Time propagation of electronic wavefunctions using nonorthogonal determinant expansions.

The use of truncated configuration interaction in real-time time-dependent simulations of electron dynamics provides a balance of computational cost and accuracy, while avoiding some of the failures associated with real-time time-dependent density functional theory. However, low-order truncated configuration interaction also has limitations, such as overestimation of polarizability in configuration interaction singles, even when perturbative doubles are included. Increasing the size of the determinant expansion may not be computationally feasible, and so, in this work, we investigate the use of nonorthogonality in the determinant expansion to establish the extent to which higher-order substitutions can be recovered, providing an improved description of electron dynamics. Model systems are investigated to quantify the extent to which different methods accurately reproduce the (hyper)polarizability, including the high-harmonic generation spectrum of H2, water, and butadiene.

Trace elements in red swamp crayfish (Procambarus clarkii) in China: Spatiotemporal variation and human health implications.

The enrichment and health risk assessment of trace elements in crayfish on a national scale are significant for food safety due to the rapidly expanding crayfish consumption in China. In the present study, 4709 samples were extracted from databases to explore the spatiotemporal variation characteristics of trace elements in crayfish. Due to the variance in the background value of trace elements, the level of trace elements varies by region. Additionally, levels of As and Cr in crayfish increased with the promotion of intensive rice-crayfish coculture in China. Health risk assessment results revealed that trace elements may cause non-carcinogenic risk for crayfish consumption for adults and children from the mid-lower reaches of the Yangtze River, and the main risk was from As and Hg. The cancer risk values of As for children and adults in Zhejiang, Anhui, Heilongjiang, Hubei, Hunan, Jiangsu, Jiangxi and Shandong provinces were above the allowable value. There is concern about the non-carcinogenic and carcinogenic risk of consuming crayfish containing trace elements in some areas in China. Therefore, the results can serve as a critical reference for policy purposes in China. In addition, it is recommended that further research and assessment on crayfish consumption are required.

A Multi-Medium Analysis of Human Health Risk of Toxic Elements in Rice-Crayfish System: A Case Study from Middle Reach of Yangtze River, China.

Rice-crayfish system has been extensively promoted in China in recent years. However, the presence of toxic elements in soil may threaten the quality of agricultural products. In this study, eight toxic elements were determined in multi-medium including soil, rice, and crayfish from the rice-crayfish system (RCS) and conventional rice culture (CRC) area. Crayfish obtained a low level of toxic element content, and mercury (Hg) in rice from RCS showed the highest bioavailability and mobility. Health risk assessment, coupled with Monte Carlo simulation, revealed that the dietary exposure to arsenic (As) and Hg from rice and crayfish consumption was the primary factor for non-carcinogenic risk, while Cd and As were the dominant contributors to the high carcinogenic risk of rice intake for adults and children, respectively. Based on the estimated probability distribution, the probabilities of the total cancer risk (TCR) of rice intake for children from RCS were lower than that from CRC.

A trace CH4 detection system based on DAS calibrated WMS technique.

We report the development of a compact near-infrared (NIR) laser-based trace methane (CH4) detection system. This detection system relied on a 2334 nm distributed feedback (DFB) fiber laser as the light source. A parallel dense light-spot pattern multipass gas cell (MGC) with 41.5 m effective absorption path length was utilized to improve the system sensitivity. A self-calibration approach based on direct absorption spectroscopy (DAS) calibrated wavelength modulation spectroscopy (WMS) technique was employed to solve the problem of extra concentration calibration requirement in traditional WMS technique, and to improve the accuracy and stability of the system. According to the Allan deviation analysis, 1-s measurement precision of 0.61 ppmv for DAS and 0.16 ppmv for WMS was obtained, which could be further reduced to 0.11 ppmv for DAS and 0.03 ppmv for WMS by averaging up to 80 s and 50 s, respectively. A week-long continuous atmospheric CH4 concentration measurement was also carried out to demonstrate the long-term performance of our CH4 detection system. With a fast dynamic response characteristics, high-accuracy and high-sensitivity, the proposed detection system is suitable for CH4 measurement in many fields such as atmospheric chemistry analyzation, industrial safety monitoring, agricultural information acquisition, etc.

Combining impregnation and co-pyrolysis to reduce the environmental risk of biochar derived from sewage sludge.

Sewage sludge derived biochar has great potential for agricultural application, whereas the risk of heavy metals in sewage sludge is a key challenge for utilization. This study investigated the synergetic effect of co-pyrolysis and ZnCl2 impregnation treatment on the surface characteristics and potential ecological risk of heavy metals in sewage sludge derived biochar. It was concluded that ZnCl2 impregnation led to an increase in biochar yield, O and S content, but decrease the ash content and pH. Additionally, the thermal stability of ZnCl2-added biochar was decreased. Semi-quantitive specific functional groups analysis suggested that ZnCl2 impregnation had a negative effect on the content of CO and C-O, while promoted the formation of aromatic CC. And the functional group of CO was retained in biochar by co-pyrolysis with Camellia oleifera shell due to its high content of potassium. For heavy metal passivation, ZnCl2 impregnation decreased total content of heavy metals by chlorination, while the oxidizable fraction (F3) of heavy metals showed an increasing tendency. Results of potential ecological risk assessment indicated that combining ZnCl2 impregnation and co-pyrolysis had great potential to reduce the ecological risk of heavy metals in sewage sludge derived biochar.

