simulations with comprehensive datasets for organic aerosol (OA), sulfate, nitrate, and ammonium in China. Model results are evaluated spatially and temporally against observations. The new OA scheme with a simplified secondary organic aerosol (SOA) parameterization significantly improves the OA simulations in polluted urban areas, highlighting the important contributions of anthropogenic SOA from semivolatile and intermediate-volatility organic compounds. The model underestimates sulfate and overestimates nitrate for most of the sites throughout the year. More significant underestimation of sulfate occurs in winter, while the overestimation of nitrate is extremely large in summer. The model is unable to capture some of the main features in the diurnal pattern of the PM2.5 chemical components, suggesting inaccuracies in the presented processes. Potential model adjustments that may lead to a better representation of the boundary layer height, the precursor emissions, hydroxyl radical concentrations, the heterogeneous formation of sulfate and nitrate, and the wet deposition of nitric acid and nitrate have been tested in the sensitivity analysis. The results show that uncertainties in chemistry perhaps dominate the model biases. The proper implementation of heterogeneous sulfate formation and the good estimates of the concentrations of sulfur dioxide, hydroxyl radical, and aerosol liquid water are essential for the improvement of the sulfate simulation. The update of the heterogeneous uptake coefficient of nitrogen dioxide significantly reduces the modeled concentrations of nitrate. However, the large overestimation of nitrate concentrations remains in summer for all tested cases. The possible bias in the chemical production and the wet deposition of nitrate cannot fully explain the model overestimation of nitrate, suggesting issues related to the atmospheric removal of nitric acid and nitrate. A better understanding of the atmospheric nitrogen budget, in particular, the role of the photolysis of particulate nitrate, is needed for future model developments. Moreover, the results suggest that the remaining underestimation of OA in the model is associated with the underrepresented production of SOA.

In this paper, a hyperbolic tangent variable step-size convex combination of the least mean square (HTVSCLMS) algorithm is proposed and analyzed. This work avoids the compromise between the convergence speed and the steady-state error for two filters in convex combination of the least mean square (CLMS) algorithm. In the proposed algorithm, the big step-size filter is replaced by a filter whose iteration step-size is a modified function based on hyperbolic tangent function. Thus it constructs hyperbolic tangent nonlinear relationship between step-size and error. At the same time, the small step-size filter remains unchanged but fixed. So, it conquers the slow convergence speed and the weak anti-interference ability of fixed step-size CLMS. Simulation results show that HTVSCLMS algorithm, compared with CLMS algorithm and variable step-size CLMS (VSCLMS) algorithm, not only has superior capability of tracking in the presence of noise and in a stable and even non-stable environment, but also can maintain a better convergence.

In recent decades, several lake models of varying complexity have been developed and incorporated into numerical weather prediction systems and climate models. To foster enhanced forecasting ability and verification, improvement of these lake models remains essential. This especially applies to the limited simulation capabilities of biogeochemical processes in lakes and greenhouse gas exchanges with the atmosphere. Here we present multi-model simulations of physical variables and dissolved gas dynamics in a temperate lake (Harp Lake, Canada). The five models (ALBM, FLake, LAKE, LAKEoneD, MTCR-1) considered within this most recent round of the Lake Model Intercomparison Project (LakeMIP) all captured the seasonal temperature variability well. In contrast, none of the models is able to reproduce the exact dates of ice cover and ice off, leading to considerable errors in the simulation of eddy diffusivity around those dates. We then conducted an additional modeling experiment with a diffusing passive tracer to isolate the effect of the eddy diffusivity on gas concentration. Remarkably, sophisticated k−ε models do not demonstrate a significant difference in the vertical diffusion of a passive tracer compared to models with much simpler turbulence closures. All the models simulate less intensive spring overturn compared to autumn. Reduced mixing in the models consequently leads to the accumulation of the passive tracer distribution in the water column. The lake models with a comprehensive biogeochemical module, such as the ALBM and LAKE, predict dissolved oxygen dynamics adequate to the observed data. However, for the surface carbon dioxide concentration the correlation between modeled (ALBM, LAKE) and observed data is weak (∼0.3). Overall our results indicate the need to improve the representation of physical and biogeochemical processes in lake models, thereby contributing to enhanced weather prediction and climate projection capabilities.

