High harmonic generation from multiple orbitals in N2

Molecular electronic states energetically below the highest occupied molecular orbital (HOMO) should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N2 molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half-revival. This feature indicates the influence of electrons occupying the orbital just below the N2 HOMO, referred to as the HOMO-1. Such observations of lower-lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser-excited molecules.     

农业土壤N_2O产生途径及其影响因素研究进展

基于目前国内外对农业土壤N_2O产生与排放过程的研究成果,分析了N_2O的产生途径及其研究方法、影响农业N_2O产生的主要因素。农业土壤N_2O产生的主要过程有硝化作用(自养硝化作用和异养硝化作用)、反硝化作用和硝化微生物反硝化作用。目前研究硝化和反硝化作用的研究方法主要包括15N示踪法和气体抑制剂抑制法;影响土壤硝化—反硝化作用及N_2O产生的因素主要包括土壤基质、土壤物理性质、土壤化学性质、生物因素以及人类活动等。在此基础上探讨了目前研究中存在的主要问题,并对今后研究提出展望与建议。     

Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy

Conical intersections play a crucial role in the chemistry of most polyatomic molecules, ranging from the simplest bimolecular reactions to the photostability of DNA. The real-time study of the associated electronic dynamics poses a major challenge to the latest techniques of ultrafast measurement. We show that high-harmonic spectroscopy reveals oscillations in the electronic character that occur in nitrogen dioxide when a photoexcited wave packet crosses a conical intersection. At longer delays, we observe the onset of statistical dissociation dynamics. The present results demonstrate that high-harmonic spectroscopy could become a powerful tool to highlight electronic dynamics occurring along nonadiabatic chemical reaction pathways.     

Structural basis of biological N2O generation by bacterial nitric oxide reductase

Nitric oxide reductase (NOR) is an iron-containing enzyme that catalyzes the reduction of nitric oxide (NO) to generate a major greenhouse gas, nitrous oxide (N(2)O). Here, we report the crystal structure of NOR from Pseudomonas aeruginosa at 2.7 angstrom resolution. The structure reveals details of the catalytic binuclear center. The non-heme iron (Fe(B)) is coordinated by three His and one Glu ligands, but a His-Tyr covalent linkage common in cytochrome oxidases (COX) is absent. This structural characteristic is crucial for NOR reaction. Although the overall structure of NOR is closely related to COX, neither the D- nor K-proton pathway, which connect the COX active center to the intracellular space, was observed. Protons required for the NOR reaction are probably provided from the extracellular side.     

Observation of a train of attosecond pulses from high harmonic generation

In principle, the temporal beating of superposed high harmonics obtained by focusing a femtosecond laser pulse in a gas jet can produce a train of very short intensity spikes, depending on the relative phases of the harmonics. We present a method to measure such phases through two-photon, two-color photoionization. We found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain. Harmonic generation may be a promising source for attosecond time-resolved measurements.     

水稻CH4和N2O的排放及其与植株特性的相关性

为比较不同水稻品种间甲烷和氧化亚氮排放的差异,采用圆柱体静止箱取样、气相色谱分析,测定了不同早、晚稻品种在不同生育期甲烷和氧化亚氮的排放通量,考察其与水稻植株特性的相关性.结果表明,早稻甲烷、氧化亚氮排放通量分别在抽穗期、孕穗期出现峰值;晚稻甲烷、氧化亚氮排放通最分别在拔节期、乳熟期出现峰值.不同水稻品种间甲烷和氧化亚...     

根际反硝化作用与N2O释放

对根际反硝化作用及N2O的释放进行了综述。反硝化过程与N2O的产生及释放有密切的关系。反硝化作用产生的N2O量不仅取决于反硝化速率，而且也取决于那些影响反硝化产物N2O／N2比值的参数。在植物根际这一特殊土壤区域中，反硝化作用受NO3^-,C及O2的综合影响，豆科作物根瘤是一个特殊的根际系统，根瘤菌的反硝化作用及N2O释放应引起更大的关注。植物根际不仅对反硝化作用产生影响，而且对N2O释放也起了重要的通道作用，特别是对渍水土壤有重要的意义。文章最后指出了一些尚需深入研究的问题。     