Global Elucidation of Self-Consistent Field Solution Space Using Basin Hopping.

Reliable global elucidation of (subsets of) self-consistent field solutions is required for continued development and application of computational approaches that utilize these solutions as reference wavefunctions. We report the derivation and implementation of a stochastic approach to perform global elucidation of self-consistent field solutions by exploiting the connection between global optimization and global elucidation problems. We discuss the design of the algorithm through combining basin-hopping search algorithms with a Lie algebraic approach to linearize self-consistent field solution space, while also allowing preservation of desired spin-symmetry properties of the wavefunction. The performance of the algorithm is demonstrated on minimal basis C2v H4 due to its use as a model system for global self-consistent field solution exploration algorithms. Subsequently, we show that the model is capable of successfully identifying low-lying self-consistent solutions of benzene and NO2 with polarized double-zeta and triple-zeta basis sets and examine the properties of these solutions.

Study on the Mechanical Properties of Bionic Protection and Self-Recovery Structures.

A novel protective structure, based on shrimp chela structure and the shape of odontodactylus scyllarus, has been shown to improve impact resistance and energy absorption. A finite element model of NiTi alloy with shape memory was constructed based on the basic principles of structural bionics. The protective structure utilizes NiTi alloy as the matrix, a material with many advantages including excellent compression energy absorption, reusability after unloading, and long life. The mechanical properties of the single-layer model were obtained by static crushing experiments and numerical simulations. Building upon the idea of the monolayer bionic structure design, a two-layer structure is also conceived. Both single-layer and double-layer structures have excellent compression energy absorption and self-recovery capabilities. Compared with the single-layer structure, the double-layer structure showed larger compression deformation and exhibited better energy absorption capacity. These results have important academic and practical significance for improving the impact resistance of protective armor. Our study makes it possible to repair automatic rebounds under the action of pressure load and improves the endurance and material utilization rate of other protective structures.

Input of Cd from agriculture phosphate fertilizer application in China during 2006-2016.

Phosphate fertilizer applications are an important source of soil Cd in China. However, the input of Cd from phosphate fertilizer has always been neglected in China because of its low content. In this paper, we calculated the Cd input from phosphate fertilizer in China during 2006-2016. According to the data, the total phosphate fertilizer consumption and agriculture application rate tended to decrease after 2014. In 2016, the phosphate fertilizer application rate ranged from 12.14 to 99.38 kg/ha with a mean value of 42.70 kg/ha, and excessive fertilizer application occurred in Xinjiang, Henan, and Hubei Provinces. The Cd content in phosphate fertilizer was 0.75 mg/kg based on 1222 samples. The national Cd input from phosphate fertilizer was estimated to be 10.52 tons in 2016, with DAP/MAP being the largest contributor, accounting for 83.31% of the total input. These findings demonstrate the necessity of performing assessments to regulate the utilization of phosphate fertilizer in China, especially in Henan and Xinjiang Provinces.

Assessing heavy metal pollution in paddy soil from coal mining area, Anhui, China.

Heavy metal pollution in agricultural soil has negative impact on crop quality and eventually on human health. A total of 24 top soil samples were collected from paddy field near the Zhangji Coal Mine in Huainan City, Anhui Province. Seven heavy metals (Cu, Zn, As, Cr, Cd, Pb, and Ni) were selected to evaluate the pollution status through total content and chemical speciation, geo-accumulation index (Igeo), and risk assessment code (RAC) and investigate leaching behavior of heavy metals under simulated rainfall. The results of present study indicated that mining activities were responsible for elevated Cu and Cd in surrounding paddy soil. Based on the results of chemical speciation, most heavy metals were associated with the residual fraction, and the environmental risk of heavy metals in soil was sequenced as Pb > Cd > Ni > As > Zn > Cu > Cr. It revealed that Pb in soil would pose a higher environmental risk due to its higher reducible fraction, then followed by Cd, Ni, As, and Zn, which would pose a medium risk. The result of simulated rainfall leaching analysis showed that heavy metals could be categorized into two groups: concentrations of Cu, Ni, Cd, Zn, and Cr in the leachates displayed a continuous decrease tendency with the increase in accumulative simulated rain volume; whereas leachable tendency of As and Pb was enhanced with increasing leaching time and rain volume. Generally, the leaching percentage of heavy metals followed the sequence of As > Zn > Ni > Cd > Cr > Cu > Pb. More attention should be paid to the higher environmental risk of Pb and higher leaching percentage of As with regard to ecosystem safety and human health.

Current status and environment impact of direct straw return in China's cropland - A review.

With the development of grain production technologies and improvement of rural living standard, the production and utilization of straw have significantly been changed in China. More than 1 billion tones of straw are produced per year, and vast amount of them are discarded without effective utilization, leading various environmental and social impacts. Straw return is an effective approach of the straw utilization that has been greatly recommended by government and scientists in China. This paper discussed the current status of the straw return in China. Specifically, the production and models of straw return were explored and their environmental impacts were extensively evaluated. It was concluded that straw could be positively effective on the improvement of the soil quality and the grain production. However, it appeared that the straw return also had several neglect negative effects, implying that further research and assessment on the returned straw are required before its large-scale promotion in China.