Advances in Chemical Physics, Vol.128 (Wiley 2004)

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Calame and A. Fan, S. Wang, J. Hong, G. Bazan, K. Plaxco and A. Xu, J. Liu, Z. He and S. Griffin, A. Singh, D. Senapati, P. Rhodes, K. Mitchell, B. Robinson, E. Yu and P.

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Miron et al. Damasco et al. Ying et al. Aidas et al. Computational Molecular Science , vol. Aldongarov et al. Rizzo and H. As a result, the local concentration of the peptide increases steadily within the confines of the shrinking domains. At the lowest temperatures, where the acyl-chain order parameter of the membrane has already drastically increased and the membrane achieves a liquid-ordered character, an efficient lipid sorting mechanism is no longer supported and aggregation of the peptide into small clusters prevails.

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In particular, the study shows the interesting ability of the peptide to induce formation of fluid microdomains at physiologically relevant cholesterol concentrations, and this effect very much depends on the concentration of fluid vs ordered lipid molecules. Single thio-substitutions at all of the phosphoryl oxygen positions and a double thio-substitution at the nonbridging positions were considered.

The reaction free energy profiles are compared with available experimental data, and the role of solvation on the barrier heights and reaction coordinate is discussed. These results provide an important step in the characterization of thio effects in reactions of biological phosphates that may aid in the interpretation of kinetic data and ultimately help to unravel the catalytic mechanisms of ribozymes.

The technique of time-dependent density functional theory TDDFT has very recently been applied to the calculation of both transparent spectral region optical rotations and electronic circular dichroism CD. Here, we report the concerted application of the new methodologies to the determination of the absolute configuration AC of [32] 1,4 barrelenophanedicarbonitrile, 1, the first optically active barrelenophane. Microcrystals of a hydrophobic cargo were stabilized by EAK16 II, a self-assembling oligopeptide, and suspended in aqueous solution.

Pyrene was used as a model hydrophobic compound. Egg phosphatidylcholine EPC vesicles were prepared to mimic a cell membrane. The excimer decay profiles were acquired. The amount of pyrene released into the EPC vesicles at a given time was quantified using a calibration curve. The concentration of pyrene released was determined as a function of time, and the concentration-versus-time profile was fitted with one exponential. The rate of pyrene release was found to depend on the peptide-to-pyrene molecular ratio.

Higher peptide-to-pyrene ratios lead to slower transfer of pyrene to the lipophilic environment. Scanning electron micrographs demonstrated that a thicker coating on the pyrene crystals results in a slower release. The data presented in this work demonstrate that the self-assembling EAK16 II can stabilize a hydrophobic cargo in aqueous solution and deliver it into a lipophilic environment, and that the rate of transfer can be adjusted by tuning the peptide-to-pyrene ratio.

A family of new uridine phosphocholine amphiphiles that were prepared using a convenient four-step synthetic route is described. In aqueous solution, the amphiphiles possessing saturated alkyl chains self-assemble into DNA-like helical fibers in the crystalline state below Tm and compact bilayers above the melting temperature Tm. The transition from bilayers to fibers is thermally reversible. A therapeutic agent such as DNA can be entrapped within the hydrogel structure. In addition to forming bilayer vesicles and hydrogels in aqueous solution, these nucleoside amphiphiles also form organogels in cyclohexane above Tm.

Scanning electron microscopy shows a continuous multilamellar phase in the organogels. A congener of the glycosylphosphatidylinositol GPI membrane anchor present on the cell surface of the malaria pathogen Plasmodium falciparum has been synthesized. This GPI is an example of a small number of such membrane anchors that carry a fatty acyl group at O-2 of the inositol.

Although the acyl group plays crucial roles in GPI biosynthesis, it rarely persits in mature molecules. The presence of bulky functionalities at three contiguous positions of the inositol moiety creates a very crowded environment that poses difficulties for carrying out selective chemical manipulations. Thus installations of the axial long-chain acyl group and neighboring phosphoglyceryl complex were fraught with obstacles.

The key solution to these obstacles in the successful synthesis of the malarial candidate and prototype structures involved stereoelectronically controlled opening of a cyclic ortho ester. The reaction proceeds in very good yields, the desired axial diastereomer being formed predominantly, even more so in the case of long-chain acyl derivatives. However, study of our synthetic intermediates and prototypes indicate that the O-2 acyl group is quite stable, and that such migration does not occur readily. The reaction of 4-substituted cyclohexenyl phenyl iodonium tetrafluoroborate with tetrabutylammonium acetate gives both the ipso and cine acetate-substitution products in aprotic solvents.

The isomeric 5-substituted iodonium salt also gives the same mixture of the isomeric acetate products.

Arieh Warshel

Cyclohexyne can also be generated in the presence of some other mild bases such as fluoride ion, alkoxides, and amines, though amines are less effective bases for the elimination. Bases are much less effective in methanol, and methoxide was the only base to efficiently afford the cyclohexyne intermediate. Nucleophiles react with the cyclohexyne to give regioisomeric products in the ratio dependent on the ring substituent.

