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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and Ox (meaning NO2+O3) measured in 10 Canadian cities during the last 2 to 3 decades. We also investigated associated driving forces in terms of emission reductions, perturbations due to varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks. Two machine learning methods, the random forest algorithm and boosted regression trees, were used to extract deweathered mixing ratios (or mass concentrations) of the pollutants. The Mann–Kendall trend test of the deweathered and original annual average concentrations of the pollutants showed that, on the timescale of 20 years or longer, perturbation due to varying weather conditions on the decadal trends of the pollutants are minimal (within ±2 %) in about 70 % of the studied cases, although it might be larger (but at most 16 %) in the remaining cases. NO2, CO and SO2 showed decreasing trends in the last 2 to 3 decades in all the cities except CO in Montréal. O3 showed increasing trends in all the cities except Halifax, mainly due to weakened titration reaction between O3 and NO. Ox, however, showed decreasing trends in all the cities except Victoria, because the increase in O3 is much less than the decrease in NO2. In three of the five eastern Canadian cities, emission reductions dominated the decreasing trends in PM2.5, but no significant trends in PM2.5 were observed in the other two cites. In the five western Canadian cities, increasing or no significant trends in PM2.5 were observed, likely due to unpredictable large-scale wildfires overwhelming or balancing the impacts of emission reductions on PM2.5. In addition, despite improving air quality during the last 2 decades in most cities, an air quality health index of above 10 (representing a very high risk condition) still occasionally occurred after 2010 in western Canadian cities because of the increased large-scale wildfires.

In this study, we utilized a 20-bin WRF-Chem (Weather Research and Forecasting coupled with Chemistry) regional model to investigate the contributions of chemical drivers to the growth of new particles, as well as to simulate the three-dimensional dynamics of new particle formation (NPF) events over the North China Plain during a summer campaign in 2019. The model replicated the occurrence of NPF and the growth pattern of newly formed particles, as well as the performance to meet the benchmarks, i.e., absolute mean fractional bias ≤ 50 % and mean fractional error ≤ 75 %, in replicating number concentrations of particles in the 10–40 nm range in five events between 29 June and 6 July 2019. Therefore, we further analyzed three NPF events with distinct particle growth characteristics. In these instances, the model overpredicted daytime condensation of H2SO4 vapor and nighttime formation of NH4NO3. These resulted in overestimation of the hygroscopicity parameter of nanometer particles. Nevertheless, the model performance met the benchmarks for reproducing cloud condensation nuclei (CCN) at a supersaturation (SS) of 0.4 % on NPF days. This was because the overestimation of inorganics was offset by the model underestimation of CCN originating from submicron particles. Additionally, three-dimensional simulations of NPF events demonstrated some key findings. First, NPF consistently begins in the upper parts of the planetary boundary layer (PBL) before expanding. Second, during daytime organics dominate growth of new particles in the PBL, whereas in the free troposphere the primary chemical drivers are inorganic species. However, to confirm these findings, vertical observations are required.

This study implements the least-squares inversion method for solving the exhumation history from the thermochronologic age–elevation relationship (AER) based on the linear equation among exhumation rate, age and total exhumation from the closure depth to the Earth surface. Modeling experiments suggest significant and systematic influence of initial geothermal model, the a priori exhumation rate and the time interval length on the a posteriori exhumation history. Lessons learned from the experiments include that (i) the modern geothermal gradient can be used for constraining the initial geothermal model, (ii) a relatively high a priori exhumation rate would lead to systematically lower a posteriori exhumation and vice versa, (iii) the variance of the a priori exhumation rate controls the variation in the inverted exhumation history, and (iv) the choice of time interval length should be optimized for resolving the potential temporal changes in exhumation. To mitigate the dependence of inverted erosion history on these initial parameters, we implemented a new stepwise inverse modeling method for optimizing the model parameters by comparing the observed and predicted thermochronologic data and modern geothermal gradients. Finally, method demonstration was performed using four synthetic datasets and three natural examples of different exhumation rates and histories. It is shown that the inverted rock exhumation histories from the synthetic datasets match the whole picture of the “truth”, although the temporal changes in the magnitude of exhumation are underestimated. Modeling of the datasets from natural samples produces geologically reasonable exhumation histories. The code and data used in this work are available on Zenodo (https://doi.org/10.5281/zenodo.10839275).

Organic aerosols from marine sources over the western Pacific Ocean of East Asia were investigated using an online coupled regional chemistry–climate model RIEMS-Chem for the entire year 2014. Model evaluation against a wide variety of observations from research cruises and in situ measurements demonstrated a good skill of the model in simulating temporal variation and spatial distribution of particulate matter with aerodynamic diameter less than 2.5 and 10 µm (PM2.5 and PM10), black carbon (BC), organic carbon (OC), sodium, and aerosol optical depth (AOD) in the marine atmosphere. The inclusion of marine organic aerosols improved model performance on OC concentration by reducing model biases of up to 20 %. The regional and annual mean near-surface marine organic aerosol (MOA) concentration was estimated to be 0.27 µg m−3, with the maximum in spring and the minimum in winter, and contributed 26 % of the total organic aerosol concentration on average over the western Pacific. Marine primary organic aerosol (MPOA) accounted for the majority of marine organic aerosol (MOA) mass, and the MPOA concentration exhibited the maximum in autumn and the minimum in summer, whereas marine secondary organic aerosol (MSOA) was approximately 1–2 orders of magnitude lower than MPOA, having a distinct summer maximum and a winter minimum. MOA induced a direct radiative effect (DREMOA) of −0.27 W m−2 and an indirect radiative effect (IREMOA) of −0.66 W m−2 at the top of the atmosphere (TOA) in terms of annual and oceanic average over the western Pacific, with the highest seasonal mean IREMOA up to −0.94 W m−2 in spring. IREMOA was stronger than, but in a similar magnitude to, the IRE due to sea salt aerosol on average, and it was approximately 9 % of the IRE due to anthropogenic aerosols in terms of annual mean over the western Pacific. This ratio increased to 19 % in the northern parts of the western Pacific in autumn. This study reveals an important role of MOA in perturbing cloud properties and shortwave radiation fluxes in the western Pacific of East Asia.

PM2.5 pollution is a major air quality issue that deteriorates human health, and numerous studies have focused on PM2.5 pollution in major regions such as the North China Plain (NCP) and Yangtze River Delta (YRD). However, the characteristics of PM2.5 concentrations and the associated formation mechanism in the transport corridor (referred to as SWLY) between the NCP and YRD are largely ignored. Based on observational data, we find that the number of PM2.5 pollution events in SWLY is comparable to that in the NCP, far exceeding that in the YRD, which is indicative of the severity of air pollution in this area. Utilizing a regional climate and air quality model, we isolate the effect of seesaw transport events, e.g., transport between the NCP and YRD, and atmospheric stagnation on the accumulation of PM2.5 over SWLY. Specifically, seesaw events and stagnation, comparable to each other, collectively account for an average of 67 % of pollution days, with PM2.5 exceeding 75 µg m−3, and this fraction (85 %) is even larger for severe haze events, with PM2.5 exceeding 150 µg m−3. Furthermore, the connection between seesaw transport and large-scale circulation is examined. The transregional transport of pollutants from the NCP to the YRD (YRD to NCP) is likely stimulated by positive (negative) to negative (positive) geopotential height anomalies at 500 hPa located in northern China. The health effect due to short-term PM2.5 exposure induced by the transregional transport and stagnation is investigated, yielding a total of 8634 (95 % CI: 6023–11 223) and 9496 (95 % CI: 6552–12 413) premature deaths, respectively, in SWLY during winter 2014–2019, which is as high as 9 % of the total premature deaths in China, even though SWLY takes up less than 1 % of China's area. While atmospheric stagnation is in general projected to occur more frequently under a warming climate, this study indicates the importance of regional emission control to alleviate PM2.5 pollution from seesaw transport and stagnation.

Nucleophilic high molecular-weight organic compounds (HMWOCs) are sensitive to protons (H+) in Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis. A comprehensive evaluation of the diurnal evolution of nucleophilic HMWOCs was performed. HMWOCs aged significantly in daily cycles, accompanied by functionality shifts, particularly oxygenated and reduced nitrogen (CHON and CHN) as well as oxygenated organics. The intensities of high molecular-weight (HMW) oxygenated compounds increased during both daytime and nighttime. The daytime evolution produced more nitrogen-containing compounds with carboxylic group (–COOH) homologues with molecular weights greater than 300, while the nighttime evolution produced mostly small CHON compounds (molecular weights < 300). During evolution, nighttime CHON removals were observed; meanwhile, carboxylation was also identified in CHON groups. The daytime evolution produced significantly more reduced-nitrogen-containing compounds; a day- and nighttime increase in CHN compounds with five members was also observed. This study can provide insights into the aging of less polar organic aerosols.

