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951.
Sakko A Galambosi S Inkinen J Pylkkänen T Hakala M Huotari S Hämäläinen K 《Physical chemistry chemical physics : PCCP》2011,13(24):11678-11685
We report non-resonant inelastic X-ray scattering experiments of several gaseous samples in the inner-shell excitation energy range. The experimental near-edge spectra from all the K-edges of N(2), N(2)O, and CO(2) including the momentum transfer dependence are presented. The results are analyzed using density functional theory calculations that accurately reproduce the experimental spectral features. We observe vibrational effects in the measured spectrum and in the calculations the atomic motion is modeled using the Franck-Condon approximation and the linear coupling model. Our findings show that vibrational effects cannot be neglected in the analysis of high resolution inelastic X-ray scattering spectroscopy. The results also support the validity of the transition potential approximation for calculating core excited state potential energy surfaces. 相似文献
952.
Buldyreva J Guinet M Eliet S Hindle F Mouret G Bocquet R Cuisset A 《Physical chemistry chemical physics : PCCP》2011,13(45):20326-20334
The case of symmetric tops CH(3)X (X = Br, Cl, F, …) perturbed by non-polar diatoms Y(2) (Y = N(2), O(2), …) is analysed from the viewpoint of theoretical collisional broadening of their rotational lines observed in atmospheric spectra. A semi-classical approach involving an exponential representation of the scattering operator and exact trajectories governed by the isotropic potential is presented. For the first time the active molecule is strictly treated as a symmetric top and the atom-atom interactions are included in the intermolecular potential model. It is shown for the CH(3)Cl-O(2) system that these interactions contribute significantly to the line width for all values of the rotational quantum numbers J and K. Additional testing of modifications required in the semi-classical formalism for a correct application of the cumulant expansion is performed and it is shown that the use of the cumulant average on the rotational states of the perturbing molecule leads to entirely negligible effects for the not very strongly interacting CH(3)Cl-O(2) system. In order to check the theoretical predictions and to extend the scarce experimental data available in the literature to higher values of the rotational quantum numbers, new measurements of room-temperature O(2)-broadened CH(3)Cl rotational lines are carried out by a photomixing continuous-wave terahertz spectrometer. The experimental line widths extracted with a Voigt profile model demonstrate an excellent agreement with theoretical results up to very high J-values (J = 31, 37, 40, 45, 50). 相似文献
953.
Four M Riehl D Mongin O Blanchard-Desce M Lawson-Daku LM Moreau J Chauvin J Delaire JA Lemercier G 《Physical chemistry chemical physics : PCCP》2011,13(38):17304-17312
In this article, the synthesis of a novel high-conjugated ligand and its corresponding Ru(II) complex PTFTF:Ru is reported, along with the linear and nonlinear optical characterizations. Two-photon absorption based optical power limiting properties (OPL), especially in the near infrared, are described and compared to those of the analogous complexes previously published. Combined with a preliminary theoretical approach, this allows us to highlight several key parameters for OPL optimization in such molecular systems and more particularly the spectral overlap between TPA and excited-state absorption. 相似文献
954.
Pospíšil L Hromadová M Fanelli N Valášek M Kolivoška V Gál M 《Physical chemistry chemical physics : PCCP》2011,13(10):4365-4371
A long organic molecule 1 with five bipyridinium functions separated by benzene rings (extended viologen) undergoes a reversible multi-step electron transfer. Here we show that this decacation accepts electrons at the heterogeneous interface with the occurrence of the periodically changing electric reduction currents. According to the applied bias voltage the observed current-time dependence changes from chaotic through periodic and irregular to sinusoidal and finally to monotonous. A careful choice of the controlling parameters yields the sustained periodic sinusoidal currents lasting for a prolonged time. Oscillations stem from a mutual interplay of the heterogeneous supply of electrons and the homogeneous redox reactions (disproportionation) between the transient redox forms. In difference to many other electrochemical oscillating systems the described oscillations do not require any additional external impedance. The principle of these oscillatory currents may serve as a model of a truly 'molecular oscillator'. 相似文献
955.
High sensitive matrix-free mass spectrometry analysis of peptides using silicon nanowires-based digital microfluidic device 总被引:1,自引:0,他引:1
Lapierre F Piret G Drobecq H Melnyk O Coffinier Y Thomy V Boukherroub R 《Lab on a chip》2011,11(9):1620-1628
We present for the first time an electrowetting on dielectric (EWOD) microfluidic system coupled to a surface-assisted laser desorption-ionization (SALDI) silicon nanowire-based interface for mass spectrometry (MS) analysis of small biomolecules. Here, the transfer of analytes has been achieved on specific locations on the SALDI interface followed by their subsequent mass spectrometry analysis without the use of an organic matrix. To achieve this purpose, a device comprising a digital microfluidic system and a patterned superhydrophobic/superhydrophilic silicon nanowire interface was developed. The digital microfluidic system serves for the displacement of the droplets containing analytes, via an electrowetting actuation, inside the superhydrophilic patterns. The nanostructured silicon interface acts as an inorganic target for matrix-free laser desorption-ionization mass spectrometry analysis of the dried analytes. The proposed device can be easily used to realize several basic operations of a Lab-on-Chip such as analyte displacement and rinsing prior to MS analysis. We have demonstrated that the analysis of low molecular weight compounds (700 m/z) can be achieved with a very high sensitivity (down to 10 fmol μL(-1)). 相似文献
956.
