应用反射式飞行时间质谱仪研究氨团簇离子解离动力学

用直射式和反射式飞行时间质谱研究了氨分子团簇体系在３５５ｎｍ激光下的多光子电离,得到一系列的质子化团簇离子（ＮＨ３）ｎＨ＾＋,同时还观察到超价氨团簇离子（ＮＨ３）ｎＨ＾＋２。在反射式飞行时间质谱研究中观测到质子化氨团簇离子在自由飞行过程中的解离现象,表明在该实验条件下生成的质子化氨团簇离子是一些亚稳态团簇离子。对子离子产率的分析,得到质子化团簇离子解离速率常数,从而可以估计亚稳态团簇离子的寿命。团     

用于二元合金团簇负离子研究的光电子能谱仪

报道了自行研制的磁瓶式飞行时间光电子能谱仪 ,它安装在自制的反射式飞行时间质谱仪的一级聚焦点的接口部位 ,将用于二元合金团簇负离子几何和电子结构的研究 .仪器测试的能量分辨好于 0 .1eV ,达到了设计指标 .对PbM-(M =Cu ,Ag ,Au)二元合金团簇负离子进行了光电子能谱的实验 ,获得的绝热电子亲合势与密度泛函的计算结果符合的很好 ,由此表明 ,该光电子能谱仪将适用于二元合金团簇负离子体系的研究 .     

Modification of Reflectron Time-of-Flight Mass Spectrometer for Photodissociation of Mass-Selected Cluster Ions

介绍了一种改进的反射式飞行时间质谱装置用于光解质量选择的团簇离子. 该装置中采用了\选质-减速-解离-再加速"的方式. 团簇离子在反射式飞行时间的一级聚焦点被选质,接着被减速,并且立即被光解,光解所产生的碎片以及没有被光解的母体离子被重新加速,这一系列过程都在靠近一级聚焦点的位置完成. 相对文献中报道的其他方式,采用这一方式更利于光解碎片和母体离子的分离,更容易确定光解激光的触发时间,同时,由于母体离子在一级聚焦点的空间分布比较窄,也有利于光解激光束照射到所有的团簇离子,从而提高光解效率. 对母体离子、碎     

氨与甲醇混合团簇的多光子电离质谱及从头算研究

用多光子电离技术结合飞行时间质谱仪对氨与甲醇混合团簇进行了研究.在脉冲激光波长分别为266nm,355nm和532nm条件下,仅在355nm作用下观测到团簇离子.主要的电离产物为质子化的(CH3OH)n(NH3)mH (n=0~6,m=0~4)混合团簇离子,且各个序列的离子强度随m的增大而减小.经分析,氨与甲醇混合团簇电离后团簇离子发生内部质子化转移反应是形成质子化团簇离子的主要原因.不同尺寸团簇离子信号强度随电离激光光强变化的光强指数曲线显示,团簇均发生四光子电离过程.应用量化计算,构造了质量数较小的几个团簇离子的可能的空间几何构型,发现二元团簇离子(CH3OH)n(NH3)mH 是以NH4 作为内核离子,再通过氢键与其它分子组合而构成团簇离子.     

甲醇/水混合团簇的多光子电离质谱研究

利用多光子电离技术结合飞行时间质谱仪对甲醇/水混合团簇进行了研究.在脉冲激光波长为355 nm条件下观测到团簇离子.主要的电离产物为质子化的(CH3OH)n(H2O)H+(n=l-13)混合团簇离子与(CH3OH)nH+团簇离子,经分析(CH3OH)1o(H2O) H+和(CH3OH)3H+为幻数结构.甲醇水混合团簇电离后团簇离子发生内部质子化转移反应是形成质子化团簇离子的主要原因.不同尺寸团簇离子信号强度随电离激光光强变化的光强指数曲线显示,团簇均发生四光子电离过程.     