This study employed multiple techniques to investigate the contribution of grown new particles to the number concentration of cloud condensation nuclei (CCN) at various supersaturation (SS) levels at a rural mountain site in the North China Plain from 29 June to 14 July 2019. On 8 new particle formation (NPF) days, the total particle number concentrations (Ncn) were 8.4 ± 6.1×103 cm−3, which was substantially higher compared to 4.7 ± 2.6×103 cm−3 on non-NPF days. However, the CCN concentration (Nccn) at 0.2 % SS and 0.4 % SS on the NPF days was significantly lower than those observed on non-NPF days (p). This was due to the lower cloud activation efficiency of preexisting particles resulting from organic vapor condensation and smaller number concentrations of preexisting particles on NPF days. A case-by-case examination showed that the grown new particles only yielded a detectable contribution to Nccn at 0.4 % SS and 1.0 % SS during the NPF event on 1 July 2019, accounting for 12 % ± 11 % and 23 % ± 12 % of Nccn, respectively. The increased Nccn during two other NPF events and at 0.2 % SS on 1 July 2019 were detectable but determined mainly by varying preexisting particles rather than grown new particles. In addition, the hygroscopicity parameter values, concentrations of inorganic and organic particulate components, and surface chemical composition of different sized particles were analyzed in terms of chemical drivers to grow new particles. The results showed that the grown new particles via organic vapor condensation generally had no detectable contribution to Nccn but incidentally did. However, this conclusion was drawn from a small size of observational data, leaving more observations, particularly long-term observations and the growth of preexisting particles to the CCN required size, needed for further investigation.

New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While many observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated in polluted environments. Using the observations in a coastal city of Qingdao, Beijing, and Gucheng in north China, we thoroughly evaluate the simulated number concentrations of CN and CCN using an NPF-explicit parameterization embedded in the WRF-Chem model. For CN, the initial simulation shows large biases of particle number concentrations at 10–40 and 40–100 nm. By adjusting the process of gas–particle partitioning, including the mass accommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H2SO4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (∼ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H2SO4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis.

Multi-temporal glacier inventories provide key information about the glaciers, their characteristics, and changes and are inevitable for glacier modelling and investigating geodetic mass changes. However, to date, no consistent multi-temporal glacier inventory for the whole of the Karakoram exists, negatively affecting the monitoring of spatio-temporal variations in glaciers' geometric parameters and their related applications. We used a semi-automatic method combining automatic segmentation and manual correction and produced a multi-temporal Karakoram glacier inventory (KGI) compiled from Landsat TM/ETM+/OLI (Thematic Mapper, Enhanced Thematic Mapper Plus, and Operational Land Imager) images for the 1990s, 2000s, 2010s, and 2020s. Our assessments using independent multiple digitisation of 37 glaciers show that the KGI is sufficiently accurate, with an overall uncertainty of ±3.68 %. We also performed uncertainty evaluation for the contiguous glacier polygons using a buffer of half a pixel, which resulted in an average mapping uncertainty of ±5.21 %. We calculated more than 20 attributes for each glacier, including coordinates, area, supraglacial debris area, date information, and topographic parameters derived from the ASTER GDEM (Advanced Spaceborne Thermal Emission and Reflection Radiometer global digital elevation model). According to KGI-2020s, approximately 10 500 alpine glaciers (>0.01 km2 each) cover an area of 22 510±828 km2 of which 10.18±0.38 % (2290±84 km2) is covered by supraglacial debris. Over the past 3 decades, the glaciers experienced a loss of clean ice and/or snow area but a gain in supraglacial debris. Supraglacial debris cover has increased by 17.63±1.44 % (343.30±27.95 km2), while non-debris-covered glaciers decreased by 1.56±0.24 % (319.85±49.92 km2). The total glacier area was relatively stable and showed only a slight insignificant increase of 23.45±28.85 km2 (0.10±0.13 %). The glacier area has declined by 3.27±0.24 % in the eastern Karakoram, while the glacier area slightly increased in central (0.65±0.10 %) and western Karakoram (1.26±0.11 %). Supraglacial debris has increased over the whole of Karakoram, especially in areas above 4200 m a.s.l. (above sea level), showing an upward shift. The glacier area changes were characterised by strong spatial heterogeneity, influenced by surging and advancing glaciers. However, due to global warming, the glaciers are on average retreating. This is in particular true for small and debris-free glaciers. The multi-temporal KGI data are available at the National Cryosphere Desert Data Center of China: https://doi.org/10.12072/ncdc.glacier.db2386.2022 (F. Xie et al., 2022).

The existence of glacial lakes in the southeastern Tibetan Plateau (SETP) is a potential hazard to downstream regions, as the outburst of such lakes has the potential to result in disastrous glacial lake outburst floods (GLOFs). In the present study, we conducted a comprehensive investigation of Bienong Co, a moraine-dammed glacial lake in the SETP. First, the lake basin morphology was determined, and the lake volume was estimated, showing that the maximum lake depth is ∼181 m and the lake volume is ∼102.3×106 m3. These scenarios included the possibility of GLOFs being triggered by ice avalanches (Scenarios A1–3) from the mother glacier or by landslides from the lateral moraines (Scenarios B1–3 and C1–3). Avalanche volumes of the nine trigger scenarios were obtained from the Rapid Mass Movement Simulation (RAMMS) modeling results. Next, the Basic Simulation Environment for Computation of Environmental Flow and Natural Hazard Simulation (BASEMENT) model was used to simulate the generation and propagation of the avalanche-induced displacement waves in the lake. With the model, the overtopping flows and erosion on the moraine dam and the subsequent downstream floods were also simulated. The results indicate that the ice avalanche scenario may cause the largest mass volume entering the lake, resulting in a displacement wave up to 25.2 m in amplitude (Scenario A3) near the moraine dam. Landslide scenarios with smaller volumes entering the lake result in smaller displacement waves. Scenarios A1, A2, and A3 result in released water volumes from the lake of 24.1×106, 25.3×106, and 26.4×106 m3, respectively. Corresponding peak discharges at the moraine dam are 4996, 7817, and 13 078 m3 s−1, respectively. These high discharges cause erosion of the moraine dam, resulting in breach widths of 295, 339, and 368 m, respectively, with the generally similar breach depth of approximately 19 m. In landslide scenarios, only overtopping flows generated by Scenarios B3 and C3 cause erosion on the moraine dam, with breach depths of 6.5 and 7.9 m and breach widths of 153 and 169 m, respectively. According to our simulations, GLOFs generated by Scenarios A1–3 all flow through 18 settlements downstream in 20 h, threatening more than half of them. Both Scenarios B3 and C3 produce GLOFs that flow through the first eight settlements downstream in 20 h and have a relatively small impact on them. Comparisons of the area, depth, and volume of glacial lakes for which the bathymetry data are available show that Bienong Co is the deepest known glacial lake with the same surface area on the Tibetan Plateau. This study could provide a new insight into moraine-dammed glacial lakes in the SETP and be a valuable reference for GLOF disaster prevention for the local government.

Abstract Phytoremediation has been explored as a cost‐effective method to remediate soil Pb contamination. A greenhouse study was conducted to evaluate the efficacy of Vigna unguiculata, Brassica pekinensis, Gomphrena globose, and Helianthus annuus for removing and immobilizing Pb in soil collected from the Westside Lead Superfund site in Atlanta. Plants were cultivated in sampled soil with a Pb concentration of 515 ± 10 mg/kg for 60 days. Soils growing H. annuus were additionally treated with ethylenediaminetetraacetic acid (EDTA) (0.1 g/kg) or compost (20% soil blend) to assess their capabilities for enhancing phytoremediation. Mean post‐phytoremediation Pb concentrations in the four plant species were 23.5, 25.7, 50.0, and 58.1 mg/kg dry weight (DW), respectively, and were substantially higher than 1.55 mg/kg DW in respective plant species grown in control soils with no Pb contamination. The highest Pb concentration, translocation factor, and biomass were found in V. unguiculate among four species without soil amendments. H. annuus treated with EDTA and compost resulted in a significant increase in the total Pb uptake and larger biomass compared to non‐treated plants, respectively. Although this study found that V. unguiculata was the best candidate for Pb accumulation and immobilization among four species, soil remediation was limited to 54 mg/kg in a growing season. We find that it is critically important to perform phytostabilization in a secure manner, since Pb bioavailability of edible plant parts implies the potential risk associated with their unintentional consumption. Efficiently and effectively remediating Pb‐contaminated soils in a low‐cost manner needs to be further studied.

In this study, three methods, i.e., the random forest (RF) algorithm, boosted regression trees (BRTs) and the improved complete ensemble empirical-mode decomposition with adaptive noise (ICEEMDAN), were adopted for investigating emission-driven interannual variations in concentrations of air pollutants including PM2.5, PM10, O3, NO2, CO, SO2 and NO2 + O3 monitored in six cities in South China from May 2014 to April 2021. The first two methods were used to calculate the deweathered hourly concentrations, and the third one was used to calculate decomposed hourly residuals. To constrain the uncertainties in the calculated deweathered or decomposed hourly values, a self-developed method was applied to calculate the range of the deweathered percentage changes (DePCs) of air pollutant concentrations on an annual scale (each year covers May to the next April). These four methods were combined together to generate emission-driven trends and percentage changes (PCs) during the 7-year period. Consistent trends between the RF-deweathered and BRT-deweathered concentrations and the ICEEMDAN-decomposed residuals of an air pollutant in a city were obtained in approximately 70 % of a total of 42 cases (for seven pollutants in six cities), but consistent PCs calculated from the three methods, defined as the standard deviation being smaller than 10 % of the corresponding mean absolute value, were obtained in only approximately 30 % of all the cases. The remaining cases with inconsistent trends and/or PCs indicated large uncertainties produced by one or more of the three methods. The calculated PCs from the deweathered concentrations and decomposed residuals were thus combined with the corresponding range of DePCs calculated from the self-developed method to gain the robust range of DePCs where applicable. Based on the robust range of DePCs, we identified significant decreasing trends in PM2.5 concentration from 2014 to 2020 in Guangzhou and Shenzhen, which were mainly caused by the reduced air pollutant emissions and to a much lesser extent by weather perturbations. A decreasing or probably decreasing emission-driven trend was identified in Haikou and Sanya with inconsistent PCs, and a stable or no trend was identified in Zhanjiang with positive PCs. For O3, a significant increasing trend from 2014 to 2020 was identified in Zhanjiang, Shenzhen, Guangzhou and Haikou. An increasing trend in NO2 + O3 was also identified in Zhanjiang and Guangzhou and an increasing or probably increasing trend in Haikou, suggesting the contributions from enhanced formation of O3. The calculated PCs from using different methods implied that the emission changes in O3 precursors and the associated atmospheric chemistry likely played a dominant role than did the perturbations from varying weather conditions. Results from this study also demonstrated the necessity of combining multiple decoupling methods in generating emission-driven trends in atmospheric pollutants.

