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1.
A nonadiabatic quantum dynamic model has been developed to study the process of electron emission from a low-work-function metal surface. The process is initiated by scattering a highly vibrationally excited NO molecule from a surface composed of a Cs layer covering a Ru crystal. The model addresses the increasing quantum yield of the electron emission as a function of the molecular vibrational excitation and incident kinetic energy. The reaction mechanism is identified as a long-range harpooning electron transfer to a molecular ion which is then accelerated toward the surface. Upon impact, the molecular ion emits its excess electron. 相似文献
2.
Rahimipour S Litichever-Coslovsky N Alaluf M Freeman D Ehrenberg B Weiner L Mazur Y Fridkin M Koch Y 《Photochemistry and photobiology》2005,81(2):250-258
A combination of light, oxygen and a photosensitizer is used to induce death of cancer cells by photodynamic therapy. In this study, we have synthesized several new methyl helianthrone derivatives and compared their phototoxicity with that of hypericin. In contrast to hypericin, methyl helianthrones are soluble in aqueous solutions and have a broad range of light absorbance, which allows the use of polychromatic light. Structural modifications of methyl helianthrone demonstrated that substitution of hydrogen atoms of methyl helianthrone at Positions 2 and 5 with Br atoms or methylation of its phenolic hydroxyls, significantly increases the corresponding singlet oxygen quantum yield and their phototoxicity toward alphaT3-1, M2R and LNCaP cells. The phototoxicity of some of these compounds was similar to that of hypericin. Methyl helianthrones, like hypericin, accumulated mainly in the perinuclear region as evident by confocal microscopy. Irradiation of cells pretreated with methyl helianthrone derivatives generates intracellular reactive oxygen species and lipid free radicals, as shown by a fluorescentic probe and electron paramagnetic resonance methods, respectively. The phototoxicity of these methyl helianthrones as well as their ability to oxidize membrane lipids were significantly decreased on addition of specific Type-II inhibitors, suggesting the involvement of singlet oxygen as the main oxidant. 相似文献
3.
Time resolved chemiluminescence spectra of pure tetramethyldioxetane are obtained for the first time using pulsed infrared laser excitation. The only major product, acetone, is shown to be formed by at least two pathways: a unimolecular, collision free, decomposition and a collision induced mechanism. Spectral and temporal behaviour indicate that neither singlet nor triplet acetone are the primary products. Other possibilities are discussed. 相似文献
4.
We consider Albrecht's theory for Raman scattering of fundamentals in the far and pre-resonance regions. Destructive interferences inherent to the A and B terms augment the conventionally suppressed C term dramatically. Raman excitation profiles for the ν1(a1g) and ν6(e2g fundamentals in benzene can be well fitted with theoretical C-term profiles involving the 1E1u(π-π*) state at 1800 A. 相似文献
5.
Rini M Pines D Magnes BZ Pines E Nibbering ET 《The Journal of chemical physics》2004,121(19):9593-9610
We investigate one of the fundamental reactions in solutions, the neutralization of an acid by a base. We use a photoacid, 8-hydroxy-1,3,6-trisulfonate-pyrene (HPTS; pyranine), which upon photoexcitation reacts with acetate under transfer of a deuteron (solvent: deuterated water). We analyze in detail the resulting bimodal reaction dynamics between the photoacid and the base, the first report on which was recently published. We have ascribed the bimodal proton-transfer dynamics to contributions from preformed hydrogen bonding complexes and from initially uncomplexed acid and base. We report on the observation of an additional (6 ps)(-1) contribution to the reaction rate constant. As before, we analyze the slower part of the reaction within the framework of the diffusion model and the fastest part by a static, sub-150 fs reaction rate. Adding the second static term considerably improves the overall modeling of the experimental results. It also allows to connect experimentally the diffusion controlled bimolecular reaction models as defined by Eigen-Weller and by Collins-Kimball. Our findings are in agreement with a three-stage mechanism for liquid phase intermolecular proton transfer: mutual diffusion of acid and base to form a "loose" encounter complex, followed by reorganization of the solvent shells and by "tightening" of the acid-base encounter complex. These rearrangements last a few picoseconds and enable a prompt proton transfer along the reaction coordinate, which occurs faster than our time resolution of 150 fs. Alternative models for the explanation of the slower "on-contact" reaction time of the loose encounter complex in terms of proton transmission through a von Grotthuss mechanism are also discussed. 相似文献
6.