氨/乙醇混合团簇多光子电离质谱

用多光子电离技术结合飞行时间质谱仪对氨与乙醇混合团簇进行了研究。在脉冲激光波长分别为266,355nm和532nm条件下,仅在355nm作用下观测到团簇离子。主要的电离产物为质子化的（C2H5OH）n（NH3）mH＋（n=0—3,m=0—4）混合团簇离子,且各个序列的离子强度随m的增大而减小。经分析,氨与乙醇混合团簇电离后团簇离子发生内部质子化转移反应是形成质子化团簇离子的主要原因。不同尺寸团簇离子信号强度随电离激光光强变化的光强指数曲线显示,团簇均发生四光子电离过程。通过理论计算得到其中性和离子团簇的稳定结构,解离能,解离通道。并证实团簇发生电离解离时发生了团簇内质子转移反应。     

1-萘酚团簇的紫外光电离质谱研究

用飞行时间质谱仪和超声速脉冲分子束技术研究了紫外激光对1-萘酚(1HN)团簇的电离质谱.观测到(1HN)_n~+系列的团簇离子,且离子强度随团簇尺寸的增大而减小.电离激光的强度(在5μJ/pulse～100μJ/pulse范围内)对团簇离子强度的相对分布影响较小,说明软电离为产生团簇离子的主要过程,团簇离子的强度分布反映出电离前中性团簇的分布特征.增大电离区的进样气压可以产生更大尺寸的团簇离子,同时在(1HN)_n~+后面观测到新系列的团簇离子.这些新生离子与(H_2O)_m有关,考虑到1-萘酚团簇可以通过OH形成H键,推测该新生团簇离子通过团簇内的反应而产生.     

吡啶团簇的飞秒光电离和从头计算研究

用飞秒激光电离飞行时间质谱研究了吡啶分子团簇在 4 0 0nm波长下的多光子光电离 ,实验观测到一系列的质子化和非质子化团簇离子 .结果表明 ,质子转移也能发生在弱氢键结合的分子间 .通过分析离子峰宽和离子信号强度随气源压力的变化 ,得到质子化团簇离子来源于大团簇离子的碎裂 ,而非质子化团簇离子是中性团簇直接电离的结果 .从头计算结果表明 ,吡啶团簇是通过弱氢键C -H…N结合在一起的 ,并且团簇离子离解倾向于生成质子化产物     

甲醇－乙醚团簇的多光子电离和从头算

在355 nm波长下用激光电离飞行时间质谱装置研究了氢键团簇甲醇/乙醚混合团簇的多光子电离,飞行时间质谱仪观测到一系列质子化团簇,为了探讨质子化团簇的形成机理,在B3LYP/6-31 G(d,p)//B3LYP/6-311 G(d,p)基组水平上计算了CH30H-(C2H5)2O离子和中性团簇的稳定几何结构和解离通道和解离能,发现存在一个质子转移过程,解离产物主要为CH3O和[(C2H5)2O]H .     

飞行时间质谱峰值的漂移

飞行时间质谱仪(time-of-flight mass spectrometer, TOF-MS)在分子团簇的激光电离/解离动力学研究中广泛使用。文章报道了在用脉冲355 nm的YAG激光进行水/甲醇二元团簇的多光子电离研究中,发现在电离激光相对于脉冲分子束的不同延时下,即激光作用于脉冲束的不同位置,飞行时间质谱仪测得的离子的质谱峰值发生漂移。在激光作用于脉冲束的中段时,离子的信号最强,同时离子的峰值漂移达到最大。分析认为：这种峰值漂移不是因为新质量数谱峰的出现,而是离子在穿越质谱仪的离子引出区和加速区极板时发生部分离子吸附,引起极板间电压的起伏造成的。离子在电场起伏下的数值模拟与实验中观测到的离子峰值漂移规律一致。     

Experimental Study on Powder Flowability Using Vibration Shear Tube Method

The flowability of powders with different mass median diameters ranging from micrometers to nanometers was measured using the vibration shear tube method. In the measurement system used in this study, the powder was discharged through a narrow gap between a vibrating tube edge and a flat bottom surface, where each particle could experience high shear forces to overcome the adhesion and friction forces. The vibration amplitude was increased during the measurement, and the mass of particles discharged was measured at constant time intervals. From the relationship between the mass flow rate and the vibration acceleration, static and dynamic properties of the powders were evaluated using the critical vibration acceleration, characteristic mass flow rate, and gradient of mass flow rate. The correlation between the static and dynamic properties was studied in detail.     