The accurate and rapid extraction of glacier boundaries plays an important role in the study of glacier inventory, glacier change and glacier movement. With the successive launches of high-resolution remote-sensing satellites and the increasing abundance of available remote-sensing data, great opportunities and challenges now exist. In this study, we improved the DeepLab V3+ as Attention DeepLab V3+ and designed a complete solution based on the improved network to automatically extract glacier outlines from Gaofen-6 panchromatic and multispectral (PMS) images with a spatial resolution of 2 m. In the solution, test-time augmentation (TTA) was adopted to increase model robustness, and the convolutional block attention module (CBAM) was added into the atrous spatial pyramid pooling (ASPP) structure in DeepLab V3+ to enhance the weight of the target pixels and reduce the impact of superfluous features. The results show that the improved model effectively increases the robustness of the model, enhances the weight of target image elements and reduces the influence of non-target elements. Compared with deep-learning models, such as full convolutional network (FCN), U-Net and DeepLab V3+, the improved model performs better in the test dataset. Moreover, our method achieves superior performance for glacier boundary extraction in parts of the Tanggula Mountains, the Kunlun Mountains and the Qilian Mountains based on Gaofen-6 PMS images. It could distinguish glaciers from terminal moraine lakes, thin snow and clouds, thus demonstrating excellent performance and great potential for rapid and precise extraction of glacier boundaries.

The length of a glacier is a key determinant of its geometry and is an important parameter in glacier inventories and modeling; glacier centerlines are the lines along which the main flow of glaciers takes place and, thus, are crucial inputs for many glaciological applications. In this study, the centerlines and maximum lengths of global glaciers were extracted using a self-designed automatic extraction algorithm based on the latest global glacier inventory data, digital elevation model (DEM), and European allocation theory. The accuracy of the dataset was evaluated through random visual assessments and comparisons with the Randolph Glacier Inventory (RGI) version 6.0. A total of 8.25 % of the outlines of the RGI were excluded, including 10 764 erroneous glacier polygons, 7174 ice caps, and 419 nominal glaciers. A total of 198 137 glacier centerlines were generated, accounting for 99.74 % of the input glaciers. The accuracy of glacier centerlines was 89.68 %. A comparison between the dataset and the previous dataset suggested that most glacier centerlines were slightly longer than those in RGI v6.0, meaning that the maximum lengths of some glaciers had been likely underestimated in the past. The constructed dataset comprises 17 sub-datasets, including global glacier centerlines, maximum lengths, and DEMs, all of which can be found at https://doi.org/10.11922/sciencedb.01643 (Zhang and Zhang, 2022).

Spatiotemporal heterogeneities in the concentrations of alkaline gases and their particulate counterparts in the marine atmosphere over China's marginal seas were investigated in terms of causes and chemical conversion during two winter cruise campaigns, using semi-continuous measurements made by an onboard URG-9000D Ambient Ion Monitor-Ion Chromatograph (AIM-IC, Thermo Fisher). During the cruise campaign over the East China Sea from 27 December 2019 to 6 January 2020, the concentrations of gas-phase atmospheric trimethylamine (TMAgas) varied by approximately 1 order of magnitude, with an average (± standard deviation) of 0.10±0.04 µg m−3 corresponding to a mixing ratio of 26±17 pptv. Corresponding mean values were 0.037±0.011 µg m−3 (14±5 pptv in mixing ratio) over the Yellow Sea during the period from 7 to 16 January 2020 and 0.031±0.009 µg m−3 (12±4 pptv in mixing ratio) over the Yellow Sea and Bohai Sea from 9 to 22 December 2019. By contrast, the simultaneously observed concentrations of TMA in PM2.5, detected as TMAH+, over the East China Sea were 0.098±0.069 µg m−3 and substantially smaller than the 0.28±0.18 µg m−3 observed over the Yellow Sea and Bohai Sea from 9 to 22 December 2019. A significant correlation between TMAgas and particulate TMAH+ was observed over the East China Sea, but no correlation was found over the Yellow Sea and Bohai Sea. Proportional or disproportional variations in concentrations of TMAgas with particulate TMAH+ over the sea zones were probably attributed to the difference in the enrichment of TMAH+ in the sea surface microlayer. In addition, spatiotemporal heterogeneities in concentrations of atmospheric ammonia (NH3gas), atmospheric dimethylamine (DMAgas), and DMA in PM2.5, detected as DMAH+, were investigated. Case analyses were performed to illustrate the formation and chemical conversion of particulate aminium ions in marine aerosols. Finally, we hypothesized the release of basic gases and particulate counterparts from the ocean to the atmosphere, together with the secondary formation of DMAH+ and chemical conversion of TMAH+, in the marine atmosphere.

Constraints are one of the main factors that hinder the optimal synthesis of linkages to obtain the global optimum. At present, the most commonly used constraint handling method is called the penalty function (PF) method, but this technique has proven to be inefficient and unreliable in path synthesis. In this paper, a novel and effective constraint handling method called the individual repairing (IR) method is developed for the optimization model of four-bar mechanisms for path synthesis. The function of the IR method is to check the conformity of each individual to the Grashof condition, the sequence condition, and the variable range condition after population initialization and each iteration as well as to repair all unreasonable individuals according to the corresponding repairing technique to make them all satisfy the constraint conditions. In other words, the new constraint handling method establishes a transformation method so that each infeasible point in the search space uniquely corresponds to a feasible point. Based on the IR method, the optimization of path synthesis can be effectively carried out. Finally, the validity and reliability of the new constraint handling method are verified using three examples.

Long-range transport of anthropogenic air pollutants from East Asia can affect the downwind marine air quality during spring and winter. Long-range transport of continental air pollutants and their interaction with sea salt aerosol (SSA) significantly modify the radiative forcing of marine aerosols and influence ocean biogeochemical cycling. Previous studies poorly characterize variations of aerosol particles along with air mass transport from the continental edge to the remote ocean. Here, the research ship R/V Dongfanghong 2 traveled from the eastern China seas (ECS) to the northwestern Pacific Ocean (NWPO) to understand what and how air pollutants were transported from the highly polluted continental air to clean marine air in spring. A transmission electron microscope (TEM) was used to find the long-range transported anthropogenic particles and the possible Cl-depletion phenomenon of SSA in marine air. Anthropogenic aerosols (e.g., sulfur (S)-rich, S-soot, S-metal/fly ash, organic matter (OM)-S, and OM coating particles) were identified and dramatically declined from 87 % to 8 % by number from the ECS to remote NWPO. For the SSA aging, 87 % of SSA particles in the ECS were identified as fully aged, while the proportion of fully aged SSA particles in the NWPO decreased to 29 %. Our results highlight that anthropogenic acidic gases in the troposphere (e.g., SO2, NOx, and volatile organic compounds) could be transported to remote marine air and exert a significant impact on aging of SSA particles in the NWPO. The study shows that anthropogenic particles and gases from East Asia significantly perturb different aerosol chemistry from coastal to remote marine air. More attention should be given to the modification of SSA particles in remote marine areas due to the influence of anthropogenic gaseous pollutants.

Atmospheric new particle formation (NPF) events have attracted increasing attention for their contribution to the global aerosol number budget and therefore their effects on climate, air quality and human health. NPF events are regarded as a regional phenomenon, occurring over a large area. Most observations of NPF events in Beijing and its vicinity were conducted in populated areas, whereas observations of NPF events on mountaintops with low anthropogenic emissions are still rare in China. The spatial variation of NPF event intensity has not been investigated in detail by incorporating both urban areas and mountain measurements in Beijing. Here, we provide NPF event characteristics in summer 2018 and 2019 at urban Beijing and a comparison of NPF event characteristics – NPF event frequency, formation rate and growth rate – by comparing an urban Beijing site and a background mountain site separated by ∼80 km from 14 June to 14 July 2019, as well as giving insights into the connection between both locations. During parallel measurements at urban Beijing and mountain background areas, although the median condensation sink during the first 2 h of the common NPF events was around 0.01 s−1 at both sites, there were notable differences in formation rates between the two locations (median of 5.42 cm−3 s−1 at the urban site and 1.13 cm−3 s−1 at the mountain site during the first 2 h of common NPF events). In addition, the growth rates in the 7–15 nm range for common NPF events at the urban site (median of 7.6 nm h−1) were slightly higher than those at the mountain site (median of 6.5 nm h−1). To understand whether the observed events were connected, we compared air mass trajectories as well as meteorological conditions at both stations. Favorable conditions for the occurrence of regional NPF events were largely affected by air mass transport. Overall, our results demonstrate a clear inhomogeneity of regional NPF within a distance of ∼100 km, possibly due to the discretely distributed emission sources.