L. Allen Kindman Charles E. Cohen Michael H. Zeldin Yehuda Ben-Shaul Jerome A. Schiff 《Photochemistry and photobiology》1978,27(6):787-794
Abstract— Absorption measurements in the 600–720 nm region of dark-grown cells of Euglena gracilis Klebs var. bacillaris Cori were made in vivo at room temperature using computer-assisted spectrophotometry. Dark-grown wild-type cells have a prominent absorption maximum at 634 nm due to protochlorophyll(ide) absorption. Upon illumination, the absorption at 634nm decreases and a peak appears at 674nm, representing the phototransformation of protochlorophyll(ide) to chlorophyll(ide). Using difference spectroscopy, the resynthesis in the dark of protochlorophyll(ide) by previously-illuminated wild-type dark-grown cells was found to begin at about 10min after illumination and reached completion by about 25 min, the amount of protochlorophyll(ide) resynthesized being equivalent to that of dark-grown cells. Resynthesis of protochlorophyll(ide) following a second illumination follows the same kinetics, indicating that protochlorophyll(ide) resynthesis is under tight regulation, possibly via feedback control. Cells of dark-grown wild-type and W3BUL, a mutant lacking protochlorophyll(ide) contain a component absorbing at 658 nm which does not undergo phototransformation when examined by difference spectroscopy at room and liquid N2 temperatures. Following the phototransformation of protochlorophyll(ide) 634 to chlorophyll(ide) 674, the chlorophyll(ide) 674 shifts to shorter wavelengths, ultimately to 671 nm. Possible relationships among the various spectroscopic forms of protochlorophyll(ide) and chlorophyll(ide) at room temperature and liquid N2 temperature in Euglena and higher plants are presented. It is concluded that Euglena, unlike older, etiolated higher plants, contains only protochlorophyll(ide) 634, making it an excellent system in which to examine the phototransformation of this pigment species in the absence of other forms. 相似文献
7.
Different methods for the interpretation of linear dichroic spectra of molecules incorporated in uniaxial matrices are discussed. A method based on the combination of both polarized absorption and emission measurements is described for the resolution of absorption and emission spectra into their different polarized components, and for the investigation of molecular distributions in the oriented matrix. The distributions of some planar molecules of different shapes incorporated in stretched polyethylene films are presented. 相似文献
8.
We show that for some absolute (explicit) constant C, the following holds for every finitely generated group G, and all d > 0: If there is some
R
0 > exp(exp(Cd
C
)) for which the number of elements in a ball of radius R
0 in a Cayley graph of G is bounded by R0d{R_0^d} , then G has a finite-index subgroup which is nilpotent (of step < C
d
). An effective bound on the finite index is provided if “nilpotent” is replaced by “polycyclic”, thus yielding a non-trivial
result for finite groups as well. 相似文献
9.
The recently developed Classical Stochastic Diffusion Theory is applied to obtain the coverage dependence of desorption rates for Xe on W(111). Using the attractive Xe-Xe potential from gas phase experiments, we find a strong coverage dependence in the desorption rates and calculate Temperature Programmed Desorption Spectra (for a potential with reduced attractiveness) that are in excellent qualitative agreement with experimental results. We also investigated the effect of purely repulsive adsorbate-adsorbate interactions where we find, for some coverage ranges, that two different adsorption configurations can be stable (at different temperatures) leading to a marked change in the corresponding desorption rates and to distinct non-Arrhenius behavior. 相似文献
10.
The anti-Ramsey number, AR(n, G), for a graph G and an integer \(n\ge |V(G)|\), is defined to be the minimal integer r such that in any edge-colouring of \(K_n\) by at least r colours there is a multicoloured copy of G, namely, a copy of G that each of its edges has a distinct colour. In this paper we determine, for large enough \(n,\, AR(n,L\cup tP_2)\) and \(AR(n,L\cup kP_3)\) for any large enough t and k, and a graph L satisfying some conditions. Consequently, we determine AR(n, G), for large enough n, where G is \(P_3\cup tP_2\) for any \(t\ge 3,\, P_4\cup tP_2\) and \(C_3\cup tP_2\) for any \(t\ge 2,\, kP_3\) for any \(k\ge 3,\, tP_2\cup kP_3\) for any \(t\ge 1,\, k\ge 2\), and \(P_{t+1}\cup kP_3\) for any \(t\ge 3,\, k\ge 1\). Furthermore, we obtain upper and lower bounds for AR(n, G), for large enough n, where G is \(P_{k+1}\cup tP_2\) and \(C_k\cup tP_2\) for any \(k\ge 4,\, t\ge 1\). 相似文献