Vehicle emissions are a major source of air pollution in urban areas and thus greatly impact air quality in the megacity Beijing. Various vehicle emission control policies have been implemented at great cost, but there is a lack of appropriate methods to evaluate the effectiveness of such policies. Here we developed a wavelet transform method (WTM) to evaluate the effectiveness of vehicle emission control policies during the 2014 Asia-Pacific Economic Cooperation (APEC) summit, taking advantage of high-time-resolution mobile measurements of NO, NOx, BC, CO, SO2, and O3 made around the 4th Ring Road of Beijing. The WTM decomposed on-road mobile measurements into high- and low-frequency components, where the former represents immediate vehicle emissions, and the latter represents the atmospheric background in addition to accumulated on-road emissions. The high-frequency component of the WTM (CH_freq.), which represents the concentrations of pollutants from vehicle emissions (Cveh.), was used to evaluate the changes in vehicle emission intensity in the full-APEC period (3–12 November 2014) relative to the pre-APEC (28 October to 2 November 2014) and post-APEC (13–22 November 2014) periods, during which different vehicle emission control policies were implemented. Our results suggest that the Cveh. of NO, NOx, BC, and CO in the full-APEC period were 19.4 %, 17.7 %, 0.0 %, and 50.0 % lower, respectively, than those in the pre-APEC period during daytime and were 50.0 %, 47.3 %, 62.5 %, and 50.0 % lower than those in the post-APEC period during daytime. The Cveh. of NO, NOx, BC, and CO in the full-APEC period were 65.3 %, 65.4 %, 14.3 %, and 50.0 % lower than those in the post-APEC period during night-time. These results indicate that the vehicle emission control policies implemented during the full-APEC period were effective. Using on-road mobile measurements in combination with the WTM, we developed a new method for the evaluation of pollution control policies.

Hydroxyl (OH) and peroxy radicals (HO2 and RO2) were measured in the Pearl River Delta, which is one of the most polluted areas in China, in autumn 2014. The radical observations were complemented by measurements of OH reactivity (inverse OH lifetime) and a comprehensive set of trace gases including carbon monoxide (CO), nitrogen oxides (NOx=NO, NO2) and volatile organic compounds (VOCs). OH reactivity was in the range from 15 to 80 s−1, of which about 50 % was unexplained by the measured OH reactants. In the 3 weeks of the campaign, maximum median radical concentrations were 4.5×106 cm−3 for OH at noon and 3×108 and 2.0×108 cm−3 for HO2 and RO2, respectively, in the early afternoon. The completeness of the daytime radical measurements made it possible to carry out experimental budget analyses for all radicals (OH, HO2, and RO2) and their sum (ROx). The maximum loss rates for OH, HO2, and RO2 reached values between 10 and 15 ppbv h−1 during the daytime. The largest fraction of this can be attributed to radical interconversion reactions while the real loss rate of ROx remained below 3 ppbv h−1. Within experimental uncertainties, the destruction rates of HO2 and the sum of OH, HO2, and RO2 are balanced by their respective production rates. In case of RO2, the budget could be closed by attributing the missing OH reactivity to unmeasured VOCs. Thus, the presumption of the existence of unmeasured VOCs is supported by RO2 measurements. Although the closure of the RO2 budget is greatly improved by the additional unmeasured VOCs, a significant imbalance in the afternoon remains, indicating a missing RO2 sink. In case of OH, the destruction in the morning is compensated by the quantified OH sources from photolysis (HONO and O3), ozonolysis of alkenes, and OH recycling (HO2+NO). In the afternoon, however, the OH budget indicates a missing OH source of 4 to 6 ppbv h−1. The diurnal variation of the missing OH source shows a similar pattern to that of the missing RO2 sink so that both largely compensate each other in the ROx budget. These observations suggest the existence of a chemical mechanism that converts RO2 to OH without the involvement of NO, increasing the RO2 loss rate during the daytime from 5.3 to 7.4 ppbv h−1 on average. The photochemical net ozone production rate calculated from the reaction of HO2 and RO2 with NO yields a daily integrated amount of 102 ppbv ozone, with daily integrated ROx primary sources being 22 ppbv in this campaign. The produced ozone can be attributed to the oxidation of measured (18 %) and unmeasured (60 %) hydrocarbons, formaldehyde (14 %), and CO (8 %). An even larger integrated net ozone production of 140 ppbv would be calculated from the oxidation rate of VOCs with OH if HO2 and all RO2 radicals react with NO. However, the unknown RO2 loss (evident in the RO2 budget) causes 30 ppbv less ozone production than would be expected from the VOC oxidation rate.