To study sea-derived gaseous amines, ammonia, and primary particulate aminium ions in the marine atmosphere of China's marginal seas, an onboard URG-9000D Ambient Ion Monitor-Ion Chromatograph (AIM-IC, Thermo Fisher) was set up on the front deck of the R/V Dongfanghong-3 to semi-continuously measure the spatiotemporal variations in the concentrations of atmospheric trimethylamine (TMAgas), dimethylamine (DMAgas), and ammonia (NH3gas) along with their particulate matter (PM2.5) counterparts. In this study, we differentiated marine emissions of the gas species from continental transport using data obtained from 9 to 22 December 2019 during the cruise over the Yellow and Bohai seas, facilitated by additional short-term measurements collected at a coastal site near the Yellow Sea during the summer, fall, and winter of 2019. The data obtained from the cruise and coastal sites demonstrated that the observed TMAgas and protonated trimethylamine (TMAH+) in PM2.5 over the Yellow and Bohai seas overwhelmingly originated from marine sources. During the cruise, no significant correlation (P>0.05) was observed between the simultaneously measured TMAH+ and TMAgas concentrations. Additionally, the concentrations of TMAH+ in the marine atmosphere varied around 0.28±0.18 µg m−3 (average ± standard deviation), with several episodic hourly average values exceeding 1 µg m−3, which were approximately 1 order of magnitude larger than those of TMAgas (approximately 0.031±0.009 µg m−3). Moreover, there was a significant negative correlation (P) between the concentrations of TMAH+ and NH4+ in PM2.5. Therefore, the observed TMAH+ in PM2.5 was overwhelmingly derived from primary sea-spray aerosols. Using TMAgas and TMAH+ in PM2.5 as tracers for sea-derived basic gases and sea-spray particulate aminium ions, the values of non-sea-derived DMAgas, NH3gas, and non-sea-spray particulate DMAH+ in PM2.5 were estimated. The estimated average values of each species contributed 16 %, 34 %, and 65 % of the observed average concentrations for non-sea-derived DMAgas, NH3gas, and non-sea-spray particulate DMAH+ in PM2.5, respectively. Uncertainties remained in the estimations, as TMAH+ may decompose into smaller molecules in seawater to varying extents. The non-sea-derived gases and non-sea-spray particulate DMAH+ likely originated from long-range transport from the upwind continents based on the recorded offshore winds and increased concentrations of non-sea-salt SO42- (nss-SO42-) and NH4+ in PM2.5. The lack of a detectable increase in particulate DMAH+, NH4+, and nss-SO42- concentrations in several SO2 plumes did not support the secondary formation of particulate DMAH+ in the marine atmosphere.

Wet scavenging is an efficient pathway for the removal of particulate matter (PM) from the atmosphere. High levels of PM have been a major cause of air pollution in Beijing but have decreased sharply under the Air Pollution Prevention and Control Action Plan launched in 2013. In this study, 4 years of observations of wet deposition have been conducted using a sequential sampling technique to investigate the detailed variation in chemical components through each rainfall event. We find that the major ions, SO42-, Ca2+, NO3-, and NH4+, show significant decreases over the 2013–2017 period (decreasing by 39 %, 35 %, 12 %, and 25 %, respectively), revealing the impacts of the Action Plan. An improved method of estimating the below-cloud scavenging proportion based on sequential sampling is developed and implemented to estimate the contribution of below-cloud and in-cloud wet deposition over the four-year period. Overall, below-cloud scavenging plays a dominant role to the wet deposition of four major ions at the beginning of the Action Plan. The contribution of below-cloud scavenging for Ca2+, SO42-, and NH4+ decreases from above 50 % in 2014 to below 40 % in 2017. This suggests that the Action Plan has mitigated PM pollution in the surface layer and hence decreased scavenging due to the washout process. In contrast, we find little change in the annual volume weighted average concentration for NO3- where the contribution from below-cloud scavenging remains at ∼ 44 % over the 2015–2017 period. While highlighting the importance of different wet scavenging processes, this paper presents a unique new perspective on the effects of the Action Plan and clearly identifies oxidized nitrogen species as a major target for future air pollution controls.

Glacier centerlines are crucial input for many glaciological applications. From the morphological perspective, we proposed a new automatic method to derive glacier centerlines, which is based on the Euclidean allocation and the terrain characteristics of glacier surface. In the algorithm, all glaciers are logically classified as three types including simple glacier, simple compound glacier, and complex glacier, with corresponding process ranges from simple to complex. The process for extracting centerlines of glaciers introduces auxiliary reference lines and follows the setting of not passing through bare rock. The program of automatic extraction of glacier centerlines was implemented in Python and only required the glacier boundary and digital elevation model (DEM) as input. Application of this method to 48 571 glaciers in the second Chinese glacier inventory automatically yielded the corresponding glacier centerlines with an average computing time of 20.96 s, a success rate of 100 % and a comprehensive accuracy of 94.34 %. A comparison of the longest length of glaciers to the corresponding glaciers in the Randolph Glacier Inventory v6.0 revealed that our results were superior. Meanwhile, our final product provides more information about glacier length, such as the average length, and the longest length, the lengths in the accumulation and ablation regions of each glacier.

The growth of newly formed particles with diameters from ∼ 10 nm to larger sizes was investigated in Beijing's urban atmosphere during 10–23 December 2011, 12–27 April 2012, and June–August 2014. In 11 out of 27 new particle formation (NPF) events during June–August, the maximum geometric median diameter (Dpgmax) of newly formed particles exceeded 75 nm, and the grown new particles may contribute to the population of cloud condensation nuclei. In contrast, no apparent growth in new particles with Dpgmax < 20 nm was observed in all of the events in December, in approximately half of the NPF events in April, and in only two events during June–August. New particles observed in the latter NPF events were too small to be activated as cloud condensation nuclei. Apparent new particle growth with Dpgmax ≤ 50 nm was observed in the remaining 18 NPF events. The 11 NPF events during June–August with Dpgmax exceeding 75 nm were analyzed in detail. The particle growth patterns can be clearly classified into three types: one-stage growth and two-stage growth-A and growth-B patterns. The one-stage growth pattern is characterized by a continuous increase in Dpg with Dpgmax ≥ 80 nm (4 out of 11 NPF events), and the two-stage growth-A and growth-B patterns are characterized by no apparent growth and shrinkage of particles, respectively, in the middle 2–4 h of the growth period (7 out of 11 NPF events). Combining the observations of gaseous pollutants and measured (or modeled) concentrations of particulate chemical species, the three growth patterns were discussed in terms of the spatial heterogeneity of NPF, formation of secondary aerosols, and evaporation of semivolatile particulates. Secondary organic species and NH4NO3 were argued to be two major contributors to the growth of new particles, but NH4NO3 likely contributed to growth only in the late afternoon and/or at nighttime.

Because anthropogenic sulfur dioxide (SO2) emissions have decreased considerably in the last decade, PM2.5 pollution in China has been alleviated to some extent. However, the effects of reduced SO2 on the particle number concentrations and subsequent contributions of grown new particles to cloud condensation nuclei (CCN) populations, particularly at high altitudes with low aerosol number loadings, are poorly understood. In contrast, the increase in provincial forest areas in China with rapid afforestation over the last few decades expectedly increases the biogenic emissions of volatile organic compounds and their oxidized products as nucleating precursors therein. In this study, we evaluated the campaign-based measurements made at the summit of Mt. Tai (1534 m a.s.l.) from 2007 to 2018. With the decrease in SO2 mixing ratios from 15 ± 13 ppb in 2007 to 1.6 ± 1.6 ppb in 2018, the apparent formation rate (FR) of new particles and the net maximum increase in the nucleation-mode particle number concentration (NMINP) in the spring campaign of 2018 was 2- to 3-fold higher than those in the spring campaign of 2007 with almost the same occurrence frequency of new particle formation (NPF) events. In contrast, the campaign-based comparison showed that the occurrence frequency, in which the maximum geometric median diameter of the grown new particles (Dpgmax) was > 50 nm, decreased considerably from 43 %–78 % of the NPF events before 2015 to < 12 % in 2017–2018. Assuming > 50 nm as a CCN threshold size at high supersaturations, the observed net CCN production decreased from 3.7 × 103 cm−3 (on average) in the five campaigns before 2015 to 1.0 × 103 cm−3 (on average) in the two campaigns in 2017–2018. We argue that the increases in the apparent FR and NMINP are mainly determined by the availability of organic precursors that participate in nucleation and initial growth, whereas the decrease in the growth probability is caused by the reduced emissions of anthropogenic precursors. However, large uncertainties still exist because of a lack of data on the chemical composition of these smaller particles.

