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61.
Mitsukazu Ochi Makoto Yoshizumi Masaki Shimbo 《Journal of Polymer Science.Polymer Physics》1987,25(9):1817-1827
Mechanisms for low-temperature relaxations of three spiro-ring-type epoxide resin systems with and without methoxy branches were investigated by comparison with those of a bisphenol A-type resin system. In the spiro-ring-type epoxide resin systems, two well-defined relaxation peaks, denoted as the β and β′ relaxations, and a shoulder peak were observed at about ?70, +60, and 0°C, respectively. The magnitude of the β relaxation was decreased by the introduction of methoxy branches on the phenylene group. This phenomenon could be interpreted as a result of the formation of hydrogen bonds between the hydroxy-ether group and methoxy branch. Moreover, it was concluded that the β′ relaxation and the shoulder peak are due to the motion of the p-phenylene group adjacent to the spiro-ring and of the hydroxy-ether group blocked by the hydrogen bond, respectively. 相似文献
62.
Junki Ochi Prof. Dr. Kazuo Tanaka Prof. Dr. Yoshiki Chujo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(2):e202214397
Herein, we report the unique solid-state excimer emission of three types of acridine-tethered o-carboranes with variable degrees of methylation at the o-carborane unit. They all showed columnar packing structures based on dimer formation, and two types of π-overlapping motifs were alternately stacked. From the photoluminescence (PL) measurements on the crystalline samples, it was found that three types of luminescence bands can simultaneously appear: monomer emission, excimer emission from the moderately π-stacked intra-dimer unit, and excimer emission from the widely π-stacked inter-dimer unit. Consequently, the PL colors were drastically changed by the steric effect of the methyl groups, with a strong correlation found between the π-overlapping and excimer character. In addition, variable-temperature PL measurements revealed that these PL species should be in thermal equilibrium at room temperature, with the intensity ratios sensitive toward temperature changes. 相似文献
63.
The C-H sigma-bond activation of methane and the N-H sigma-bond activation of ammonia by (Me3SiO)2Ti(=NSiMe3) 1 were theoretically investigated with DFT, MP2 to MP4(SDQ), and CCSD(T) methods. The C-H sigma-bond activation of methane takes place with an activation barrier (Ea) of 14.6 (21.5) kcal/mol and a reaction energy (DeltaE) of -22.7 (-16.5) kcal/mol to afford (Me3SiO)2Ti(Me)[NH(SiMe3)], where DFT- and MP4(SDQ)-calculated values are given without and in parentheses, respectively, hereafter. The electron population of the CH3 group increases, but the H atomic population decreases upon going to the transition state from the precursor complex, which indicates that the C-H sigma-bond activation occurs in heterolytic manner unlike the oxidative addition. The Ti atomic population considerably increases upon going to the transition state from the precursor complex, which indicates that the charge transfer (CT) occurs from methane to Ti. These population changes are induced by the orbital interactions among the d(pi)-p(pi) bonding orbital of the Ti=NSiMe3 moiety, the Ti d(z2) orbital and the C-H sigma-bonding and sigma*-antibonding orbitals of methane. The reverse regioselective C-H sigma-bond activation which leads to formation of (Me3SiO)2Ti(H)[NMe(SiMe3)] takes place with a larger Ea value and smaller exothermicity. The reasons are discussed in terms of Ti-H, Ti-CH3, Ti-NH3, N-H, and N-CH3 bond energies and orbital interactions in the transition state. The N-H sigma-bond activation of ammonia takes place in a heterolytic manner with a larger Ea value of 19.0 (27.9) kcal/mol and considerably larger exothermicity of -45.0 (-39.4) kcal/mol than those of the C-H sigma-bond activation. The N-H sigma-bond activation of ammonia by a Ti-alkylidyne complex, [(PNP)Ti(CSiMe3)] 3 (PNP = N-[2-(PH2)2-phenyl]2-]) ,was also investigated. This reaction takes place with a smaller E(a) value of 7.5 (15.3) kcal/mol and larger exothermicity of -60.2 (-56.1) kcal/mol. These results lead us to predict that the N-H sigma-bond activation of ammonia can be achieved by these complexes. 相似文献
64.
M. Suzuki H. Kiriyama I. Daito Y. Ochi H. Okada M. Sato Y. Tamaoki T. Yoshii J. Maeda S. Matsuoka H. Kan P. R. Bolton A. Sugiyama K. Kondo S. Kawanishi 《Applied physics. B, Lasers and optics》2011,105(2):181-184
The authors have demonstrated an optical parametric chirped-pulse amplification (OPCPA)/Yb:YAG ceramic thin disk hybrid laser system having hundred mJ level pulse energy sub-picosecond pulse duration with high temporal contrast. At an input chirped-pulse energy of 3.8?mJ from an OPCPA preamplifier an output energy of 130?mJ has been generated from multipass diode-pumped Yb:YAG ceramic thin disk amplifier. A recompressed pulse duration of 450?fs with a contrast level of less than 7.2×10?9 at ?150?ps before the main pulse has been obtained. The contrast level is the highest value achieved in Yb:YAG chirped-pulse amplification (CPA) laser system at 100?mJ level. 相似文献
65.
66.
