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41.
MPW1K density functional calculations, carried out with the 6-31+G(d,p) basis set, have been combined with canonical variational transition state theory (CVT) and small-curvature tunneling (SCT) corrections in order to compute the primary kinetic isotope effects for rearrangement of 5-methyl-1,3-cyclopentadiene (1) to 1-methyl-1,3-cyclopentadiene (2). The Swain-Schaad exponents, SSE = ln(kH/kT)/ln(kD/kT), for this reaction have been computed over the temperature range 100-600 K. Tunneling results in both large positive and large negative deviations from the value of SSE = 3.26, expected from consideration of only the effect of the isotopic mass on passage over the reaction barrier. In the rearrangement of 1 to 2, SSE approximately 3.26, not only at temperatures >400 K, where tunneling is relatively unimportant, but also around 170 K, where tunneling by both H and D is the dominant mode of reaction. Thus, from an experimental finding that SSE approximately 3.26 at a single temperature, it cannot be rigorously concluded that tunneling is unimportant. Measurement of SSEs over a broad temperature range is advisable; but measurement of the temperature dependence of just kH/kD can be used to establish more unequivocally whether tunneling is important, without the necessity of measuring kT. 相似文献
42.
A newly developed interface coupling a CHN combustion device (elemental analyser 'EA') to an isotope ratio mass spectrometer is described and evaluated. The purpose of the device is to extend the dynamic range of delta(13)C and delta(15)N analysis from less than 2 orders of magnitude to more than 3 orders of magnitude. Carbon isotope ratio measurements of atropine as a model compound have been performed analysing between 1 μg to 5 mg C with acceptable to excellent precision (0.6 to 0.06 per thousand, delta-notation). The correction due to the blank signal is critical for sample amounts smaller than 4 μg C. The maximum sample weight is determined by the combustion capacity of the EA. Larger sample amounts are measured using dilution of a small part of the EA effluent with helium. The dilution mechanism works virtually free of isotope fractionation. Copyright 1999 John Wiley & Sons, Ltd. 相似文献
43.
Modeling and analysis of time series are important in applications including economics, engineering, environmental science and social science. Selecting the best time series model with accurate parameters in forecasting is a challenging objective for scientists and academic researchers. Hybrid models combining neural networks and traditional Autoregressive Moving Average (ARMA) models are being used to improve the accuracy of modeling and forecasting time series. Most of the existing time series models are selected by information-theoretic approaches, such as AIC, BIC, and HQ. This paper revisits a model selection technique based on Minimum Message Length (MML) and investigates its use in hybrid time series analysis. MML is a Bayesian information-theoretic approach and has been used in selecting the best ARMA model. We utilize the long short-term memory (LSTM) approach to construct a hybrid ARMA-LSTM model and show that MML performs better than AIC, BIC, and HQ in selecting the model—both in the traditional ARMA models (without LSTM) and with hybrid ARMA-LSTM models. These results held on simulated data and both real-world datasets that we considered.We also develop a simple MML ARIMA model. 相似文献
44.
DP Shelton 《The Journal of chemical physics》2012,137(4):044312
Measurements of hyper-Rayleigh scattering intensities and polarization ratios are presented for nine small molecules in the gas phase [CH(4), CF(4), CCl(4), N(2)O, NH(3), D(2)O, SO(2), CF(2)Cl(2), and (CH(3))(2)CO]. In four cases [CH(4), CF(4), CCl(4), and N(2)O] all molecular hyperpolarizability tensor components can be determined from the measurements. The results of this experiment are compared with the results of previous ab initio calculations, finding discrepancies up to 60%. Including vibrational contributions decreases the discrepancies for CH(4) and CF(4) and increases them for CCl(4), D(2)O, and NH(3). 相似文献
45.
David G. Parker 《中国颗粒学报》2009,7(2)
This paper describes the operation and outcome of one of the United Kingdom's largest multi-partner research activities in nanoparticles.The research covers the discovery and development of organic and inorganic crystals/nanoparticles,nanoparticle properties towards specific product applications,The research also encompassed bespoke measurement technology for nanoparticles and structure interactions.Significant research outcomes are summarised.The paper illustrates the advantages from industrially motivated research and value of collective action between a broad group of researchers in a nation. 相似文献
46.