Surgical site infection risk continues to increase due to lack of efficacy in current standard of care drugs. New methods to treat or prevent antibiotic-resistant bacterial infections are needed. Multivalent Adhesion Molecules (MAM) are bacterial adhesins required for virulence. We developed a bacterial adhesion inhibitor using recombinant MAM fragment bound to polymer scaffold, mimicking MAM7 display on the bacterial surface. Here, we test MAM7 inhibitor efficacy to prevent Gram-positive and Gram-negative infections. Using a rodent model of surgical infection, incision sites were infected with antibiotic-resistant bioluminescent strains of Staphylococcus aureus or Pseudomonas aeruginosa. Infections were treated with MAM7 inhibitor or control suspension. Bacterial abundance was quantified for nine days post infection. Inflammatory responses and histology were characterized using fixed tissue sections. MAM7 inhibitor treatment decreased burden of S. aureus and P. aeruginosa below detection threshold. Bacterial load of groups treated with control were significantly higher than MAM7 inhibitor-treated groups. Treatment with inhibitor reduced colonization of clinically-relevant pathogens in an in vivo model of surgical infection. Use of MAM7 inhibitor to block initial adhesion of bacteria to tissue in surgical incisions may reduce infection rates, presenting a strategy to mitigate overuse of antibiotics to prevent surgical site infections.

Water-soluble inorganic ions such as ammonium, nitrate and sulfate are major components of fine aerosols in the atmosphere and are widely used in the estimation of aerosol acidity. However, different experimental practices and instrumentation may lead to uncertainties in ion concentrations. Here, an intercomparison experiment was conducted in 10 different laboratories (labs) to investigate the consistency of inorganic ion concentrations and resultant aerosol acidity estimates using the same set of aerosol filter samples. The results mostly exhibited good agreement for major ions Cl−, SO42-, NO3-, NH4+ and K+. However, F−, Mg2+ and Ca2+ were observed with more variations across the different labs. The Aerosol Chemical Speciation Monitor (ACSM) data of nonrefractory SO42-, NO3- and NH4+ generally correlated very well with the filter-analysis-based data in our study, but the absolute concentrations differ by up to 42 %. Cl− from the two methods are correlated, but the concentration differ by more than a factor of 3. The analyses of certified reference materials (CRMs) generally showed a good detection accuracy (DA) of all ions in all the labs, the majority of which ranged between 90 % and 110 %. The DA was also used to correct the ion concentrations to showcase the importance of using CRMs for calibration check and quality control. Better agreements were found for Cl−, SO42-, NO3-, NH4+ and K+ across the labs after their concentrations were corrected with DA; the coefficient of variation (CV) of Cl−, SO42-, NO3-, NH4+ and K+ decreased by 1.7 %, 3.4 %, 3.4 %, 1.2 % and 2.6 %, respectively, after DA correction. We found that the ratio of anion to cation equivalent concentrations (AE / CE) and ion balance (anions–cations) are not good indicators for aerosol acidity estimates, as the results in different labs did not agree well with each other. In situ aerosol pH calculated from the ISORROPIA II thermodynamic equilibrium model with measured ion and ammonia concentrations showed a similar trend and good agreement across the 10 labs. Our results indicate that although there are important uncertainties in aerosol ion concentration measurements, the estimated aerosol pH from the ISORROPIA II model is more consistent.

In this study, a cruise campaign was conducted over marginal seas in China to measure the concentrations of condensation nuclei (Ncn), cloud condensation nuclei (Nccn) and other pollutants from day of year (DOY) 110 to DOY 135 of 2018. The ship self-emission signals were exhaustively excluded, and the mean values of Nccn during the cruise campaign were found to slightly increase from 3.2±1.1×103 cm−3 (mean ± standard deviation) at supersaturation (SS) of 0.2 % to 3.9±1.4×103 cm−3 at SS of 1.0 %, and the mean value for Ncn was 8.1±4.4×103 cm−3. Data analysis showed that marine traffic emissions apparently largely contributed to the increase in Ncn in the daytime, especially in the marine atmospheres over heavily traveled sea zones; however, the fresh sources made no clear contribution to the increase in Nccn. This finding was supported by the quantitative relations between Ncn and Nccn at SS = 0.2 %–1.0 % against the mixing ratios of SO2 in the ship self-emission plumes – i.e., a 1 ppb increase in SO2 corresponded to a 1.4×104 cm−3 increase in Ncn but only a 30–170 cm−3 increase in Nccn, possibly because of abundant organics in the aerosols. Smooth growth can be observed in the marine-traffic-derived particles, reflecting aerosol aging. The estimated hygroscopicity parameter (κ) values were generally as high as 0.46–0.55 under the dominant onshore winds, suggesting that inorganic ammonium aerosols likely acted as the major contributor to Nccn largely through aerosol aging processes of decomposing organics. Moreover, the influences of the new transported particles from the continent on the Ncn and Nccn in the marine atmosphere were investigated.

Two single-particle aerosol mass spectrometers (SPAMSs) were deployed simultaneously at an urban and a rural site in Beijing during an intensive field campaign from 1 to 29 November 2016 to investigate the source and process of airborne particles in Beijing. In the first part of this research, we report the single-particle chemical composition, mixing state, and evolution at both sites. A total of 96 % and 98 % of collected particles were carbonaceous at the urban and rural sites, respectively. Five particle categories, including elemental carbon (EC), organic carbon (OC), internal-mixed EC and OC (ECOC), potassium-rich (K-rich), and metals, were observed at both sites. The categories were partitioned into particle types depending on different atmospheric processing stages. A total of 17 particle types were shared at both sites. In the urban area, nitrate-containing particle types, such as EC-Nit (Nit: nitrate) and ECOC-Nit, were enriched especially at night, sulfate-containing particles were transported when wind speed was high, and ECOC-Nit-Sul (Sul: sulfate) were mostly aged locally. In sum, these processed particles added up to 85.3 % in the urban areas. In the rural area, regional particles were abundant, but freshly emitted ECOC and OC had distinct patterns that were pronounced at cooking and heating times. Biomass burning, traffic, and coal burning were major sources of particulate matter (PM2.5) in both rural and urban areas. Moreover, particles from the steel industry located in the south were also identified. In summary, the chemical composition of urban and rural particle types was similar in Beijing; the urban particles were influenced significantly by rural processing and transport. The work is useful to understand the evolution of urban and rural particles in Beijing during winter.

Two parallel field studies were conducted simultaneously at both urban and rural sites in Beijing from 1 to 29 November 2016. An online single-particle chemical composition analysis was used as a tracer system to investigate the impact of heating activities and the formation of haze events. Central heating elevated EC-Nit (elemental carbon-nitrate), EC-Nit-Sul (EC-nitrate-sulfate), and ECOC-Nit (ECOC: internal-mixed elemental carbon and organic carbon) levels by 1.5–2.0 times due to the increased use of coal in the urban areas. However, in the rural areas, residential heating, which mainly consumes low-quality coal, and biomass burning elevated ECOC-Nit-Sul, NaK-Nit, and OC-Sul levels by 1.2–1.5 times. Four severe haze events (hourly PM2.5 > 200 µg m−3) occurred at both sites during the studies. In each event, a pattern of transport and accumulation was found. In the first stage of the pattern, particles were regionally transported from the south and southwest and accumulated under air stagnation, creating significant secondary formation, then PM2.5 was elevated to 300 µg m−3. At both sites, the severe haze occurred due to different patterns of local emission, transport, and secondary processes. At Pinggu (PG), the sulfate-rich residential coal burning particles were dominant. The regional transport between PG and Peking University (PKU) was simulated using the Weather Research and Forecasting HYbrid Single-Particle Lagrangian Integrated Trajectory (WRF-HYSPLIT) model, confirming that the transport from PG to PKU was significant, but PKU to PG occurred occasionally. These cases can explain the serious air pollution in the urban areas of Beijing and the interaction between urban and rural areas. This study can provide references for enhancing our understanding of haze formation in Beijing.

We investigated the geographic distributions of organic tracers in total suspended particles over the marginal seas of China, including the Yellow and Bohai seas (YBS) and the South China Sea (SCS), and the northwest Pacific Ocean (NWPO) in spring, when Asian outflows strongly affect downwind marine atmospheres. The comparison of levoglucosan observed in this study with values from the literature showed that the concentrations of biomass burning aerosols over the NWPO increased largely in 2014. However more observations, in addition to our snapshot measurement, are need to confirm whether the large increase has occurred continuously over the last few decades. The increase led to a mean observed levoglucosan value (8.2±14 ng m−3) over the NWPO that was close to that over the SCS (9.6±8.6 ng m−3) and almost half of that over the YBS (21±11 ng m−3). Small geographic differences in monoterpene-derived and sesquiterpene-derived secondary organic tracer concentrations were obtained among the three atmospheres, although the causes may differ. By contrast, a large difference in isoprene-derived secondary organic tracer concentrations was observed among the three atmospheres, with the sum of tracer concentrations over the SCS (45±54 ng m−3) being several times and approximately 1 order of magnitude greater than that over the YBS (15±16 ng m−3) and the NWPO (2.3±1.6 ng m−3), respectively. The geographic distribution of aromatic-derived secondary organic tracers was similar to that of isoprene-derived secondary organic tracers, with a slightly narrower difference: 1.8±1.7, 1.1±1.4 and 0.3±0.5 ng m−3 over the SCS, the YBS and the NWPO, respectively. We discuss the causes of the distinctive geographic distributions of these tracers and present the tracer-based estimation of organic carbon.

