Sub-laser-cycle electron pulses for probing molecular dynamics

Experience shows that the ability to make measurements in any new time regime opens new areas of science. Currently, experimental probes for the attosecond time regime (10(-18) 10(-15) s) are being established. The leading approach is the generation of attosecond optical pulses by ionizing atoms with intense laser pulses. This nonlinear process leads to the production of high harmonics during collisions between electrons and the ionized atoms. The underlying mechanism implies control of energetic electrons with attosecond precision. We propose that the electrons themselves can be exploited for ultrafast measurements. We use a 'molecular clock', based on a vibrational wave packet in H(2)(+) to show that distinct bunches of electrons appear during electron ion collisions with high current densities, and durations of about 1 femtosecond (10(-15) s). Furthermore, we use the molecular clock to study the dynamics of non-sequential double ionization.     

改进分子动力学的车辆跟驰模型

为了更好地研究复杂情况下的车辆跟驰特性,将车辆跟驰行为类比为分子在一维管道中相互作用的结果.已有的基于分子动力学的车辆跟驰模型利用需求安全间距和车道限速作为因素建立分子跟驰模型,忽略了车辆相对速度对驾驶员跟驰行为的影响,不符合真实的跟驰情况.因此,将车辆相对速度纳入模型结构中,建立分子相互作用势函数和壁面势函数,并据此构建改进分子动力学的车辆跟驰模型.用高精度车载定位仪器对车辆跟驰过程中的参数进行采集,利用遗传算法对模型参数进行标定并对模型进行分析,分别验证模型在不同跟驰状态下的准确性,并与改进前的分子跟驰模型进行对比.结果表明,改进的分子跟驰模型可以更有效地预测车辆的跟驰行为.     

Cd/Ba/F/Cl 系玻璃结构的X射线衍射和分子动力学研究

采用Ｘ射线衍射和分子动力学（ＭＤ）计算模拟等手段研究了６７ＣｄＦ２／３３ＢａＣｌ２玻璃（Ⅰ）和４０ＣｄＦ２／４０ＢａＦ２／２０ＣｄＣｌ２玻璃（Ⅱ）的结构。研究表明，在Ⅰ中Ｃｄ原子主要为６配位，Ⅱ中Ｃｄ原子主要为６或７配位。Ｃｄ—Ｆ的平均键长分别为２３１．６ｐｍ和２３０．４ｐｍ。在ＭＤ计算的玻璃中同时存在非桥Ｆ，桥Ｆ，３配位Ｆ和４配位Ｆ，几乎不存在不和Ｃｄ原子成键的游离Ｆ。弱的形成体阳离子和阴离子的连接较弱，Ｃｄ在大的阴离子空隙中的位置较松弛，体系随Ｃｄ含量增加稳定性下降。对混合卤化物玻璃的结构与形成的特点进行了讨论。     

Complex zeolite structure solved by combining powder diffraction and electron microscopy

Many industrially important materials, ranging from ceramics to catalysts to pharmaceuticals, are polycrystalline and cannot be grown as single crystals. This means that non-conventional methods of structure analysis must be applied to obtain the structural information that is fundamental to the understanding of the properties of these materials. Electron microscopy might appear to be a natural approach, but only relatively simple structures have been solved by this route. Powder diffraction is another obvious option, but the overlap of reflections with similar diffraction angles causes an ambiguity in the relative intensities of those reflections. Various ways of overcoming or circumventing this problem have been developed, and several of these involve incorporating chemical information into the structure determination process. For complex zeolite structures, the FOCUS algorithm has proved to be effective. Because it operates in both real and reciprocal space, phase information obtained from high-resolution transmission electron microscopy images can be incorporated directly into this algorithm in a simple way. Here we show that by doing so, the complexity limit can be extended much further. The power of this approach has been demonstrated with the solution of the structure of the zeolite TNU-9 (|H9.3|[Al9.3Si182.7O384]; ref. 10) with 24 topologically distinct (Si,Al) atoms and 52 such O atoms. For comparison, ITQ-22 (ref. 11), the most complex zeolite known to date, has 16 topologically distinct (Si,Ge) atoms.     

六方单晶电子衍射花样的计算机标定

以工业纯钛为例，用 Ｄｅｌｐｈｉ语言对六方单晶选区电子衍射花样进行计算机标定，简化了标定 中繁复的计算工作．可视化结果表明标定程序的设计是正确可行的．     

Imaging in the era of molecular oncology

New technologies for imaging molecules, particularly optical technologies, are increasingly being used to understand the complexity, diversity and in vivo behaviour of cancers. 'Omic' approaches are providing comprehensive 'snapshots' of biological indicators, or biomarkers, of cancer, but imaging can take this information a step further, showing the activity of these markers in vivo and how their location changes over time. Advances in experimental and clinical imaging are likely to improve how cancer is understood at a systems level and, ultimately, should enable doctors not only to locate tumours but also to assess the activity of the biological processes within these tumours and to provide 'on the spot' treatment.     