Atmospheric oxidation capacity is the basis for converting freshly emitted substances into secondary products and is dominated by reactions involving hydroxyl radicals (OH) during daytime. In this study, we present in situ measurements of ROx radical (hydroxy OH, hydroperoxy HO2, and organic peroxy RO2) precursors and products; the measurements are carried out in four Chinese megacities (Beijing, Shanghai, Guangzhou, and Chongqing) during photochemically polluted seasons. The atmospheric oxidation capacity is evaluated using an observation-based model and radical chemistry precursor measurements as input. The radical budget analysis illustrates the importance of HONO and HCHO photolysis, which account for ∼50 % of the total primary radical sources. The radical propagation is efficient due to abundant NO in urban environments. Hence, the production rate of secondary pollutants, that is, ozone (and fine-particle precursors (H2SO4, HNO3, and extremely low volatility organic compounds, ELVOCs) is rapid, resulting in secondary air pollution. The ozone budget demonstrates its high production in urban areas; also, its rapid transport to downwind areas results in rapid increase in local ozone concentrations. The O3–NOx–VOC (volatile organic compound) sensitivity tests show that ozone production is VOC-limited and that alkenes and aromatics should be mitigated first for ozone pollution control in the four studied megacities. In contrast, NOx emission control (that is, a decrease in NOx) leads to more severe ozone pollution. With respect to fine-particle pollution, the role of the HNO3–NO3 partitioning system is investigated using a thermal dynamic model (ISORROPIA 2). Under high relative humidity (RH) and ammonia-rich conditions, nitric acid converts into nitrates. This study highlights the efficient radical chemistry that maintains the atmospheric oxidation capacity in Chinese megacities and results in secondary pollution characterized by ozone and fine particles.

Sufficient amino acid (AA) transport is essential to ensure the normal physiological function and growth of growing animals. The processes of AA sensing and transport in humans and murine animals, but rarely in goats, have been arousing great interest recently. This study was conducted to investigate the messenger RNA expression patterns of lysophosphatidic acid receptor 5 (LPAR5), guanine nucleotide-binding protein α-transducing 3 (GNAT3) and important partial AA transporters in digestive tracts, metabolic organs and muscles of growing goats. The results showed that these genes were widely expressed in goats, and had different expression patterns. LPAR5, GNAT3, solute carrier (SLC38A2), SLC7A7, SLC7A1 and SLC3A1 were rarely expressed in the rumen, but were highly expressed in the abomasum and intestine which are the main sites of AA absorption. GNAT3, SLC38A1, SLC38A2, SLC6A19, SLC7A7 and SLC7A1 showed comparatively high expression in the pancreas and the vital digestive glands, and the relatively high expression of these nine genes were noted in the tibialis posterior, the active muscle in energy metabolism. The correlation analysis showed that there were certain positive correlation among most genes. The current results indicate that the AA sensing and transport occur extensively in the abomasum and small intestine, metabolic organs and muscle tissues of ruminants, and that related genes have tissue specificity.

Summary: Iron is essential for DNA synthesis, respiration, energy metabolism, and key metabolic reactions intrinsic to life because of its capability to accept and release electrons easily and its indispensability for most of the creatures on the earth including bacteria and poultry. Salmonella species, the gram-negative foodborne facultative anaerobes, are notorious enteric pathogens that have a wild range of animal hosts, causing the deterioration of animal health, compromised animal welfare, enormous agricultural loss and medical burden around the world. Nontyphoidal Salmonella enterica (NTS) infections in poultry are the important cause of human salmonellosis. Poultry can be infected by NTS and have no obvious symptoms and are sold, transported and slaughtered as healthy animals. However, birds may carry in their intestine this organism undetected into the abattoir at the time of slaughter, thereby representing a food-safety risk for consumers. To reduce the risk of salmonellosis, the prevention of S. enterica serovars from colonization and invasion of the gut through limiting their iron acquisition can be an effective approach. This review summarizes the biological roles of iron and iron homeostasis in both Salmonella and poultry, competition for iron between Salmonella and hosts, and potential strategies targeting iron acquisitions to control Salmonella infection in poultry.