Long-term trends of wet deposition of inorganic ions are affected by multiple factors, among which emission changes and climate conditions are dominant ones. To assess the effectiveness of emission reductions on the wet deposition of pollutants of interest, contributions from these factors to the long-term trends of wet deposition must be isolated. For this purpose, a two-step approach for preprocessing wet deposition data is presented herein. This new approach aims to reduce the impact of climate anomalies on the trend analysis so that the impact of emission reductions on the wet deposition can be revealed. This approach is applied to a 2-decade wet deposition dataset of sulfate (SO42-), nitrate (NO3-), and ammonium (NH4+) at rural Canadian sites. Analysis results show that the approach allows for statistically identifying inflection points on decreasing trends in the wet deposition fluxes of SO42- and NO3- in northern Ontario and Quebec. The inflection points match well with the three-phase mitigation of SO2 emissions and two-phase mitigation of NOx emissions in Ontario. Improved correlations between the wet deposition of ions and their precursors' emissions were obtained after reducing the impact from climate anomalies. Furthermore, decadal climate anomalies were identified as dominating the decreasing trends in the wet deposition fluxes of SO42- and NO3- at a western coastal site. Long-term variations in NH4+ wet deposition showed no clear trends due to the compensating effects between NH3 emissions, climate anomalies, and chemistry associated with the emission changes of sulfur and nitrogen.

In the summer of 2017, heavy ozone pollution swamped most of the North China Plain (NCP), with the maximum regional average of daily maximum 8 h ozone concentration (MDA8) reaching almost 120 ppbv. In light of the continuing reduction of anthropogenic emissions in China, the underlying mechanisms for the occurrences of these regional extreme ozone episodes are elucidated from two perspectives: meteorology and biogenic emissions. The significant positive correlation between MDA8 ozone and temperature, which is amplified during heat waves concomitant with stagnant air and no precipitation, supports the crucial role of meteorology in driving high ozone concentrations. We also find that biogenic emissions are enhanced due to factors previously not considered. During the heavy ozone pollution episodes in June 2017, biogenic emissions driven by high vapor pressure deficit (VPD), land cover change and urban landscape yield an extra mean MDA8 ozone of 3.08, 2.79 and 4.74 ppbv, respectively, over the NCP, which together contribute as much to MDA8 ozone as biogenic emissions simulated using the land cover of 2003 and ignoring VPD and urban landscape. In Beijing, the biogenic emission increase due to urban landscape has a comparable effect on MDA8 ozone to the combined effect of high VPD and land cover change between 2003 and 2016. In light of the large effect of urban landscape on biogenic emission and the subsequent ozone formation, the types of trees may be cautiously selected to take into account of the biogenic volatile organic compound (BVOC) emission during the afforestation of cities. This study highlights the vital contributions of heat waves, land cover change and urbanization to the occurrence of extreme ozone episodes, with significant implications for ozone pollution control in a future when heat wave frequency and intensity are projected to increase under global warming.

Iron metal anode satisfies the safety, low-cost, non-toxicity, and energy-dense pursuits chasing by the battery community, but passivation, parasitic hydrogen evolution reaction, and low plating efficiency challenging its electrochemical performance limit its continuous practical applications. Here, the redox behaviors of the iron metal anode in both alkaline and acidic electrolytes have been summarized first to shape the fundamental mechanisms. Recent progress in developing high-performance iron metal anodes has been introduced with the highlights on representative strategies, including electrode additives, electrolyte modification, and nanoarchitecture. Especially, the history of aqueous battery systems with iron metal anode is overviewed from its earliest beginning to the new era, following by the discussion regarding the specialization of each system. We believe this review could bring the fundament of redox behavior for optimizing the iron metal anode and pave a way toward a reliable iron-based aqueous battery.

Determination of the updated concentrations of atmospheric particles (Ncn) and the concentrations of cloud condensation nuclei (Nccn) over the northwestern Pacific Ocean (NWPO) are important to accurately evaluate the influence of aerosol outflow from the Asian continent on the climate by considering the rapid changes in emissions of air pollutants therein. However, field observations in the last two decades are scarce. We conducted a cruise campaign over the NWPO to simultaneously measure Ncn, Nccn and the size distribution of aerosol particles from day of year (DOY) 81 to DOY 108 of 2014. The mean values of Nccn at supersaturation (SS) of levels 0.2 % and 0.4 % were 0.68±0.38×103 and 1.1±0.67×103 cm−3, respectively, with an average of 2.8±1.0×103 cm−3 for Ncn during the cruise over the NWPO. All are approximately 1 order of magnitude larger than spring observations made during the preceding two decades in the remote marine atmosphere. The larger values, against the marine natural background reported in the literature, imply an overwhelming contribution from continental inputs. The calculated activity ratios (ARs) of the cloud condensation nuclei (CCN) were 0.30±0.11 and 0.46±0.19 at SS levels of 0.2 % and 0.4 %, respectively, which are almost the same as those of upwind semi-urban sites. High Nccn and CCN activities were observed from DOY 98 to DOY 102, when the oceanic zone received even stronger continental input. Excluding biomass burning (BB) and dust aerosols, good correlation between Nccn at 0.4 % SS and the number concentrations of > 60 nm particles (N>60 nm) was obtained during the entire cruise period, with a slope of 0.98 and R2=0.94, and the corresponding effective hygroscopicity parameter (κ) was estimated to be 0.40. A bimodal size distribution pattern of the particle number concentration was generally observed during the entire campaign when the N>90 nm varied largely. However, the N, accounting for approximately one-third of the total number concentration, varied narrowly, and two NPF events associated with vertical transport were observed. This implies that a pool of nucleation-mode atmospheric particles is aloft. BB and dust events were observed over the NWPO, but their aerosol contributions to Ncn and Nccn were minor (i.e., 10 % or less) on a monthly timescale.

The seismic effects in Nyalam, Gyirong, Tingri and Dinggye counties along the southern border of Tibet were investigated during 2–8 May 2015, a week after the great Nepal earthquake along the Main Himalaya Thrust. The intensity was VIII in the region and reached IX at two towns on the Nepal border, resulting in the destruction of 2700 buildings, seriously damaging over 40 000 others, while killing 27 people and injuring 856 in this sparsely populated region. The main geologic effects in this steep rugged region are collapses, landslides, rockfalls, and ground fissures, many of which are reactivations of older land slips. These did great damage to the buildings, roads, and bridges in the region. Most of the effects are along four incised valleys which are controlled by N-trending rifts and contain rivers that pass through the Himalaya Mountains and flow into Nepal; at least two of the larger aftershocks occurred along the normal faults. And, the damage is not related to the faulting of N-trending rifts but rather is distributed along the intensity of Nepal earthquake. Areas weakened by the earthquake pose post-seismic hazards. Another main characteristic of damage is the recurrence of the old landslide and rockfalls. In addition, there is an increased seismic hazard along active N-trending grabens in southern Tibet due to the shift in stress resulting from the thrust movement that caused the Nepal earthquake. NW-trending right-lateral strike-slip faults also may be susceptible to movement. The results of the findings are incorporated in some principle recommendations for the repair and reconstruction after the earthquake.

Utilizing a recent observational dataset of particulate matter with diameters less than 2.5 µm (PM2.5) in North China, this study reveals a distinct seesaw feature of abnormally high and low PM2.5 concentrations in the adjacent two months of December 2015 and January 2016, accompanied by distinct meteorological modulations. The seesaw pattern is postulated to be linked to a super El Niño and the Arctic Oscillation (AO). During the mature phase of El Niño in December 2015, the weakened East Asian winter monsoon (EAWM) and the associated low-level southerly wind anomaly reduced planetary boundary layer (PBL) height, favoring strong haze formation. This circulation pattern was completely reversed in the following month, in part due to a sudden phase change of the AO from positive to negative and the beginning of a decay of the El Niño, which enhanced the southward shift of the upper tropospheric jet from December to January relative to climatology, leading to an enhanced EAWM and substantially lower haze formation. This sub-seasonal change in circulation is also robustly found in 1982–1983 and 1997–1998, implicative of a general physical mechanism dynamically linked to El Niño and the AO. Numerical experiments using the Weather Research and Forecasting (WRF) Community Multiscale Air Quality (CMAQ) model were used to test the modulation of the meteorological conditions on haze formation. With the same emission, simulations for three super El Niño periods (1983, 1997 and 2015) robustly show higher PM2.5 concentrations under the mature phase of the super El Niño, but substantially lower PM2.5 concentrations during the decay phase of El Niño (and the sudden AO phase change), further verifying the modulation effect of the sub-seasonal circulation anomaly on PM2.5 concentrations in North China.