Absorption kinetics of ozone in water with ultrasonic radiation

A mathematical model was proposed to depict classical unsteady state method that was used to determine volumetric mass transfer coefficient of ozone from gaseous phase to aqueous phase during sonolysis. The rate constant of ozone self-decomposition with ultrasonic radiation, which was one of the parameters in the model, was determined with separate experiments. The results showed that self-decomposition rate constants of ozone were enhanced by ultrasound. The self-decomposition rate constant of ozone is linearly dependent on ultrasonic power, but the increase of the decomposition rate could not enhance ozone mass transfer coefficient. The volumetric mass transfer coefficients of ozone were also enhanced by ultrasonic radiation, while ultrasonic power had little effect on volumetric mass transfer coefficient of ozone. The degassing effect of ozone due to ultrasonic radiation was insignificant in the sparged system when ozone was bubbled during sonolysis.     

基于离散伴随方法的透平叶栅气动优化设计

本文研究并给出了基于离散伴随理论和自动微分技术构建离散伴随系统的方法、伴随系统的求解策略以及基于离散伴随方法的透平叶栅气动优化设计流程,建立了相应的优化设计系统。利用该优化系统在无黏环境下,以叶栅通道进出口的熵增率为目标函数、以叶栅通道内的质量流量为约束,对某二维跨音速透平叶栅进行了气动优化设计。与优化前相比,优化后透平叶栅进出口熵增率减少8.82%,质量流量变化幅度小于0.003%。优化结果表明,本文提出的优化系统能够有效改善透平叶栅的气动优化性能,验证了本文提出的基于离散伴随方法的透平叶栅气动优化设计方法的正确性与有效性。     

Further experimental study of fast fission with the Cl + Au system

The onset of fast fission was investigated with the Cl + Au system. The mass distribution of the fragments and the fusion cross sections were determined at six different bombarding energies. It turns out that the width of the symmetric component of the mass distribution increases strongly with the critical angular momentum. This could be related with the disappearance of the fission barrier due to centrifugal effects. A semi-static model is developed and the results are compared with the experimental data. In this framework, the observed broadening of the mass distribution can be attributed to the presence of the fast fission phenomenon.     

分级再生式转轮除湿空调系统的性能分析

提出了分级再生式转轮除湿和蒸发冷却相结合的空调系统,依据除湿和再生过程的质量守恒和能量守恒方程,结合边界条件和初始条件建立除湿转轮和空调系统的数学模型,对比分析了分级再生空调系统的性能。研究结果表明:采用分级再生的转轮可达到与一般再生转轮相同的除湿效果。与一般再生的空调系统相比,分级再生式空调系统的再生能耗降低了约50%,热力性能系数提高了约90%。     

Added mass matrix estimation of beams partially immersed in water using measured dynamic responses

An added mass matrix estimation method for beams partially immersed in water is proposed that employs dynamic responses, which are measured when the structure is in water and in air. Discrepancies such as mass and stiffness matrices between the finite element model (FEM) and real structure could be separated from the added mass of water by a series of correction factors, which means that the mass and stiffness of the FEM and the added mass of water could be estimated simultaneously. Compared with traditional methods, the estimated added mass correction factors of our approach will not be limited to be constant when FEM or the environment of the structure changed, meaning that the proposed method could reflect the influence of changes such as water depth, current, and so on. The greatest improvement is that the proposed method could estimate added mass of water without involving any water-related assumptions because all water influences are reflected in measured dynamic responses of the structure in water. A five degrees-of-freedom (dofs) mass-spring system is used to study the performance of the proposed scheme. The numerical results indicate that mass, stiffness, and added mass correction factors could be estimated accurately when noise-free measurements are used. Even when the first two modes are measured under the 5 percent corruption level, the added mass could be estimated properly. A steel cantilever beam with a rectangular section in a water tank at Ocean University of China was also employed to study the added mass influence on modal parameter identification and to investigate the performance of the proposed method. The experimental results demonstrated that the first two modal frequencies and mode shapes of the updated model match well with the measured values by combining the estimated added mass in the initial FEM.     