The first wintertime in situ measurements of hydroxyl (OH), hydroperoxy (HO2) and organic peroxy (RO2) radicals (ROx = OH + HO2 + RO2) in combination with observations of total reactivity of OH radicals, kOH in Beijing are presented. The field campaign Beijing winter finE particle STudy – Oxidation, Nucleation and light Extinctions (BEST-ONE) was conducted at the suburban site Huairou near Beijing from January to March 2016. It aimed to understand oxidative capacity during wintertime and to elucidate the secondary pollutants' formation mechanism in the North China Plain (NCP). OH radical concentrations at noontime ranged from 2.4×106 cm−3 in severely polluted air (kOH ∼ 27 s−1) to 3.6×106 cm−3 in relatively clean air (kOH ∼ 5 s−1). These values are nearly 2-fold larger than OH concentrations observed in previous winter campaigns in Birmingham, Tokyo, and New York City. During this campaign, the total primary production rate of ROx radicals was dominated by the photolysis of nitrous acid accounting for 46 % of the identified primary production pathways for ROx radicals. Other important radical sources were alkene ozonolysis (28 %) and photolysis of oxygenated organic compounds (24 %). A box model was used to simulate the OH, HO2 and RO2 concentrations based on the observations of their long-lived precursors. The model was capable of reproducing the observed diurnal variation of the OH and peroxy radicals during clean days with a factor of 1.5. However, it largely underestimated HO2 and RO2 concentrations by factors up to 5 during pollution episodes. The HO2 and RO2 observed-to-modeled ratios increased with increasing NO concentrations, indicating a deficit in our understanding of the gas-phase chemistry in the high NOx regime. The OH concentrations observed in the presence of large OH reactivities indicate that atmospheric trace gas oxidation by photochemical processes can be highly effective even during wintertime, thereby facilitating the vigorous formation of secondary pollutants.

Nocturnal reactive nitrogen compounds play an important role in regional air pollution. Here we present the measurements of dinitrogen pentoxide (N2O5) associated with nitryl chloride (ClNO2) and particulate nitrate (pNO3−) at a suburban site of Beijing in the summer of 2016. High levels of N2O5 and ClNO2 were observed in the outflow of the urban Beijing air masses, with 1 min average maxima of 937 and 2900 pptv, respectively. The N2O5 uptake coefficients, γ, and ClNO2 yield, f, were experimentally determined from the observed parameters. The N2O5 uptake coefficient ranged from 0.012 to 0.055, with an average of 0.034 ± 0.018, which is in the upper range of previous field studies reported in North America and Europe but is a moderate value in the North China Plain (NCP), which reflects efficient N2O5 heterogeneous processes in Beijing. The ClNO2 yield exhibited high variability, with a range of 0.50 to unity and an average of 0.73 ± 0.25. The concentration of the nitrate radical (NO3) was calculated assuming that the thermal equilibrium between NO3 and N2O5 was maintained. In NOx-rich air masses, the oxidation of nocturnal biogenic volatile organic compounds (BVOCs) was dominated by NO3 rather than O3. The production rate of organic nitrate (ON) via NO3 + BVOCs was significant, with an average of 0.10 ± 0.07 ppbv h−1. We highlight the importance of NO3 oxidation of VOCs in the formation of ON and subsequent secondary organic aerosols in summer in Beijing.

Hole doping to the Co3+ ion in cobaltite perovskites can significantly modify the electromagnetic properties. We prepared the hole-doped cobaltite perovskites La0.5Ba0.5CoO2.75+x (x = 0.06 and x = 0.15). Neutron powder diffraction and dc-magnetization experiments were performed to investigate the crystal structure and magnetic properties. We found that both of the samples have the cubic crystal structure with space group Pmm in all the measured temperatures. Ferromagnetic transition occurs at 160K in x = 0.15 sample. For x = 0.06, we found the short-range ordered ferromagnetic state and a long-range ordered antiferromagnetic state coexist in low temperature.