We measured the particle number concentration, size distribution, and new particle formation (NPF) events in the marine atmosphere during six cruise campaigns over the marginal seas of China in 2011–2016 and one campaign from the marginal seas to the Northwest Pacific Ocean (NWPO) in 2014. We observed relatively frequent NPF events in the atmosphere over the marginal seas of China, i.e., on 23 out of 126 observational days, with the highest frequency of occurrence in fall, followed by spring and summer. In total, 22 out of 23 NPF events were found to be associated with the long-range transport of continental pollutants based on 24 h air mass back trajectories and pre-existing particle number concentrations, which largely exceeded the clean marine background, leaving one much weaker NPF event that was likely induced by oceanic precursors alone, as supported by multiple independent pieces of evidence. Although the long-range transport signal of continental pollutants can be clearly observed in the remote marine atmosphere over the NWPO, NPF events were observed on only 2 out of 36 days. The nucleation-mode particles (<30 nm), however, accounted for as high as 35 %±13 % of the total particle number concentration during the NWPO cruise campaign, implying the existence of many undetected NPF events in the near-sea-level atmosphere or above. To better characterize NPF events, we introduce a term called the net maximum increase in the nucleation-mode particle number concentration (NMINP) and correlate it with the formation rate of new particles (FR). We find a moderately good linear correlation between NMINP and FR at FR≤8 cm−3 s−1, but no correlation exists at FR>8 cm−3 s−1. The possible mechanisms are argued in terms of the roles of different vapor precursors. We also find that a ceiling exists for the growth of new particles from 10 nm to larger sizes in most NPF events. We thereby introduce a term called the maximum geometric median diameter of new particles (Dpgmax) and correlate it with the growth rate of new particles (GR). A moderately good linear correlation is also obtained between the Dpgmax and GR, and only GR values larger than 7.9 nm h−1 can lead to new particles growing with a Dpgmax beyond 50 nm based on the equation. By combining simultaneous measurements of the particle number size distributions and cloud condensation nuclei (CCN) at different super saturations (SS), we observed a clear increase in CCN when the Dpg of new particles exceeded 50 nm at SS=0.4 %. However, this case did not occur for SS=0.2 %. Consistent with the results of previous studies in the continental atmosphere, our results imply that particles smaller than 50 nm are unlikely activated as CCN at SS=0.4 % in the marine atmosphere. Moreover, κ decrease from 0.4 to 0.1 during the growth period of new particles, implying that organics likely overwhelm the growth of new particles to CCN size. The chemical analysis of nano-Micro-Orifice Uniform Deposit Impactor (nano-MOUDI) samples reveals that trimethylamine (TMA) and oxalic acid might appreciably contribute to the growth of new particles in some cases.

A multi-model ensemble of Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) simulations is used to study the atmospheric oxidized nitrogen (NOy) deposition over East Asia under climate and emission changes projected for the future. Both dry and wet NOy deposition show significant decreases in the 2100s under RCP4.5 and RCP8.5, primarily due to large anthropogenic emission reduction over both land and sea. However, in the near future of the 2030s, both dry and wet NOy deposition increase significantly due to continued increase in emissions. Marine primary production from both dry and wet NOy deposition increases by 19 %–34 % in the 2030s and decreases by 34 %–63 % in the 2100s over the East China Sea. The individual effect of climate or emission changes on dry and wet NOy deposition is also investigated. The impact of climate change on dry NOy deposition is relatively minor, but the effect on wet deposition, primarily caused by changes in precipitation, is much higher. For example, over the East China Sea, wet NOy deposition increases significantly in summer due to climate change by the end of this century under RCP8.5, which may subsequently enhance marine primary production. Over the coastal seas of China, as the transport of NOy from land becomes weaker due to the decrease in anthropogenic emissions, the effect of ship emissions and lightning emissions becomes more important. On average, the seasonal mean contribution of ship emissions to total NOy deposition is projected to be enhanced by 24 %–48 % and 3 %–37 % over the Yellow Sea and East China Sea, respectively, by the end of this century. Therefore, continued control of both anthropogenic emissions over land and ship emissions may reduce NOy deposition to the Chinese coastal seas.

The continent-to-ocean supply of phosphorus (P) in the soluble state, recognized as bioavailable P, via the atmosphere is hypothesized to be crucial to the biological cycle in offshore surface seawater. To investigate the solubility of P in aerosol particles moving towards the northwestern Pacific from the Asian continent, we measured the total P (TP), total dissolved P (TDP) and dissolved inorganic P (DIP) in aerosols at Qingdao (36∘06′ N, 120∘33′ E), a coastal city in eastern China. The samples were collected in December 2012 and January 2013 (winter) and in March and April 2013 (spring), when the middle-latitude westerly wind was prevailing. On average, P solubility, i.e., the ratio of TDP to TP, was 32.9±16.7 % in winter and 21.3±9.8 % in spring, and the TP concentrations in the two seasons were similar. This seasonal solubility difference is attributed to the aerosol sources containing the P. Particles in winter were predominantly anthropogenic particles from local and regional areas, and particles in spring were significantly influenced by natural dust from the arid and semiarid areas in the inland part of the continent. Moreover, acidification processes associated with the formation of sulfate and nitrate in the winter samples enhanced P solubility, suggesting that the P in anthropogenic particles was more susceptible to the production of acidic species than that in natural dust particles. There was a strong positive correlation between P solubility and relative humidity (RH). P solubility was usually less than 30 % when RH was below 60 %, even when the content of acidic species and/or anthropogenic particles in the aerosols was high, suggesting humidity had a critical role in the production of TDP. In addition, the proportion of DIP in TDP was high when the particles were predominantly anthropogenic, and the proportion of dissolved organic P (DOP; quantified as TDP minus DIP) in TDP was high when the particles were dominated by natural dust. These results indicate that, as the contents of bioavailable P in Asian continent outflows are closely dependent on the aerosol particle origins, atmospheric acidic processes could convert P into a bioavailable state under certain meteorological conditions. Therefore, the recent severe air pollution over East Asia might have enhanced the input of bioavailable P to downwind marine areas.

Assessments of the burden of air pollution at the national scale over long-term of time in China would help government managers control historic health impacts of air pollution and institute measures to avoid these risks in future. We took a new 0.01° × 0.01° satellite-based PM2.5 dataset to analyse spatial and temporal trends of PM2.5 associated premature mortality in China from 1998 to 2017. Results showed that national PM2.5 related deaths from STK, IHD, COPD, LC and ALRI increased from approximately 0.89 million cases in 1998 to the peak of 1.34 million in 2014 and steady declined to 1.17 million cases in 2017. The health burden exhibited strong spatial variations, with high attributable deaths concentrated in regions such as Shandong, Hebei, Henan, Beijing, Guangdong, et al. Changing trends varied from different provinces such as Shandong increased mostly, and Sichuan showed a significant decreasing trend. Meanwhile, the results also showed that the expand directions of premature mortality was similar to that of population and the changing of absolute number of premature mortality more depended on the growth of PM2.5 concentration. The findings recommend that government should make better policies to the health risk controlling which take population and pollution into consideration than only focus on pollution concentration.

A comprehensive adaptive compensation control strategy based on feedback linearization design is proposed for multivariable nonlinear systems with uncertain actuator fault and unknown mismatched disturbances. Firstly, the linear dynamic system is obtained through nonlinear feedback linearization, and the dynamic model of the mismatched disturbances as well as its relevance to the nonlinear system is given. The effect of disturbances on the system output is suppressed with the basic controller of the linearized system. Then, a direct adaptive controller is developed for the multiple uncertain actuator faults. Finally, an integrated algorithm based on adaptive weighted fusion could provide an effective compensation for the effect of multiple uncertain faults and mismatched disturbances. Thus, the stability and asymptotic tracking performance of the closed-loop system are ensured. The feasibility and performance of the proposed control strategy are validated by the numerical simulation results.

A fast Fourier transform was applied to fit the geomagnetic diurnal variation. Fitting results showed that when the polynomial degree was greater than 160, the residual error was close to 0 nT. White noise is the main component of the residual error when the polynomial degree was greater than 160, so this method was adopted to calculate the background noise of the geomagnetic field. Spectrum analysis further demonstrated that the noise estimation result is reliable.

Atmospheric deposition of long-range transport of anthropogenic reactive nitrogen (Nr, mainly comprised of NHx, NOy and water-soluble organic nitrogen, WSON) from continents may have profound impact on marine biogeochemistry. In addition, surface ocean dissolved organic nitrogen (DON) may also contribute to aerosol WSON in the overlying atmosphere. Despite the importance of off-continent dispersion and Nr interactions at the atmosphere–ocean boundary, our knowledge of the sources of various nitrogen species in the atmosphere over the open ocean remains limited due to insufficient observations. We conducted two cruises in the spring of 2014 and 2015 from the coast of China through the East China seas (ECSs, i.e. the Yellow Sea and East China Sea) to the open ocean (i.e. the Northwest Pacific Ocean, NWPO). Concentrations of water-soluble total nitrogen (WSTN), NO3− and NH4+, as well as the δ15N of WSTN and NO3− in marine aerosol, were measured during both cruises. In the spring of 2015, we also analysed the concentrations and δ15N of NO3− and the DON of surface seawater (SSW; at a depth of 5 m) along the cruise track. Aerosol NO3−, NH4+ and WSON decreased logarithmically (1–2 orders of magnitude) with distance from the shore, reflecting strong anthropogenic emission sources of NO3−, NH4+ and WSON in China. Average aerosol NO3− and NH4+ concentrations were significantly higher in 2014 (even in the remote NWOP) than in 2015 due to the stronger wind field in 2014, underscoring the role of the Asian winter monsoon in the seaward transport of anthropogenic NO3− and NH4+. However, the background aerosol WSON over the NWPO in 2015 (13.3 ± 8.5 nmol m−3) was similar to that in 2014 (12.2 ± 6.3 nmol m−3), suggesting an additional non-anthropogenic WSON source in the open ocean. Obviously, marine DON emissions should be considered in model and field assessments of net atmospheric WSON deposition in the open ocean. This study contributes information on parallel isotopic marine DON composition and aerosol Nr datasets, but more research is required to explore complex Nr sources and deposition processes in order to advance our understanding of anthropogenic influences on the marine nitrogen cycle and nitrogen exchange at land–ocean and atmosphere–ocean interfaces.