Zi Jie Lin Jared Bies Shanina S. Johnson John D. Gorden Jacqueline F. Strickland Monica Frazier Jonathan M. Meyers Kerri L. Shelton 《Journal of heterocyclic chemistry》2019,56(2):533-538
A series of 1,4‐N,N′‐bis‐substituted 1,2,4‐triazolium bromide salts were synthesized and tested for anti‐proliferative activity. 1,4‐Bis(naphthalen‐2‐ylmethyl)‐1,2,4‐triazolium bromide ( 2 ) showed activity against MDA‐MB‐468 breast cancer and PC‐3 prostate cancer cell lines. 相似文献
47.
D. Allasia C. Angelini A. Baldini L. Bertanza F. Bianchi A. Bigi F. Bobisut A. Borg P. Capiluppi R. Cirio J. Derkaoui M. L. Faccini-Turluer A. G. Frodesen D. Gamba G. Giacomelli B. Jongejans G. Mandrioli A. Margiotta-Neri A. Marzari-Chiesa R. Pazzi L. Patrizii C. Petri F. Predieri A. Romero A. M. Rossi A. Sconza P. Serra-Lugaresi M. Spurio A. G. Tenner G. W. van Apeldoorn P. H. A. van Dam N. A. M. van Eijndoven D. Vignaud WA Collaboration 《Zeitschrift fur Physik C Particles and Fields》1988,37(4):527-533
Bose-Einstein correlations between pions of equal charge have been observed in Charged Current and Neutral Current (anti)neutrino-deuterium interactions in the BEBC bubble chamber exposed to the SPS wide band beam. The pion emission region is found to be essentially spherical with a mean radius of (0.48±0.07) fm; the chaoticity parameter is 0.36±0.04. 相似文献
48.
Twenty-seven ternary intermetallic compounds belonging to either the ThCr2Si2-type or the CaBe2Ge2-type structures are investigated for their superconducting properties. The primitive tetragonal CaBe2Ge2-type structure consistently favors superconductivity over the ThCr2Si2-type structure for which we find no superconductivity above 1.1 K. 相似文献
49.
M. Bonesini E. Bonvin P. S. L. Booth R. Bopp L. J. Carroll A. J. Cass D. Cavalli S. U. Chung G. Costa M. Donnat P. A. Dorsaz E. Durieux M. E. J. Feliks J. R. Fischer L. Fluri F. Gianotti S. Jack J. N. Jackson M. Kelly M. N. Kienzle-Focacci R. Lucock J. G. Lynch L. Mandelli M. Martin L. Mathys A. Maxwell M. Mazzanti P. J. Negus L. Perini D. Perrin G. Polesello R. Poultney W. H. Range L. Rosselet S. W. Snow A. S. Thompson R. M. Turnbull M. Werlen WA -Collaboration 《Zeitschrift fur Physik C Particles and Fields》1989,42(4):527-532
The inclusive cross sections for η production by the interactions of 280 GeV/c momentum π?, π+, and proton beams in hydrogen have been measured. The kinematical range covered is ?0.45<x F <0.45, and 4.0<P T <7.0 GeV/c for Feynmanx F and transverse momentum respectively. The η to π0 cross section ratios are given for the three reactions. The ratio of π? p to π+ p cross sections for η production in the above kinematic ranges is 1.22±0.08±0.11. 相似文献
50.
M. K. Hasan J. S. Kouvel H. B. Radousky T. J. Goodwin R. N. Shelton 《Physica C: Superconductivity and its Applications》1996,270(3-4):216-222
Rotational magnetization-vector measurements were carried out on a superconducting polycrystalline disk of EuCSCNO. The results at 4.2 K and low fields resemble recent results for YBa2Cu3O7−δ (YBCO) and Ba0.57K0.43BiO3 (BKBO) in revealing a broad distribution in the strength of the vortex pinning torques. This resemblance extends to higher fields, where it was found that the average pinning torque per vortex (τp), which is directly related to the critical current density, decreases steadily with increasing field in a manner consistent with vortex bundling. Quantitatively, however, the values of τp for EuCSCNO are smaller by an order of magnitude than those for YBCO but are only moderately smaller than those for BKBO. This comparison supports the notion that the vortex pinning may derive in part from deviations from oxygen stoichiometry, which are normally present in YBCO but are essentially absent in EuCSCNO and BKBO. Moreover, as in YBCO and BKBO, the τp in EuCSCNO at fixed field is found to diminish rapidly as the temperature rises towards Tc. 相似文献