Structural dynamics of a catalytic monolayer probed by ultrafast 2D IR vibrational echoes

Ultrafast two-dimensional infrared (2D IR) vibrational echo spectroscopy has proven broadly useful for studying molecular dynamics in solutions. Here, we extend the technique to probing the interfacial dynamics and structure of a silica surface-tethered transition metal carbonyl complex--tricarbonyl (1,10-phenanthroline)rhenium chloride--of interest as a photoreduction catalyst. We interpret the data using a theoretical framework devised to separate the roles of structural evolution and excitation transfer in inducing spectral diffusion. The structural dynamics, as reported on by a carbonyl stretch vibration of the surface-bound complex, have a characteristic time of ~150 picoseconds in the absence of solvent, decrease in duration by a factor of three upon addition of chloroform, and decrease another order of magnitude for the bulk solution. Conversely, solvent-complex interactions increase the lifetime of the probed vibration by 160% when solvent is applied to the monolayer.     

Effect of Biogas Digested Liquid on OH4 and N2O Flux in Paddy Ecosystem

Biogas production generates digested slurry as a byproduct. It can be used as a fertilizer especially after its conversion into digested liquid. A pot based study was conducted in order to evaluate the effect of the application of digested liquid on CH4 and N2O flux, and plant biomass in paddy. Analysis revealed that digested liquid treated soils released more CH4 compared to ammonium sulphate and the control. Ammonium sulphate treated soil emitted the highest N20 whereas digested liquid application decreased its emission significantly. Further, the cumulative emission over 101 d of the experiment was found to be higher for CHa （16.9 to 29.9 g m^-2） compared to N20 （-49.3 to 18.9 mg m^-2） for all treatments. Digested liquid application had positive impact on plant variables such as panicle number and weight of panicles. This study suggests that digested liquid application significantly decrease N20 emission and increase CH4 emission possibly due to affecting the availability of organic C in the soil to microbial activity for methanogenesis. Another possibility for enhancing CH4 emission by following biogas digested liquid could be attributed to the increase in plant biomass.     

Effect of Biogas Digested Liquid on CH4 and N2O Flux in Paddy Ecosystem

Biogas production generates digested slurry as a byproduct. It can be used as a fertilizer especially after its conversion into digested liquid. A pot based study was conducted in order to evaluate the effect of the application of digested liquid on CH₄ and N₂O flux, and plant biomass in paddy. Analysis revealed that digested liquid treated soils released more CH₄ compared to ammonium sulphate and the control. Ammonium sulphate treated soil emitted the highest N₂O whereas digested liquid application decreased its emission significantly. Further, the cumulative emission over 101 d of the experiment was found to be higher for CH₄ (16.9 to 29.9 g m⁻²) compared to N₂O (−49.3 to 18.9 mg m⁻²) for all treatments. Digested liquid application had positive impact on plant variables such as panicle number and weight of panicles. This study suggests that digested liquid application significantly decrease N₂O emission and increase CH₄ emission possibly due to affecting the availability of organic C in the soil to microbial activity for methanogenesis. Another possibility for enhancing CH₄ emission by following biogas digested liquid could be attributed to the increase in plant biomass.     

华北平原不同作物－潮土系统中N2O 排放量的测定

在中国科学院封丘农业生态试验站应用原状土柱培养法测定了华北平原主要农作物－潮土系统中N     

超声辅助磁性纳米四氧化三铁催化过氧化氢降解亚甲蓝染料的研

建立了一种基于超声辅助磁性四氧化三铁纳米微粒催化过氧化氢降解亚甲蓝染料的方法,研究了四氧化三铁纳米微粒浓度、过氧化氢浓度、pH值、反应时间、超声时间和温度等对催化降解反应的影响.结果表明,当四氧化三铁纳米粒子浓度为600mg/L,过氧化氢浓度为0.32mol/L,pH值为5,超声时间为3min,温度为30℃,反应时间为2h时,模拟染料废水中亚甲蓝的去除率最高可达到95%.     

