Krylov subspace methods for computing hydrodynamic interactions in Brownian dynamics simulations

Hydrodynamic interactions play an important role in the dynamics of macromolecules. The most common way to take into account hydrodynamic effects in molecular simulations is in the context of a Brownian dynamics simulation. However, the calculation of correlated Brownian noise vectors in these simulations is computationally very demanding and alternative methods are desirable. This paper studies methods based on Krylov subspaces for computing Brownian noise vectors. These methods are related to Chebyshev polynomial approximations, but do not require eigenvalue estimates. We show that only low accuracy is required in the Brownian noise vectors to accurately compute values of dynamic and static properties of polymer and monodisperse suspension models. With this level of accuracy, the computational time of Krylov subspace methods scales very nearly as O(N(2)) for the number of particles N up to 10 000, which was the limit tested. The performance of the Krylov subspace methods, especially the "block" version, is slightly better than that of the Chebyshev method, even without taking into account the additional cost of eigenvalue estimates required by the latter. Furthermore, at N = 10 000, the Krylov subspace method is 13 times faster than the exact Cholesky method. Thus, Krylov subspace methods are recommended for performing large-scale Brownian dynamics simulations with hydrodynamic interactions.     

Performance of a biomimetic oxidation catalyst immobilized on silicon wafers: comparison with its gold congener

With the aim of extending the usefulness of an existing biomimetic catalytic system, cobalt porphyrin catalytic units with thiol linkers were heterogenized via chemical grafting to silicon wafers and utilized for the catalytic oxidation of hydroquinone to p-benzoquinone. Atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS) were used to analyze the morphology and composition of the heterogeneous catalyst. The results of the catalytic oxidation of hydroquinone obtained with porphyrins grafted on silicon were compared with those obtained earlier with the same catalyst in homogeneous phase and immobilized on gold. It was found that the catalysis could run over 400 h, without showing any sign of deactivation. The measured catalytic activity is at least 10 times higher than that measured under homogeneous conditions, but also 10 times lower than that observed with the catalytic unit immobilized on gold. The reasons of this discrepancy are discussed in term of substrate influence and overlayer organization. The silicon-immobilized catalyst has potential as an advanced functional material with applications in oxidative heterogeneous catalysis of organic reactions, as it combines long-term relatively high activity with low cost.     

Design and operation of microelectrochemical gates and integrated circuits

Here we report a simple design philosophy, based on the principles of bipolar electrochemistry, for the operation of microelectrochemical integrated circuits. The inputs for these systems are simple voltage sources, but because they do not require much power they could be activated by chemical or biological reactions. Device output is an optical signal arising from electrogenerated chemiluminescence. Individual microelectrochemical logic gates are described first, and then multiple logic circuits are integrated into a single microfluidic channel to yield an integrated circuit that can perform parallel logic functions. AND, OR, NOR, and NAND gates are described. Eventually, systems such as those described here could provide on-chip data processing functions for lab-on-a-chip devices.     

Subfrequency noise signal extraction in fiber-optic strain sensors using postprocessing

Laser frequency fluctuations typically limit the performance of high-resolution interferometric fiber strain sensors. Using time delay interferometry, we demonstrate a frequency noise immune fiber sensing system, where strain signals were extracted well below the noise floor normally imposed by the frequency fluctuations of the laser. Initial measurements show a reduction in the noise floor by a factor of 30, with strain sensitivities of a nanostrain/Hz at 100 mHz and reaching 100 ps/Hz at 1 Hz. Further characterization of the system indicates the potential for at least 4.5 orders of magnitude frequency fluctuation rejection.     

Syntheses, spectroscopies and structures of molybdenum(VI) complexes with homocitrate

Initial investigations into the possible role of homocitric acid in iron molybdenum cofactor (FeMo-co) of nitrogenase lead us to isolate and characterize two tetrameric molybdate(VI) species. The complexes K2(NH4)2[(MoO2)4O3(R,S-Hhomocit)2].6H2O (1) and K5[(MoO2)4O3(R,S-Hhomocit)2]Cl.5H2O (2) (homocitric acid = H4homocit, C7H10O7) are prepared from the reactions of acyclic homocitric acid and molybdates, which represent the first synthetic structural examples of molybdenum homocitrate complexes. The homocitrate ligand trapped by tetranuclear molybdate coordinates to the molybdenum(VI) atom through alpha-alkoxy and alpha-, beta-carboxy groups. The physical properties, structural parameters, and their possible biological relevances are discussed.     

Near-surface structural phase transition of SrTiO3 studied with zero-field beta-detected nuclear spin relaxation and resonance

We demonstrate that zero-field beta-detected nuclear quadrupole resonance and spin relaxation of low energy (8)Li can be used as a sensitive local probe of structural phase transitions near a surface. We find that the transition near the surface of a SrTiO(3) single crystal occurs at T(c) approximately 150K, i.e., approximately 45K higher than T(c)bulk, and that the tetragonal domains formed below T(c) are randomly oriented.     

低温GaAs被动调Q锁模Nd:Gd0.42 Y0.58VO4 混晶激光器特性研究

采用低温生长GaAs晶体作为被动饱和吸收体兼输出镜,实现了Nd:Gd0.42Y0.58VO4混晶激光器的调Q锁模运转.研究了Nd:Gd0.42Y0.588VO4激光器的基频运转特性.在输出镜透射率T=10%、腔长L=40 mm的情况下,当抽运功率为8.6 W时,获得激光输出功率3.78 W,光-光转换效率为43.9%.并测量了Nd:Gd0.42Y0.58VO4混晶被动调Q激光器的输出特性.实验结果表明激光器调Q运转阈值为2 W,当抽运功率为3.7 W时,激光器出现调Q锁模行为;当抽运功率为8.6 W时,激光器调Q锁模深度达70%以上,对应的脉冲包络重复频率为670 kHz,半峰全宽为180 ns,平均输出功率为1.35 W,光-光转换效率为15.7%.     

低温生长GaAs在Nd∶YVO_4激光器中调Q特性的研究

采用一种新型的被动调Q饱和吸收体,低温生长GaAs薄膜,实现了半导体抽运Nd∶YVO4激光器的调Q运转.研究了激光器的调Q特性,调Q抽运阈值为2W.在抽运功率9.2W时,获得的最短脉冲半峰全宽为15ns,最大单脉冲能量为4.84μJ,最高峰值功率为330W,最大平均输出功率为1.16W;脉冲重复频率在220kHz到360kHz之间.     

A versatile reagent to synthesize diverse ionic liquids ranging from small molecules and dendrimers to functionalized proteins

An ionic liquid "reagent" bearing a succinimidyl activated ester is reported that can be used to synthesize a variety of small molecule and macromolecular ionic liquids. In addition, the ionic liquid reagent was used to modify lysozyme, and the protein retained its structure and function after modification. This study describes a facile and reliable route to new ionic liquid compositions.     

Cyclometalated platinum(II) complexes as topoisomerase IIα poisons

A platinum(II)-based major groove binder [Pt(II)(C^N)(C≡NR)(2)](+) (HC^N = 2-phenylpyridine (phpy), R = 2-naphthyl) was identified as a potent human topoisomerase IIα poison. It stabilizes the covalent TopoIIα-DNA cleavage complex and induces cancer cell death with potency significantly higher than the widely clinically used TopoIIα poison Vp-16.