Anthropogenic emissions such as NOx and SO2 influence the biogenic secondary organic aerosol (SOA) formation, but detailed mechanisms and effects are still elusive. We studied the effects of NOx and SO2 on the SOA formation from the photooxidation of α-pinene and limonene at ambient relevant NOx and SO2 concentrations (NOx: 2: 2 induced nucleation and enhanced SOA mass formation. NOx strongly suppressed not only new particle formation but also SOA mass yield. However, in the presence of SO2 which induced a high number concentration of particles after oxidation to H2SO4, the suppression of the mass yield of SOA by NOx was completely or partly compensated for. This indicates that the suppression of SOA yield by NOx was largely due to the suppressed new particle formation, leading to a lack of particle surface for the organics to condense on and thus a significant influence of vapor wall loss on SOA mass yield. By compensating for the suppressing effect on nucleation of NOx, SO2 also compensated for the suppressing effect on SOA yield. Aerosol mass spectrometer data show that increasing NOx enhanced nitrate formation. The majority of the nitrate was organic nitrate (57–77 %), even in low-NOx conditions (−1. SOA from α-pinene photooxidation at high NOx had a generally lower hydrogen to carbon ratio (H ∕ C), compared to low NOx. The NOx dependence of the chemical composition can be attributed to the NOx dependence of the branching ratio of the RO2 loss reactions, leading to a lower fraction of organic hydroperoxides and higher fractions of organic nitrates at high NOx. While NOx suppressed new particle formation and SOA mass formation, SO2 can compensate for such effects, and the combining effect of SO2 and NOx may have an important influence on SOA formation affected by interactions of biogenic volatile organic compounds (VOCs) with anthropogenic emissions.

Understanding the recent evolution of methane emissions in the Arctic is necessary to interpret the global methane cycle. Emissions are affected by significant uncertainties and are sensitive to climate change, leading to potential feedbacks. A polar version of the CHIMERE chemistry-transport model is used to simulate the evolution of tropospheric methane in the Arctic during 2012, including all known regional anthropogenic and natural sources, in particular freshwater emissions which are often overlooked in methane modelling. CHIMERE simulations are compared to atmospheric continuous observations at six measurement sites in the Arctic region. In winter, the Arctic is dominated by anthropogenic emissions; emissions from continental seepages and oceans, including from the East Siberian Arctic Shelf, can contribute significantly in more limited areas. In summer, emissions from wetland and freshwater sources dominate across the whole region. The model is able to reproduce the seasonality and synoptic variations of methane measured at the different sites. We find that all methane sources significantly affect the measurements at all stations at least at the synoptic scale, except for biomass burning. In particular, freshwater systems play a decisive part in summer, representing on average between 11 and 26 % of the simulated Arctic methane signal at the sites. This indicates the relevance of continuous observations to gain a mechanistic understanding of Arctic methane sources. Sensitivity tests reveal that the choice of the land-surface model used to prescribe wetland emissions can be critical in correctly representing methane mixing ratios. The closest agreement with the observations is reached when using the two wetland models which have emissions peaking in August–September, while all others reach their maximum in June–July. Such phasing provides an interesting constraint on wetland models which still have large uncertainties at present. Also testing different freshwater emission inventories leads to large differences in modelled methane. Attempts to include methane sinks (OH oxidation and soil uptake) reduced the model bias relative to observed atmospheric methane. The study illustrates how multiple sources, having different spatiotemporal dynamics and magnitudes, jointly influence the overall Arctic methane budget, and highlights ways towards further improved assessments.

In 2014, a large, comprehensive field campaign was conducted in the densely populated North China Plain. The measurement site was located in a botanic garden close to the small town Wangdu, without major industry but influenced by regional transportation of air pollution. The loss rate coefficient of atmospheric hydroxyl radicals (OH) was quantified by direct measurements of the OH reactivity. Values ranged between 10 and 20 s−1 for most of the daytime. Highest values were reached in the late night with maximum values of around 40 s−1. OH reactants mainly originated from anthropogenic activities as indicated (1) by a good correlation between measured OH reactivity and carbon monoxide (linear correlation coefficient R2 = 0.33) and (2) by a high contribution of nitrogen oxide species to the OH reactivity (up to 30 % in the morning). Total OH reactivity was measured by a laser flash photolysis–laser-induced fluorescence instrument (LP-LIF). Measured values can be explained well by measured trace gas concentrations including organic compounds, oxygenated organic compounds, CO and nitrogen oxides. Significant, unexplained OH reactivity was only observed during nights, when biomass burning of agricultural waste occurred on surrounding fields. OH reactivity measurements also allow investigating the chemical OH budget. During this campaign, the OH destruction rate calculated from measured OH reactivity and measured OH concentration was balanced by the sum of OH production from ozone and nitrous acid photolysis and OH regeneration from hydroperoxy radicals within the uncertainty of measurements. However, a tendency for higher OH destruction compared to OH production at lower concentrations of nitric oxide is also observed, consistent with previous findings in field campaigns in China.