In this study, five on-board microcosm experiments were performed in the subtropical gyre, the Kuroshio Extension region of the northwest Pacific Ocean (NWPO), and the Yellow Sea (YS) in order to investigate phytoplankton growth following the addition of artificially modified mineral dust (AM dust) and various nutrients (nitrogen (N), phosphorus (P), iron (Fe), N + P, and N + P + Fe). The two experiments carried out with AM-dust addition in the subtropical gyre showed a maximum chlorophyll a (Chl a) concentration increase of 1.7- and 2.8-fold, while the cell abundance of large-sized phytoplankton ( > 5 µm) showed a 1.8- and 3.9-fold increase, respectively, relative to the controls. However, in the Kuroshio Extension region and the YS, the increases in maximum Chl a and cell abundance of large-sized phytoplankton following AM-dust addition were at most 1.3-fold and 1.7-fold larger than those in the controls, respectively. A net conversion efficiency index (NCEI) newly proposed in this study, size-fractionated Chl a, and the abundance of large-sized phytoplankton were analysed to determine which nutrients contribute to supporting phytoplankton growth. Our results demonstrate that a combination of nutrients, N–P or N + P + Fe, is responsible for phytoplankton growth in the subtropical gyre following AM-dust addition. Single nutrient addition, i.e., N in the Kuroshio Extension region and P or N in the YS, controls the phytoplankton growth following AM-dust addition. In the AM-dust-addition experiments, in which the increased N–P or P was identified to determine phytoplankton growth, the dissolved inorganic P from AM dust (8.6 nmol L−1) was much lower than the theoretically estimated minimum P demand (∼ 20 nmol L−1) for phytoplankton growth. These observations suggest that additional supply augments the bioavailable P stock in incubated seawater with AM-dust addition, most likely due to an enhanced solubility of P from AM dust or the remineralization of the dissolved organic P.

Asian dust has been reported to carry anthropogenic reactive nitrogen during transport from source areas to the oceans. In this study, we attempted to characterize NH4+ and NO3− in atmospheric particles collected at a coastal site in northern China during spring dust events from 2008 to 2011. Based on the mass concentrations of NH4+ and NO3− in each total suspended particle (TSP) sample, the samples can be classified into increasing or decreasing types. In Category 1, the concentrations of NH4+ and NO3− were 20–440 % higher in dust day samples relative to samples collected immediately before or after a dust event. These concentrations decreased by 10–75 % in the dust day samples in Categories 2 and 3. Back trajectory analysis suggested that multiple factors, such as the transport distance prior to the reception site, the mixing layer depth on the transport route and the residence time across highly polluted regions, might affect the concentrations of NH4+ and NO3−. NH4+ in the dust day samples was likely either in the form of ammonium salts existing separately to dust aerosols or as the residual of incomplete reactions between ammonium salts and carbonate salts. NO3− in the dust day samples was attributed to various formation processes during the long-range transport. The positive matrix factorization (PMF) receptor model results showed that the contribution of soil dust increased from 23 to 36 % on dust days, with decreasing contributions from local anthropogenic inputs and associated secondary aerosols. The estimated deposition flux of NNH4++NO3− varied greatly from event to event; e.g., the dry deposition flux of NNH4++NO3− increased by 9–285 % in Category 1 but decreased by 46–73 % in Category 2. In Category 3, the average dry deposition fluxes of particulate nitrate and ammonium decreased by 46 % and increased by 10 %, respectively, leading to 11–48 % decrease in the fluxes of NNH4++NO3−.

This study is the first to use two identical Fast Mobility Particle Sizers for simultaneous measurement of particle number size distributions (PNSDs) at a street site and a rooftop site within 500 m distance in wintertime and springtime to investigate new particle formation (NPF) in Beijing. The collected datasets at 1 s time resolution allow deduction of the freshly emitted traffic particle signal from the measurements at the street site and thereby enable the evaluation of the effects on NPF in an urban atmosphere through a site-by-site comparison. The number concentrations of 8 to 20 nm newly formed particles and the apparent formation rate (FR) in the springtime were smaller at the street site than at the rooftop site. In contrast, NPF was enhanced in the wintertime at the street site with FR increased by a factor of 3 to 5, characterized by a shorter NPF time and higher new particle yields than at the rooftop site. Our results imply that the street canyon likely exerts distinct effects on NPF under warm or cold ambient temperature conditions because of on-road vehicle emissions, i.e., stronger condensation sinks that may be responsible for the reduced NPF in the springtime but efficient nucleation and partitioning of gaseous species that contribute to the enhanced NPF in the wintertime. The occurrence or absence of apparent growth for new particles with mobility diameters larger than 10 nm was also analyzed. The oxidization of biogenic organics in the presence of strong photochemical reactions is suggested to play an important role in growing new particles with diameters larger than 10 nm, but sulfuric acid is unlikely to be the main species for the apparent growth. However, the number of datasets used in this study is relatively small, and larger datasets are essential to draw a general conclusion.

In a stratified water column, the nitracline is a layer where the nitrate concentration increases below the nutrient-depleted upper layer, exhibiting a strong vertical gradient in the euphotic zone. The subsurface chlorophyll maximum layer (SCML) forms near the bottom of the euphotic zone, acting as a trap to diminish the upward nutrient supply. Depth and steepness of the nitracline are important measurable parameters related to the vertical transport of nitrate into the euphotic zone. The correlation between the SCML and the nitracline has been widely reported in the literature, but the analytic solution for the relationship between them is not well established. By incorporating a piecewise function for the approximate Gaussian vertical profile of chlorophyll, we derive analytical solutions of a specified nutrient–phytoplankton model. The model is well suited to explain basic dependencies between a nitracline and an SCML. The analytical solution shows that the nitracline depth is deeper than the depth of the SCML, shoaling with an increase in the light attenuation coefficient and with a decrease in surface light intensity. The inverse proportional relationship between the light level at the nitracline depth and the maximum rate of new primary production is derived. Analytic solutions also show that a thinner SCML corresponds to a steeper nitracline. The nitracline steepness is positively related to the light attenuation coefficient but independent of surface light intensity. The derived equations of the nitracline in relation to the SCML provide further insight into the important role of the nitracline in marine pelagic ecosystems.

Interannual variabilities in atmospheric ammonia (NH3) during the most recent 7–11 years were investigated at 14 sites across North America using the monitored data obtained from NAPS, CAPMoN and AMoN networks. The long-term average of atmospheric NH3 ranged from 0.8 to 2.6 ppb, depending on location, at four urban and two rural/agricultural sites in Canada. The annual average at these sites did not show any deceasing trend with largely decreasing anthropogenic NH3 emission. An increasing trend was actually identified from 2003 to 2014 at the downtown Toronto site using either the Mann–Kendall or the ensemble empirical mode decomposition method, but “no” or “stable” trends were identified at other sites. The ∼ 20 % increase during the 11-year period at the site was likely caused by changes in NH4+–NH3 partitioning and/or air–surface exchange process as a result of the decreased sulfur emission and increased ambient temperature. The long-term average from 2008 to 2015 was 1.6–4.9 ppb and 0.3–0.5 ppb at four rural/agricultural and at four remote US sites, respectively. A stable trend in NH3 mixing ratio was identified at one rural/agricultural site while increasing trends were identified at three rural/agricultural (0.6–2.6 ppb, 20–50 % increase from 2008 to 2015) and four remote sites (0.3–0.5 ppb, 100–200 % increase from 2008 to 2015). Increased ambient temperature was identified to be a cause for the increasing trends in NH3 mixing ratio at four out of the seven US sites, but what caused the increasing trends at other US sites needs further investigation.

Intense laser pulses have recently emerged as a tool to tune between different orders in complex quantum materials. Among different light-induced phenomena, transient superconductivity far above the equilibrium transition temperature in cuprates is particularly attractive. Key to those experiments was the resonant pumping of specific phonon modes, which was believed to induce superconducting phase coherence by suppressing the competing orders or modifying the structure slightly. Here, we present a comprehensive study of photoinduced nonequilibrium response in underdoped YBa_{2}Cu_{3}O_{6+x}. We find that upon photoexcitations, the Josephson plasma edge in the superconducting state is initially removed accompanied by quasiparticle excitations, and subsequently reappears at a frequency lower than the static plasma edge within a short time. In the normal state, an enhancement or weaker edgelike shape is indeed induced by pump pulses in the reflectance spectrum accompanied by simultaneous rises in both real and imaginary parts of conductivity. We compare the pump-induced effects between near- and midinfrared excitations and exclude phonon pumping as a scenario for the photoinduced effects above. We further elaborate that the transient responses in the normal state are unlikely to be explained by photoinduced superconductivity.