n+233U裂变碎片质量分布的唯象模型研究

本模型基于裂变多通道无规颈断裂模型,考虑宏观液滴能、壳效应能以及壳效应与温度的关系,得到参数化的势能表示形式。通过拟合不同测量方法得到的实验数据(经过评价) 获得3 组模型参数。3 组参数计算的碎片质量分布均很好地再现了不同能点的实验数据,除了基于动能法实验数据得到的参数外,其14 MeV的计算结果与实验数据符合较差。研究发现,不同入射中子能量的裂变碎片质量分布有4 个主要交叉点,在叉点之上的产额随入射中子能量增加减少,之下的产额则随入射中子能量上升;内侧(或外侧) 的两个交叉点质量数之和近似等于裂变复合核的质量数;不同裂变系统的重峰左侧的交叉点都保持在132 附近。Present model was based upon Brosa model, where macro energy,shell effect energy and its decreasing with system temperature were considered and parameterized. 3 sets of model parameters were obtained by fitting to 3 groups of evaluated experimental data, respectively, where the groups were classified by measured method: radiochemistry (RA) method, double kinetic energy (KE) method, and both (ALL). All the 3 sets of parameters could well reproduce themeasured mass distributions on different energies, except the KE set on 14 MeV. The result shows the mass distributions mainly had 4 trend turning points, above which the yield decreasing and below which the yield increasing with energy.The sum of the 1st and 4th (or 2nd and 3rd) point positions was equal to the compound nuclei mass approximately. And the 3rd point was kept at ~132 constantly for different fission systems n+233 U, n+235U, n+233Pu.     

近场光学用于激光解吸飞行时间质谱的亚微米级空间分辨成像

基于激光离子源的飞行时间质谱法作为一门新兴的成像方法,已经被广泛应用于材料、地质、环境、药物和生命科学领域中。但受限于光学衍射极限、聚焦透镜的焦距和数值孔径等因素,使其难以实现亚微米尺寸的高空间分辨率成像。近场技术的引入成功地解决了光学衍射极限的限制,将近场技术与激光电离技术相结合,可以实现对固体样品表面纳米级弹坑的剥蚀。此外,传统的质谱成像技术常常假设样品表面是平整的,忽略其表面形貌的高低起伏,但这往往会导致信号强度不稳定和成像假象。为此,不仅需要获得样品中的化学组成与空间分布,还需同时获得样品表面的形貌信息,才能实现多功能的原位表征。在自行研制的激光解吸/电离飞行时间质谱的基础上,采用近场纳米有孔针尖离子源代替传统的远场激光聚焦,以532 nm波长激光为第一束解析激光,355 nm波长激光为后电离激光,音叉式原子力显微镜控制系统针尖与样品之间的距离维持在近场范围内,对酞菁铜镀层样品表面进行了弹坑剥蚀实验,获得了直径为550～850 nm的弹坑点阵;并对7.5 μm×7.5 μm的标准酞菁铜网格样品进行了铜离子亚微米级的高分辨率成像;此外,纳米有孔针尖离子源作为原子力显微镜的一种变体,还可同时获得成像区域的表面形貌信息,这一结合优势大大拓展了质谱技术在微纳尺度下的原位表征能力。     

麦秆添加大量CaO热解的TG-FTIR实验研究

利用热重-傅里叶变换红外光谱联用方法研究添加CaO对麦秆热解过程和挥发份析出特性的影响.热重和红外光谱分析均表明添加CaO后麦秆热解旱现两个明显的失重和挥发份析出阶段,而纯麦秆热解则只有一个.CaO在第一阶段不但能够吸收CO2,而且能够降低甲苯、苯酚和蚁酸等焦油类物质的产生,使得该阶段失重率和最大失重速率随CaO添加量增加而减小.CaCO3的煅烧分解是添加CaO麦秆热解第二阶段产生的原因,该阶段失重率和最大失重速率随CaO添加量增加而增大.研究结果表明,在采用生物质为原料的零排放系统中添加CaO有利于捕获CO2和减少焦油物质的产生,系统的气化温度应适当降低以防止CaCO3的煅烧分解.     

Frequency-dependent C(V) spectroscopy of the hole system in InAs quantum dots

The hole system in InAs quantum dots was investigated by frequency-dependent capacitance–voltage spectroscopy. Up to eight distinct charging peaks could be observed and the energy difference between the individual peaks could be estimated. All charging peaks decrease with increasing measurement frequency; however, the lower the energy of the hole level the stronger the decrease. A comparison with the results of the electron system in similar quantum dots yields that for all hole levels the effective mass in the barrier is much larger than in the electron system.