A comprehensive field campaign was carried out in summer 2014 in Wangdu, located in the North China Plain. A month of continuous OH, HO2 and RO2 measurements was achieved. Observations of radicals by the laser-induced fluorescence (LIF) technique revealed daily maximum concentrations between (5–15) × 106 cm−3, (3–14) × 108 cm−3 and (3–15) × 108 cm−3 for OH, HO2 and RO2, respectively. Measured OH reactivities (inverse OH lifetime) were 10 to 20 s−1 during daytime. The chemical box model RACM 2, including the Leuven isoprene mechanism (LIM), was used to interpret the observed radical concentrations. As in previous field campaigns in China, modeled and measured OH concentrations agree for NO mixing ratios higher than 1 ppbv, but systematic discrepancies are observed in the afternoon for NO mixing ratios of less than 300 pptv (the model–measurement ratio is between 1.4 and 2 in this case). If additional OH recycling equivalent to 100 pptv NO is assumed, the model is capable of reproducing the observed OH, HO2 and RO2 concentrations for conditions of high volatile organic compound (VOC) and low NOx concentrations. For HO2, good agreement is found between modeled and observed concentrations during day and night. In the case of RO2, the agreement between model calculations and measurements is good in the late afternoon when NO concentrations are below 0.3 ppbv. A significant model underprediction of RO2 by a factor of 3 to 5 is found in the morning at NO concentrations higher than 1 ppbv, which can be explained by a missing RO2 source of 2 ppbv h−1. As a consequence, the model underpredicts the photochemical net ozone production by 20 ppbv per day, which is a significant portion of the daily integrated ozone production (110 ppbv) derived from the measured HO2 and RO2. The additional RO2 production from the photolysis of ClNO2 and missing reactivity can explain about 10 % and 20 % of the discrepancy, respectively. The underprediction of the photochemical ozone production at high NOx found in this study is consistent with the results from other field campaigns in urban environments, which underlines the need for better understanding of the peroxy radical chemistry for high NOx conditions.

Megacities have strong interactions with the surrounding regions through transport of air pollutants. It has been frequently addressed that the air quality of Beijing is influenced by the influx of air pollutants from the North China Plain (NCP). Estimations of air pollutant cross-boundary transport between Beijing and the NCP are important for air quality management. However, evaluation of cross-boundary transport using long-term observations is very limited. Using the observational results of the gaseous pollutants SO2, NO, NO2, O3, and CO from August 2006 to October 2008 at the Yufa site, a cross-boundary site between the megacity Beijing and the NCP, together with meteorological parameters, we explored a method for evaluating the transport flux intensities at Yufa, as part of the “Campaign of Air Quality Research in Beijing and Surrounding Region 2006–2008” (CAREBeijing 2006–2008). The hourly mean ± SD (median) concentration of SO2, NO, NO2, NOx, O3, Ox, and CO was 15 ± 16 (9) ppb, 12 ± 25 (3) ppb, 24 ± 19 (20) ppb, 36 ± 39 (23) ppb, 28 ± 27 (21) ppb, 52 ± 24 (45) ppb, and 1.6 ± 1.4 (1.2) ppm during the observation period, respectively. The bivariate polar plots showed the dependence of pollutant concentrations on both wind speed and wind direction, and thus inferred their dominant transport directions. Surface flux intensity calculations further demonstrated the regional transport influence of Beijing and the NCP on Yufa. The net surface transport flux intensity (mean ± SD) of SO2, NO, NO2, NOx, O3, Ox, and CO was 6.2 ± 89.5, −4.3 ± 29.5, −0.6 ± 72.3, −4.9 ± 93.0, 14.7 ± 187.8, 14.8 ± 234.9, and 70 ± 2830 µg s−1 m−2 during the observation period, respectively. For SO2, CO, O3, and Ox the surface flux intensities from the NCP to Yufa surpassed those from Beijing to Yufa in all seasons except winter, with the strongest net fluxes largely in summer, which were about 4–8 times those of other seasons. The surface transport flux intensity of NOx from Beijing to Yufa was stronger than that from the NCP to Yufa except in summer, with the strongest net flux in winter, which was about 1.3–8 times that of other seasons. The flux intensities were then assigned to the corresponding trajectories in the potential source contribution function analysis (PSCF), which confirmed the results of flux intensity calculations. Our study also suggested that various factors, such as the wind field, emission inventory, and photochemical reactions, could influence transport of air pollutants. The decrease of surface flux intensity during the Olympic Games implied the role of both local emission reduction and regional cooperation in successful air quality management. Three dimensional observations are needed for further comprehensive discussion of the regional transport between Beijing and the NCP.