分子动力学的格波理论

应用固体物理学和固体力学的理论,建立了分子动力学的格波理论.该理论将符合周期性几何结构的三维晶体看作代表性体元,研究三维晶体在有限温度下的本构响应.基于周期边界条件,建立三维晶格振动的特征方程,求得三维晶体固有频率,进而得到各个原子动力学方程的解析解.在此基础上求得有限温度下,三维晶体的热应力.该理论有效地克服了经典分子动力学在时间尺度和空间尺度上的困难.     

Probing molecular dynamics with attosecond resolution using correlated wave packet pairs

Spectroscopic measurements with increasingly higher time resolution are generally thought to require increasingly shorter laser pulses, as illustrated by the recent monitoring of the decay of core-excited krypton using attosecond photon pulses. However, an alternative approach to probing ultrafast dynamic processes might be provided by entanglement, which has improved the precision of quantum optical measurements. Here we use this approach to observe the motion of a D2+ vibrational wave packet formed during the multiphoton ionization of D2 over several femtoseconds with a precision of about 200 attoseconds and 0.05 ?ngstr?ms, by exploiting the correlation between the electronic and nuclear wave packets formed during the ionization event. An intense infrared laser field drives the electron wave packet, and electron recollision probes the nuclear motion. Our results show that laser pulse duration need not limit the time resolution of a spectroscopic measurement, provided the process studied involves the formation of correlated wave packets, one of which can be controlled; spatial resolution is likewise not limited to the focal spot size or laser wavelength.     

Optical nonlinearity and ultrafast dynamics of ion exchanged silver nanoparticles embedded in soda-lime silicate glass

Ag nanoparticles embedded in soda-lime silicate glass were fabricated by ion-exchange and subse-quently annealing method. Z-scan technique, femtosecond time-resolved optical Kerr effect （OKE） technique and femtosecond pump-probe experiment were used to investigate the effects of laser wavelength and laser pulse duration as well as annealing temperature on the third-order optical nonlinearity and ultrafast dynamics of the composites. It was found that the third-order susceptibility of Ag nanoparticles composite glass measured by 400 nm pulse source is larger than that measured by 800 nm pulse source due to an enhancement effect of local field near surface plasmon resonance of Ag nanoparticles in silicate glass. The third-order optical nonlinearity measured by ns laser source is about two orders of magnitude larger than that measured from fs pulse. The annealing temperature has an important effect on the third-order optical nonlinearity and ultrafast dynamics of the composites. Third-order nonlinear susceptibility up to 10^-l0 esu and fast relaxation process up to 0.2 ps have been obtained in Ag nanoparticles doped glass.     

Temperature-dependent X-ray diffraction as a probe of protein structural dynamics.

X-ray diffraction at four temperatures from 220 to 300 K coupled with crystallographic refinement yields the mean-square displacements and conformational potentials of all 1,261 non-hydrogen atoms of metmyoglobin. The results are interpreted to indicate a condensed core around the haem, semi-liquid regions towards the outside and a possible pathway for ligands. It is concluded that X-ray diffraction can provide the spatial distribution of the dynamic features of a protein.     

The effect of hydrogen-bond in alcoholic solvent on the solvation ultrafast dynamics of oxazine 750 dye

The ultrafast dynamics of oxazine 750 dye was studied in methanol, ethanol, 1-propanol, 1-butanol solvents using the femtosecond time-resolved stimulated emission pumping fluorescence depletion （FS TR SEP FD） technique. The faster decays on the hundreds of femtosecond time scale and the slower decays on the order of picosecond were found. The intramolecular vibrational redistribution （IVR） and the solute-solvent intermolecular photoinduced electron transfer （ET） should account for the faster decay, while the slower decay is attributable to the diffusive solvent relaxation. The results show that the intermolecular hydrogen-bonding network will hinder the rearrangement of the alcoholic molecules in the solvaUon process and the time constants of the slower diffusive solvent relaxation decays are found to increase with the hydrogen-bonding energy in alcoholic solvents.     

Parallel molecular dynamics on the connection machines

We have demonstrated using vectorized parallel Lennard-Jones fluid program that vectorizing general-purpose parallel molecular package for simulating biomolecules which currently runs on the Connection Machine CM-5 using CMMD message passing would offer a significant improvement over a non-vectorized version. Our results indicate that the Lennard-Jones fluid program written in C^*/CMMD is five times faster than the same program written in C/CMMD.     