间歇灌溉模式下稻田CH4和N2O排放及温室效应评估

 【目的】研究间歇灌溉和长期淹灌模式下稻田CH4和N2O排放规律及其温室效应,为全面评价不同水分管理对稻田生态环境带来的影响及有效控制稻田温室效应提供理论依据。【方法】采用静态箱技术对稻田CH4和N2O排放通量进行监测,并运用增温潜势对稻田生态系统CH4和N2O排放的温室效应进行了估算。【结果】间歇灌溉稻田CH4排放峰值主要集中在水稻分蘖前期和中期,N2O排放峰值出现在水稻分蘖前期和成熟期。与长期淹灌相比,间歇灌溉稻田CH4排放通量明显降低,其累积排放量为20.04 g?m-2,比长期淹灌处理37.27 g?m-2减少了46.23%;而N2O累积排放量显著高于长期淹灌稻田,其排放量为127.42 mg?m-2,比长期淹灌处理增加51.36 mg?m-2。间歇灌溉稻田CH4和N2O温室效应总和为4651.70 kgCO2?ha-1,比长期淹灌处理减少3418.35 kgCO2?ha-1。【结论】间歇灌溉能有效地抑制温室气体排放并显著降低CH4和N2O的温室效应。因此,间歇灌溉是减少温室气体排放和减轻全球变暖的有效措施之一。     

巢湖流域河流沉积物N2O释放对水体溶存N2O贡献研究

2010年11月在巢湖支流丰乐河与杭埠河采用现场培养和实测方法研究了沉积物N2O释放对水体（水柱）溶存N2O的影响,并采用NO-3削减法估算了沉积物的反硝化速率。研究结果表明,丰乐河与杭埠河N2O平均溶存浓度分别为0.26±0.10（SD）μg N-N2O·L-1和0.18±0.04（SD）μg N-N2O·L-1,饱和度分别为186%和151%,表明两条河流为大气N2O的潜在释放源。丰乐河与杭埠河沉积物-水界面N2O平均释放通量分别为0.39±0.44、0.15±0.16 μg N-N2O·m-2·h-1,由此可分别贡献水体中约89% 和45%的溶存N2O。对河流沉积物的反硝化速率估算结果表明,丰乐河与杭埠河沉积物反硝化速率分别为0.12±0.07、0.10±0.05 mg N·m-2·h-1,与已有的沉积物反硝化速率报道相比较低。     

稻田CO2、CH4和N2O排放通量测定方法研究

介绍了经过改装并配有火焰离子检测器（FID）和电子捕获检测器（ECD），能同步分析稻田CO2、CH4和N2O排放通量的气相色谱仪Aglient4890D的基本原理、主要配置及性能。该仪器与GC-14A气相色谱仪的分析结果十分接近。对2001年南京市江宁区稻田CO2、CH4和N2O的季节排放通量的实测结果表明，该仪器具有简便易行，准确可靠等优点，能够满足农田生态系统几种温室气体同步分析的要求。     

施肥量对福州平原稻田CH_4和N_2O通量的影响

为阐明施肥量对福州平原稻田CH_4和N_2O排放的影响,以不施肥处理为对照(CK),采用静态箱—气相色谱法,分析了常规施肥和倍增施肥稻田CH_4和N_2O通量及其影响因子。结果表明,CK、常规施肥和倍增施肥处理下稻田CH_4累积排放量依次为7.67、9.23和10.69 g·m~(-2),平均通量依次为3.47、4.18和4.84 mg·m~(-2)·h~(-1),倍增施肥显著促进稻田CH_4排放(P0.05);稻田N_2O排放量依次为-0.03、-0.05和-0.06 mg·m~(-2),平均通量依次为-13.99、-22.77和-28.10μg·m~(-2)·h~(-1),施肥量对N_2O排放的影响不显著(P0.05)。电导率与稻田CH_4通量呈极显著正相关(P0.01);常规施肥电导率与稻田N_2O通量呈显著负相关(P0.05)。土壤p H、Eh、温度和含水率等环境因子与不同施肥处理下稻田CH_4和N_2O排放量相关性存在差异。CK、常规施肥和倍增施肥观测期内所产生的综合增温潜势分别为2 515.03、2 989.07和3 450.45 kg·hm~(-2),倍增施肥处理显著提高稻田温室气体综合增温潜势。     