Understanding methane emissions from the Arctic, a fast-warming carbon reservoir, is important for projecting future changes in the global methane cycle. Here we optimized methane emissions from north of 60° N (pan-Arctic) regions using a nested-grid high-resolution inverse model that assimilates both high-precision surface measurements and column-average SCanning Imaging Absorption spectroMeter for Atmospheric CHartogrphY (SCIAMACHY) satellite retrievals of methane mole fraction. For the first time, methane emissions from lakes were integrated into an atmospheric transport and inversion estimate, together with prior wetland emissions estimated with six biogeochemical models. In our estimates, in 2005, global methane emissions were in the range of 496.4–511.5 Tg yr−1, and pan-Arctic methane emissions were in the range of 11.9–28.5 Tg yr−1. Methane emissions from pan-Arctic wetlands and lakes were 5.5–14.2 and 2.4–14.2 Tg yr−1, respectively. Methane emissions from Siberian wetlands and lakes are the largest and also have the largest uncertainty. Our results indicate that the uncertainty introduced by different wetland models could be much larger than the uncertainty of each inversion. We also show that assimilating satellite retrievals can reduce the uncertainty of the nested-grid inversions. The significance of lake emissions cannot be identified across the pan-Arctic by high-resolution inversions, but it is possible to identify high lake emissions from some specific regions. In contrast to global inversions, high-resolution nested-grid inversions perform better in estimating near-surface methane concentrations.

Direct detection of highly reactive, atmospheric hydroxyl radicals (OH) is widely accomplished by laser-induced fluorescence (LIF) instruments. The technique is also suitable for the indirect measurement of HO2 and RO2 peroxy radicals by chemical conversion to OH. It requires sampling of ambient air into a low-pressure cell, where OH fluorescence is detected after excitation by 308 nm laser radiation. Although the residence time of air inside the fluorescence cell is typically only on the order of milliseconds, there is potential that additional OH is internally produced, which would artificially increase the measured OH concentration. Here, we present experimental studies investigating potential interferences in the detection of OH and peroxy radicals for the LIF instruments of Forschungszentrum Jülich for nighttime conditions. For laboratory experiments, the inlet of the instrument was over flowed by excess synthetic air containing one or more reactants. In order to distinguish between OH produced by reactions upstream of the inlet and artificial signals produced inside the instrument, a chemical titration for OH was applied. Additional experiments were performed in the simulation chamber SAPHIR where simultaneous measurements by an open-path differential optical absorption spectrometer (DOAS) served as reference for OH to quantify potential artifacts in the LIF instrument. Experiments included the investigation of potential interferences related to the nitrate radical (NO3, N2O5), related to the ozonolysis of alkenes (ethene, propene, 1-butene, 2,3-dimethyl-2-butene, α-pinene, limonene, isoprene), and the laser photolysis of acetone. Experiments studying the laser photolysis of acetone yield OH signals in the fluorescence cell, which are equivalent to 0.05 × 106 cm−3 OH for a mixing ratio of 5 ppbv acetone. Under most atmospheric conditions, this interference is negligible. No significant interferences were found for atmospheric concentrations of reactants during ozonolysis experiments. Only for propene, α-pinene, limonene, and isoprene at reactant concentrations, which are orders of magnitude higher than in the atmosphere, could artificial OH be detected. The value of the interference depends on the turnover rate of the ozonolysis reaction. For example, an apparent OH concentration of approximately 1 × 106 cm−3 is observed when 5.8 ppbv limonene reacts with 600 ppbv ozone. Experiments with the nitrate radical NO3 reveal a small interference signal in the OH, HO2, and RO2 detection. Dependencies on experimental parameters point to artificial OH formation by surface reactions at the chamber walls or in molecular clusters in the gas expansion. The signal scales with the presence of NO3 giving equivalent radical concentrations of 1.1 × 105 cm−3 OH, 1 × 107 cm−3 HO2, and 1.7 × 107 cm−3 RO2 per 10 pptv NO3.