Catalyst loading was successfully reduced to as little as 0. The high turnover frequency and high volumetric productivity of the present reaction are also noteworthy. Finally, the utility of the N-acylpyrrole unit for further transformations is demonstrated. In earlier calculations J. Photoinduced electron transfer from a variety of electron donors including alkylbenzenes to the singlet excited state of acridine and pyrene is accelerated significantly by the presence of scandium triflate [Sc OTf 3] in acetonitrile, whereas no photoinduced electron transfer from alkylbenzenes to the singlet excited state of acridine or pyrene takes place in the absence of Sc OTf 3.

The rate constants of the Sc OTf 3-promoted photoinduced electron-transfer reactions ket of acridine to afford the complex between acridine radical anion and Sc OTf 3 remain constant under the conditions such that all the acridine molecules form the complex with Sc OTf 3. In contrast to the case of acridine, the ket value of the Sc OTf 3-promoted photoinduced electron transfer of pyrene increases with an increase in concentration of Sc OTf 3 to exhibit first-order dependence on [Sc OTf 3] at low concentrations, changing to second-order dependence at high concentrations.

The first-order and second-order dependence of ket on [Sc OTf 3] is ascribed to the and complexes formation between pyrene radical anion and Sc OTf 3. The positive shifts of the one-electron redox potentials for the couple between the singlet excited state and the ground-state radical anion of acridine and pyrene in the presence of Sc OTf 3 as compared to those in the absence of Sc OTf 3 have been determined by adapting the free energy relationship for the photoinduced electron-transfer reactions. The Sc OTf 3-promoted photoinduced electron transfer from hexamethylbenzene to the singlet excited state of acridine or pyrene leads to efficient oxygenation of hexamethylbenzene to produce pentamethylbenzyl alcohol which is further oxygenated under prolonged photoirradiation of an O2-saturated acetonitrile solution of hexamethylbenzene in the presence of acridine or pyrene which acts as a photocatalyst together with Sc OTf 3.

The photocatalytic oxygenation mechanism has been proposed based on the studies on the quantum yields, the fluorescence quenching, and direct detection of the reaction intermediates by ESR and laser flash photolysis. Metal oxides and solids with weak acidic and basic properties, like silica, carbon, and organic polymers, do not react with C18H37SiH3.

Department of Chemistry

Increasing the temperature of the reaction or doping neutral surfaces with acids or bases greatly increases their activity in the reaction with RSiH3. The rhodium I -species-catalyzed cycloisomerization reaction of a wide spectrum of 1,6-enynes with an unusual intramolecular halogen shift was investigated. We have studied photoinduced charge separation in a bare, 3. The initial increase is attributed to the gradual filling of surface electron trapping sites.

The trap-free mobility of electrons within these 9 nm nanoparticles is estimated to be 0. The after-pulse decay of the photoconductivity showed a power law behavior over a time scale of nanoseconds to several hundreds of microseconds, which is attributed to multiple trapping and detrapping events at chemical or physical defects within the semiconductor matrix. In this study, a series of novel luminescent cyclometalated Ir III complexes has been synthesized and evaluated for use in unimolecular oxygen-sensing materials. These luminophore complexes were characterized by NMR, absorption, and emission spectroscopy, luminescence lifetime and quantum yield measurements, elemental analysis, and cyclic voltammetry.

These combined results suggest that while Ni II may serve as a competent replacement for Zn II in alkyl group transfer enzymes, turnover may be limited by slow product release from the Ni II center. The synthesis and structural, spectroscopic, and electrochemical properties of a series of trinuclear tridentate cyclometalated platinum II complexes tethered by bis diphenylphosphinomethyl phenylphosphine dpmp have been studied and compared with their mono- and binuclear homologues and a propeller-like congener.

The tendencies of the absorption and emission energies to red-shift from mono- to linearly tethered bi- and trinuclear Pt II species are evident. A light-emitting electrochemical cell using a trinuclear Pt II derivative as emitter has been demonstrated. Qualitative and, in the case of P99, quantitative agreement was achieved with experimental kinetics.

This is found to be in large part accomplished by the ability of P99 to covalently bind the ligand without concurrent elimination of hydrogen bonds to Tyr, which proves not to be the case with Tyr in R Surface native oxide was decomposed and assembled into protruded lines when the negatively biased AFM tip was scanned over surface areas.

The mechanism of decomposition was found to be governed by the Fowler-Nordheim emission current enhanced by the negatively biased AFM tip. Direct oxide growth on the SiC surface was achieved when the AFM tip was immobilized and longer bias duration applied. In particular, the aspect ratio of oxide grown on SiC was found to be several times higher than that on the Si surface. The dielectrical strength of AFM oxide against degradation and breakdown under electrical stressing was evaluated.

Films of polyions and octahedral layered manganese oxide OL-1 nanoparticles on carbon electrodes made by layer-by-layer alternate electrostatic adsorption were active for electrochemical catalysis of styrene epoxidation in solution in the presence of hydrogen peroxide and oxygen. Oxygen and hydrogen peroxide activate the OL-1 catalyst for the epoxidation.

The pathway for styrene epoxidation in the highest yields required oxygen, hydrogen peroxide, and a reducing voltage and may involve an activated oxygen species in the OL-1 matrix. Localized water molecules in the binding pockets of proteins play an important role in noncovalent association of proteins and small drug compounds.