二元CoFe2O4-p-MgFe2O4磁性液体的制备及磁化特性研究

采用化学共沉淀法制备了CoFe2O4强磁性纳米微粒和p-MgFe2O4(Mg(OH)2与Fe(OH)3的混合物)弱磁性纳米微粒.并按体积比为1:1将CoFe2O4磁性液体、p-MgFe2O4顺磁磁性液体混合,得到二元CoFe2O4-p-Mg-Fe2O4磁性液体.实验结果表明混合磁性液体的磁化强度不能简单等于两种单一磁性液体磁化强度的叠加.在CoFe2O4磁性液体中,其磁性微粒在无场时会自发组装形成对磁化强度无贡献的闭合环状团聚体结构.二元磁性液体磁化时,这种CoFe2O4微粒环可能部分破裂.根据偶极子相互作用能判断CoFe2O4体系与p-MgFe2O4体系无相互作用,因此可根据单元磁性液体的磁化性质为基础来分析二元磁性液体的磁化性质.

Abstract：

Strong magnetic CoFe2O4 nanoparticles and weak magnetic p-MgFe2O4 (mixture of hydroxide Mg(OH)2 and Fe(OH)3) nanoparticles are produced by the chemical co-precipitation technology. Binary ferrofluids of CoFe2O4-p-MgFe2O4 are obtained by mixing CoFe2O4 ferrofluids and p-MgFe2O4 paramagnetic fluids in a ratio of 1: 1 (v/v). The experimental results indicate that the magnetization of the binary ferrofluid is not simple summation of the two single magnetic fluids. Without external magnetic field,some particles can self-assemble into aggregates of closed ring-like structures, which make no contribution to the magnetization for the CoFe2O4 ferofluid. In the magnetization process of the binary ferrofluid, the closed ring-like structure can partially break. Based on the interaction between two dipoles, it can be judged that there is no magnetic interaction between the CoFe2O4 magnetic system and the p-MgFe2O4 magnetic system. Therefore, the magnetization behavior of the binary ferrofluids can be analyzed based on the single magnetic fluids.     

Morse势阱中三次谐波产生的研究

利用量子力学中的密度矩阵算符理论,推导在具有多频率的复光场作用下线性和非线性极化率的一般表达式,然后利用图形技术,即利用费曼(Feynman)图方法来考虑三阶非线性过程,得到三次谐波系数的解析表达式.并以典型的GaAs/AlGaAs Morse势阱为例引入参数进行数值计算.结果表明,在该系统中得到了比体材料大的三次谐波系数,并适当增大势阱参数a可以获得较大的三次谐波系数;三次谐波系数随着弛豫常数hГ减小而增大.     

冬水田休闲期温室气体排放通量的研究

冬水田生态系统在西南地区大面积存在,长期淹水,其温室气体排放可能对中国温室效应有重要贡献。采用静态箱-气相色谱法对川中丘陵地区冬水田休闲期温室气体排放通量进行了原位观测研究,获得冬水田休闲期CH4、CO2、N2O的平均排放通量依次为5.37mg·m-·2h-1、81.88mg·m-·2h-1、0.01μg·m-·2h-1。同时研究发现,冬水田休闲期温室气体排放通量具有明显的动态变化,土壤温度和水分在很大程度上影响着3种温室气体的排放通量。研究还表明,改冬水田为水旱轮作可减少甲烷排放。     

Advances in Nitrogen Denitrification and N2O Emission in Agro-ecosystem

Nitrification and denitrification are two key links of nitrogen flow cycle in soil.N2O and N2,generated from biochemical process of nitrogen,can cause not only the nitrogen losses and reduction of nitrogen use efficiency,but also the boosted concentration of greenhouse gases,severely endangering the environment.Accordingly,nitrification-denitrification has been more and more concerned from whether an agricultural view,or an environmental one.Referring to the related literatures published at home and abroad in recent years,we overviewed the denitrification-caused N loss and N2O emission in various agro-ecosystems,and based on which we put forward countermeasures to reduce the denitrification-caused N loss and N2O emission and its research prospects in the future.