Timely and effective estimation of road damage degree can provide scientific and reasonable support for emergency rescue. In this paper, we shall first briefly introduced a generalized information diffusion model to evaluate the damage degree of roads. Since the road earthquake loss system is influenced by many factors, which has some characters such as smaller and random sample size, the excessive features and nonlinear, etc. Based on it, several measured indicators of road damage were selected as key impacting indicators to estimate the failure grade, including the damage degree of road and bridge x1, damage degree of subgrade and pavement x2 and damage degree of roadside environment destruction on road x3. Moreover, the fuzzy diffusion and interpolation mapping for sparse data points has been defined by the fuzzy mapping theory. Next, the heterogeneous information diffusion from limited data point information to its adjacent area points was implemented. In this procedure, the fuzzy approximate reasoning and information centralization of road rupture width are also has been estimated. The numerical results show that the Generalized Information Diffusion (GID) model can reasonably approximate and extend effective information for incomplete data samples, which also can be applied to treat the nonlinear relationship between road damage degree of postearthquake. Finally, an example is given to illustrate the effectiveness and feasibility of the method.

Deep venous thrombosis (DVT) is a common surgical complication in cancer patients and evidence that inflammation plays a role in the occurrence of DVT is increasing. We studied a population of cancer patients with abdominal malignancies with the aim of investigating whether the levels of circulating inflammatory cytokines were associated with postoperative DVT, and to determine the levels in DVT diagnoses. The serum levels of C-reactive protein (CRP), interleukins (IL)-6 and IL-10, nuclear transcription factor-κB (NF-κB) and E-selectin (E-Sel) were determined in 120 individuals, who were divided into 3 groups: healthy controls, patients with and patients without DVT after surgery for an abdominal malignancy. Data were analyzed by ANOVA, Dunnet's T3 test, chi-square test, and univariate and multivariate logistic regression as needed. The CRP, IL-6, NF-κB, and E-Sel levels in patients with DVT were significantly higher than those in the other groups (P

This paper deals with Carrier Frequency Offset (CFO) estimation for OFDM systems using repetitive patterns in the training symbol. A theoretical comparison based on Cramer Rao Bounds (CRB) for two kinds of CFO estimation methods has been presented in this paper. Through the comparison, it is shown that the performance of CFO estimation can be improved by exploiting the repetition property and the exact training symbol rather than exploiting the repetition property only. The selection of Q (number of repetition patterns) is discussed for both situations as well. Moreover, for exploiting the repetition and the exact training symbol, a new numerical procedure for the Maximum-Likelihood (ML) estimation is designed in this paper to save computational complexity. Analysis and numerical result are also given, demonstrating the conclusions in this paper.

We used the General Ensemble biogeochemical Modeling System (GEMS) to simulate responses of natural and managed ecosystems to changes in land use and land cover, management, and climate for a forest/savanna transitional zone in central Ghana. Model results show that deforestation for crop production during the 20th century resulted in a substantial reduction in ecosystem carbon (C) stock from 135.4 Mg C ha−1 in 1900 to 77.0 Mg C ha−1 in 2000, and in soil organic C stock within the top 20 cm of soil from 26.6 Mg C ha−1 to 21.2 Mg C ha−1. If no land use change takes place from 2000 through 2100, low and high climate change scenarios (increase in temperature and decrease in precipitation over time) will result in losses of soil organic C stock by 16% and 20%, respectively. A low nitrogen (N) fertilization rate is the principal constraint on current crop production. An increase in N fertilization under the low climate change scenario would lead to an increase in the average crop yield by 21% with 30 kg N ha−1 and by 42% with 60 kg N ha−1 (varying with crop species), accordingly, the average soil C stock would decrease by 2% and increase by 17%, in all cropping systems by 2100. The results suggest that a reasonable N fertilization rate is critical to achieve food security and agricultural sustainability in the study area through the 21st century. Adaptation strategies for climate change in this study area require national plans to support policies and practices that provide adequate N fertilizers to sustain soil C and crop yields and to consider high temperature tolerant crop species if these temperature projections are exceeded.

Pattern recognition by chaotic neural networks is studied using a hyperchaotic neural network as model. Virtual basins of attraction are introduced around unstable periodic orbits which are then used as patterns. Search for periodic orbits in dynamical systems is treated as a process of pattern recognition. The role of synapses on patterns in chaotic networks is discussed. It is shown that distorted states having only limited information of the patterns are successfully recognized.