Prof. Dr. Masato Ikeda Rika Ochi Yu‐shi Kurita Prof. Dr. Darrin J. Pochan Prof. Dr. Itaru Hamachi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(41):13091-13096
Controlling the morphology of supramolecular nanostructures in response to external stimuli is an important challenge in the development of functional soft materials. Here we show that a morphological transformation from 2D nanosheets to a network of 1D nanofibers is triggered by heating, which induces molecular conversion of a bolaamphiphile to a hydrogelator by means of a retro‐Diels–Alder reaction, thereby producing a new heat‐set supramolecular hydrogel. We anticipate that our design will be a starting point for more sophisticated supramolecular systems that integrate the thermodynamics of molecular assembly and the kinetics of chemical reactions to create complex supramolecular nanostructures. 相似文献
67.
Hiroyuki Matsuda Makoto Fukano Shinichiro Kikkawa Dana Constantinescu Kiyofumi Kurihara Katsumi Tochigi Kenji Ochi Jürgen Gmehling 《The Journal of chemical thermodynamics》2012,44(1):84-96
(Vapor + liquid) equilibrium (VLE) data for a ternary mixture, namely {methanol + propan-1-ol + dimethyl carbonate (DMC)}, and four binary mixtures, namely an {alcohol (C3 or C4) + DMC}, containing the binary constituent mixtures of the ternary mixture, were measured at p = (40.00 to 93.32) kPa using a modified Swietoslawski-type ebulliometer. The experimental data for the binary systems were correlated using the Wilson model. The Wilson model was also applied to the ternary system to predict the VLE behavior using parameters from the binary mixtures. The modified UNIFAC (Dortmund) model was also tested for the predictions of the VLE behavior of the binary and ternary mixtures. In addition, the experimental VLE data for the ternary and constituent binary mixtures were correlated using the extended Redlich–Kister (ERK) model, which can completely represent the azeotropic points. For the ternary system, a comparison of the experimental and the predicted or correlated boiling points obtained using the Wilson and ERK models showed that the ERK model is more accurate. The valley line, i.e., the curve which divides the patterns of vapor–liquid tie lines, was found in the (methanol + propan-1-ol + DMC) system. This valley line could be represented by the ERK model. Finally, the composition profile for simple distillation of this ternary mixture was obtained by analysis of the residue curves from the estimated Wilson parameters of the constituent binary mixtures. 相似文献
68.
Haroldo Gambini Santos Eduardo Uchoa Luiz Satoru Ochi Nelson Maculan 《Annals of Operations Research》2012,194(1):399-412
This work presents an integer programming formulation for a variant of the Class-Teacher Timetabling problem, which considers
the satisfaction of teacher preferences and also the proper distribution of lessons throughout the week. The formulation contains
a very large number of variables and is enhanced by cuts. Therefore, a cut and column generation algorithm to solve its linear
relaxation is provided. The lower bounds obtained are very good, allowing us to prove the optimality of previously known solutions
in three formerly open instances. 相似文献
69.
Osamu Yamashita Hirotaka Odahara Takahiro Ochi Kouji Satou 《Applied Physics A: Materials Science & Processing》2009,94(1):57-64
The resultant local Seebeck coefficient α
R (=α
S−α
T) at the interface of a thermoelement has not yet been measured, although it is an important factor governing the thermoelectric
efficiency, where α
S is the local Seebeck coefficient and α
T is the one caused by the Thomson effect. It is shown in this paper that α
S, α
T, and α
R of the p- and n-type Cu/Bi–Te/Cu composites are obtained analytically and experimentally on the assumption that the local temperature of
the composite on which the temperature difference ΔT is imposed varies linearly with changes in position along the composite. They were indeed estimated as a function of position
from the local experimental data of R,ΔI,ΔT, and V generated by applying an additional current of ±I to the composite, where R is the electrical resistance and ΔI is a current generated by the composite. As a result, it was found that the absolute values of α
S at the hot interface of the p- and n-type composites are approximately 1.5 and 1.4 times higher than their lowest values in the middle region of the composite,
respectively, while those of α
T are less than 8% of α
S all over the composite and are so small that the relation α
R≈α
S can be held. We thus succeeded in measuring α
R at the interfaces of the composite. 相似文献
70.
Osamu Yamashita Hirotaka Odahara Takahiro Ochi Jun-ichi Shigeto 《Applied Physics A: Materials Science & Processing》2009,97(1):133-141
The local Seebeck coefficient α
L
and the resultant Seebeck coefficient α
R
of M/Bi0.88Sb0.12/M (M = Cu and Ni) composites with different thicknesses t
Bi–Sb of Bi–Sb alloy were measured as functions of z and T, where T is the absolute temperature, z is the distance from a center of Bi–Sb alloy to the middle point of two probes and α
L
and α
R
were measured using two probes separated by s=1.0 mm and s=t
Bi−Sb+0.1 mm, respectively. As a result, α
L
was enhanced extremely at the position of 0.2–0.3 mm away from the interfaces, while the local temperature along a composite
varies linearly with changes in z within Bi–Sb alloy. The local maximum of α
R
at 344 K appeared at t
Bi−Sb≈0.9 mm, so that it is expected to increase up to −167 μV/K at t
Bi−Sb=0.87 mm from the expression fitted well to the experimental data, which is 2.1 times as large as the intrinsic α at 344 K of Bi–Sb alloy. Such a local enhancement in α
L
would probably be caused by a temperature gradient across the depletion layer formed at the interface. The thermoelectric
figure of merit ZT of a composite with an optimum t
Bi−Sb of 0.87 mm is expected to reach the large value of 0.98 at 344 K, which corresponds to 4.5 times as high a value as ZT=0.22 at 344 K of Bi–Sb alloy. It is thus considered that the increase in α
L
at the interface is available as a useful mean of further increase in ZT of thermoelectric devices. 相似文献