Assembly dynamics of microtubules at molecular resolution

Microtubules are highly dynamic protein polymers that form a crucial part of the cytoskeleton in all eukaryotic cells. Although microtubules are known to self-assemble from tubulin dimers, information on the assembly dynamics of microtubules has been limited, both in vitro and in vivo, to measurements of average growth and shrinkage rates over several thousands of tubulin subunits. As a result there is a lack of information on the sequence of molecular events that leads to the growth and shrinkage of microtubule ends. Here we use optical tweezers to observe the assembly dynamics of individual microtubules at molecular resolution. We find that microtubules can increase their overall length almost instantaneously by amounts exceeding the size of individual dimers (8 nm). When the microtubule-associated protein XMAP215 (ref. 6) is added, this effect is markedly enhanced and fast increases in length of about 40-60 nm are observed. These observations suggest that small tubulin oligomers are able to add directly to growing microtubules and that XMAP215 speeds up microtubule growth by facilitating the addition of long oligomers. The achievement of molecular resolution on the microtubule assembly process opens the way to direct studies of the molecular mechanism by which the many recently discovered microtubule end-binding proteins regulate microtubule dynamics in living cells.     

超临界甲醇的分子动力学模拟

本文采用分子动力学（MD）方法对超临界甲醇体系结构性质和动力学性质进行了模拟研究．结果表明,在超临界条件下甲醇体系因密度涨落存在分子聚集现象,且在低密度区域更明显．与常温常压条件下相比甲醇分子间的氢键作用明显减弱,结构变得松散,分子极性大大降低,自扩散系数上升了十几甚至几百倍．随着压强的增大,甲醇分子间的氢键作用增强,扩散系数减小;随着温度的升高,甲醇分子间的氢键作用减弱,自扩散系数增大,且在接近临界压力时、自扩散系数随温度的变化幅度更大．     

低温回火马氏体取向关系的电子背散射衍射研究

为了研究马氏体的相变特征,利用电子背散射衍射(EBSD)技术并结合金相显微镜和显微硬度计分析低温回火的20MnCr5渗碳齿轮钢的性能和组织。根据马氏体相变理论中的K-S和N-W取向关系分别计算得到马氏体{110}α极射赤面投影图。利用EBSD技术对20MnCr5齿轮钢心部选定的区域进行扫描,分析区域中马氏体的取向分布特征。研究结果表明:马氏体取向整体呈随机分布,但在局部区域呈有规律分布。整个扫描区域的取向差主要分布在5°以下和45°以上。为反映马氏体局部区域取向分布的规律,选定一个原奥氏体晶粒,并做出区域中所有马氏体{110}α晶面的极射赤面投影图,得到极点有规律分布的极图。通过对{110}α极图分别使用K-S和N-W关系拟合,确定所选区域的马氏体的取向关系以N-W关系为主,实际极点离散分布在理论极点周围;使用协同形变机理解释实际取向分布与理论分布的偏差是由马氏体相变导致周围组织复杂的畸变引起。     

Design of a compact C-band high brightness photoinjector for an ultra-fast electron diffraction

A compact C-band high brightness photoinjector for ultra-fast electron diffraction （UED） is under development at Tsinghua Uni- versity. The C-band photoinjector, operating at 5.172 GHz, uses a 1.45-cell C-band RF gun as the electron source. The design of the RF gun has addressed the physics, beam dynamics and mechanical aspects, and based on these design studies, a prototype has been fabricated. In order to obtain optimized performance for the UED, beam dynamics simulation has been carried out using the particle tracking code Astra for the photoinjector consisting of an alternative multi-cell RF gun design and a C-band compressor downstream. The beam dynamics parameters that are optimized include the bunch length, peak current, horizontal emittance, and position of the minimum bunch length.     

Direct observation of electron dynamics in the attosecond domain

Dynamical processes are commonly investigated using laser pump-probe experiments, with a pump pulse exciting the system of interest and a second probe pulse tracking its temporal evolution as a function of the delay between the pulses. Because the time resolution attainable in such experiments depends on the temporal definition of the laser pulses, pulse compression to 200 attoseconds (1 as = 10(-18) s) is a promising recent development. These ultrafast pulses have been fully characterized, and used to directly measure light waves and electronic relaxation in free atoms. But attosecond pulses can only be realized in the extreme ultraviolet and X-ray regime; in contrast, the optical laser pulses typically used for experiments on complex systems last several femtoseconds (1 fs = 10(-15) s). Here we monitor the dynamics of ultrafast electron transfer--a process important in photo- and electrochemistry and used in solid-state solar cells, molecular electronics and single-electron devices--on attosecond timescales using core-hole spectroscopy. We push the method, which uses the lifetime of a core electron hole as an internal reference clock for following dynamic processes, into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell. This allows us to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as.