The biochemical composition of leaves from Coffea pseudozanguebariae, a wild caffeine-free coffee species, was determined. Two phenolic compounds were extracted from leaves, separated and characterized. Their structures were elucidated by mass spectrometry, and 1D and 2D NMR spectroscopy and were shown to be mangiferin (1) and isomangiferin (2), which were the main polyphenol products. Multiphoton fluorescence imaging was performed to visualize polyphenol distribution in leaf cross sections. Consistent biochemical analysis cell imaging techniques on leaves revealed yellow fluorescence in the epidermis and parenchyma cells corresponding to xanthone compounds. 相似文献
957.
Vincent Denoël Emmanuel Detournay 《International Journal of Solids and Structures》2011,48(3-4):625-636
The formulation of the constrained elastica problem proposed in this paper is predicated on two key concepts: first, the deformed elastica is described by means of the distance from the conduit axis; second, the problem is formulated in terms of the Eulerian curvilinear coordinate of the conduit rather than the natural curvilinear coordinate of the elastica. This approach is further implemented within a segmentation algorithm, which transforms the global constrained elastica problem into a sequence of analogous auxiliary problems that result from dividing the conduit and the elastica into segments limited by contacts. Each auxiliary segment entails solving a segment of elastica subject to isoperimetric constraints corresponding to the assumed positions of the segment ends along the conduit. This new formulation resolves in one stroke a series of issues that afflict the classical Lagrangian approach: (i) the contact detection is reduced to checking whether a threshold on the distance function is violated, (ii) the isoperimetric conditions are transformed into regular boundary conditions, instead of being treated as external integral constraints, (iii) the method yields a well-conditioned set of equations that does not degenerate with decreasing flexural rigidity of the elastica and/or decreasing clearance between the conduit and the elastica. 相似文献
958.
Pekka Kekäläinen Mikko Voutilainen Antti Poteri Pirkko Hölttä Aimo Hautojärvi Jussi Timonen 《Transport in Porous Media》2011,87(1):125-149
A model transport system is considered in which a pulse of tracer molecules is advected along a flow channel with porous walls.
The advected tracer thus undergoes diffusion, matrix-diffusion, inside the walls, which affects the breakthrough curve of
the tracer. Analytical solutions in the form of series expansions are derived for a number of situations which include a finite
depth of the porous matrix, varying aperture of the flow channel, and longitudinal diffusion and Taylor dispersion of the
tracer in the flow channel. Novel expansions for the Laplace transforms of the concentration in the channel facilitated closed-form
expressions for the solutions. A rigorous result is also derived for the asymptotic form of the breakthrough curve for a finite
depth of the porous matrix, which is very different from that for an infinite matrix. A specific experimental system was created
for validation of matrix-diffusion modeling for a matrix of finite depth. A previously reported fracture-column experiment
was also modeled. In both cases model solutions gave excellent fits to the measured breakthrough curves with very consistent
values for the diffusion coefficients used as the fitting parameters. The matrix-diffusion modeling performed could thereby
be validated. 相似文献
959.
Refractive-index and density matching in concentrated particle suspensions: a review 总被引:1,自引:0,他引:1
Sébastien Wiederseiner Nicolas Andreini Gaël Epely-Chauvin Christophe Ancey 《Experiments in fluids》2011,50(5):1183-1206
Optical measurement techniques such as particle image velocimetry (PIV) and laser Doppler velocimetry (LDV) are now routinely used in experimental fluid mechanics to investigate pure fluids or dilute suspensions. For highly
concentrated particle suspensions, material turbidity has long been a substantial impediment to these techniques, which explains
why they have been scarcely used so far. A renewed interest has emerged with the development of specific methods combining
the use of iso-index suspensions and imaging techniques. This review paper gives a broad overview of recent advances in visualization
techniques suited to concentrated particle suspensions. In particular, we show how classic methods such as PIV, LDV, particle tracking velocimetry, and laser induced fluorescence can be adapted to deal with concentrated particle suspensions. 相似文献
960.
For homogeneous isotropic turbulence study, the acquisition of band-pass filtered velocity increments (FVI) in a non-forced turbulent box is still a challenge both experimentally and numerically. Turbulence and associated physical processes, at a given instant, are permanently contaminated by a forcing process which can seldom be universal. The situation tends to be the origin of intermittency and the non-Gaussian probability density distribution for acceleration and velocity gradients. To reveal implied mechanism, grid turbulence is adapted to observe non-perturbed homogeneous isotropic turbulence. The velocity increments (VI) can be obtained following Comte-Bellot and Corrsin (GCBC) by means of two point-two time shifted velocity measurements. It is difficult to obtain decaying turbulence (DT) at large turbulent Reynolds number without pollution coming from walls. Nevertheless it is also significant to investigate DT in low Reynolds number regimes to determine non-polluted tendencies. The similarity of DT between particle image velocimetry (PIV) and hot wire anemometry measurements by GCBC are presented. Here we focus our tendency on VI and FVI probability density function (PDF) shapes in this letter. In conclusion, the tendency to Gaussian shape in inertial zone wavenumbers, demonstrates that there will be no intermittency if turbulent cascade is not perturbed. 相似文献