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951.
Colvin MT Ricks AB Scott AM Smeigh AL Carmieli R Miura T Wasielewski MR 《Journal of the American Chemical Society》2011,133(5):1240-1243
A covalent, fixed-distance donor-bridge-acceptor (D-B-A) molecule was synthesized that upon photoexcitation undergoes ultrafast charge separation to yield a radical ion pair (RP) in which the spin-spin exchange interaction (2J) between the two radicals is sufficiently large to result in preferential RP intersystem crossing to the highest-energy RP eigenstate (T(+1)) at the 350 mT magnetic field characteristic of X-band (9.5 GHz) EPR spectroscopy. This behavior is unprecedented in covalent D-B-A molecules, and is evidenced by the time-resolved EPR (TREPR) spectrum at X-band of (3*)D-B-A derived from RP recombination, which shows all six canonical EPR transitions polarized in emission (e,e,e,e,e,e). In contrast, when the RP is photogenerated in a 3400 mT magnetic field, the TREPR triplet spectrum at W-band (94 GHz) of (3*)D-B-A displays the (a,e,e,a,a,e) polarization pattern characteristic of a weakly coupled RP precursor, similar to that observed in photosynthetic reaction center proteins, and indicates a switch to selective population of the lower-energy T(0) eigenstate. 相似文献
952.
Fujiwara N Kinoshita M Uchida A Ono M Kato K Akita H 《Chemical & pharmaceutical bulletin》2012,60(4):562-570
The reactions of (±)-α-epoxy drimenol (4) and (±)-α-epoxy drimenyl cyanide (6) with acids (proton acid or Lewis acid) selectively gave the rearranged aldehyde (±)-13 and (±)-15 having the hydroindane skeleton, respectively, while the reactions of (±)-4 and (±)-6 with Dibal-H selectively afforded the allyl alcohol (±)-14 and (±)-16, respectively. The reactions of (8aR)-6 and (8aS)-6 with Dibal-H were applied for the determination of the absolute structure of natural 7β-acetoxy-ent-labda-8(17),13(14)E-dien-15-ol (18). The reaction of (±)-α-epoxy bicyclofarnesol (5) and (8aS)-5 with proton acid selectively provided the rearranged ketol (±)- and (8aS)-31 having the hydroindane skeleton, respectively. The optically active (8aS)-31 was converted to the natural (9S)-austrodoric acid (33). 相似文献
953.
This paper presents a simple method to change the hydrophilic nature of the glass surface in a poly(dimethylsiloxane) (PDMS)-glass hybrid microfluidic device to hydrophobic by an extra-heating step during the fabrication process. Glass substrates bonded to a native or oxygen plasma-treated PDMS chip having microchambers (12.5 mm diameter, 110 μm height) were heated at 200°C for 3 h, and then the hydrophobicity of the glass surfaces on the substrate was evaluated by measuring the contact angle of water. By the extra-heating process, the glass surfaces became hydrophobic, and its contact angle was around 109°, which is nearly the same as native PDMS surfaces. To demonstrate the usefulness of this surface modification method, a PDMS-glass hybrid microfluidic device equipped with microcapillary vent structures for pneumatic manipulation of droplets was fabricated. The feasibility of the microcapillary vent structures on the device with the hydrophobic glass surfaces are confirmed in practical use through leakage tests of the vent structures and liquid handling for the electrophoretic separation of DNA molecules. 相似文献
954.
Dr. Hironobu Ozawa Megumi Awa Dr. Takahiko Ono Prof. Dr. Hironori Arakawa 《化学:亚洲杂志》2012,7(1):156-162
The effects of the dye‐adsorption solvent on the performances of the dye‐sensitized solar cells (DSSCs) based on black dye have been investigated. The highest conversion efficiency (10.6 %) was obtained in the cases for which 1‐PrOH and the mixed solvent of EtOH and tBuOH (3:1 v/v) were employed as dye‐adsorption solvents. The optimized value for the dielectric constant of the dye‐adsorption solvent was found to be around 20. The DSSCs that used MeOH as a dye‐adsorption solvent showed inferior solar‐cell performance relative to the DSSCs that used EtOH, 1‐PrOH, 2‐PrOH, and 1‐BuOH. Photo‐ and electrochemical measurements of black dye both in solution and adsorbed onto the TiO2 surface revealed that black dye aggregates at the TiO2 surface during the adsorption process in the case for MeOH. Both the shorter electron lifetime in the TiO2 photoelectrode and the greater resistance in the TiO2–dye–elecrolyte interface, attributed to the dye aggregation at the TiO2 surface, cause the decrease in the solar‐cell performance of the DSSC that used MeOH as a dye adsorption solvent. 相似文献
955.
Okada T Yago T Takamasu T Wakasa M 《Physical chemistry chemical physics : PCCP》2012,14(10):3490-3497
Magnetic field effects (MFEs) on the photoinduced hydrogen abstraction reaction of benzophenone with phenol were investigated in ionic liquids (ILs) with a short alkyl chain (N,N,N-trimethyl-N-propylammonium bis(trifluoromethanesulfonyl)amide (TMPA TFSA)) and long alkyl chains ((N,N,N-trimethyl-N-octylammonium bis(trifluoromethanesulfonyl)amide (TMOA TFSA) and N-decyl-N,N,N-trimethylammonium bis(trifluoromethanesulfonyl)amide (DTMA TFSA)) by a nanosecond laser flash photolysis technique. In each ionic liquid, escaped radical yield of a benzophenone ketyl radical rapidly increased with increasing magnetic field strength (B) of 0 T < B≤ 0.01 T. At 0.01 T < B≤ 0.4 T, the escaped radical yield almost saturated in TMPA TFSA or gradually increased in TMOA TFSA and DTMA TFSA. At much higher fields of 0.4 T < B≤ 30 T, the yield gradually decreased, resulting in 10-15% decrease at 30 T. The observed MFEs can be explained by the hyperfine coupling and Δg mechanisms together with the relaxation mechanism. On the time profiles of the transient absorption observed for the benzophenone ketyl radical, MFEs were generated in the time range of 0 < t < 0.6 μs. The cage lifetimes of TMOA TFSA and DTMA TFSA were estimated to be at least 120 ns. 相似文献
956.
J Matos LK Ono F Behafarid JR Croy S Mostafa AT DeLaRiva AK Datye AI Frenkel B Roldan Cuenya 《Physical chemistry chemical physics : PCCP》2012,14(32):11457-11467
The thermal stability of inverse micelle prepared Pt nanoparticles (NPs) supported on nanocrystalline γ-Al(2)O(3) was monitored in situ under different chemical environments (H(2), O(2), H(2)O) via extended X-ray absorption fine-structure spectroscopy (EXAFS) and ex situ via scanning transmission electron microscopy (STEM). Drastic differences in the stability of identically synthesized NP samples were observed upon exposure to two different pre-treatments. In particular, exposure to O(2) at 400 °C before high temperature annealing in H(2) (800 °C) was found to result in the stabilization of the inverse micelle prepared Pt NPs, reaching a maximum overall size after moderate coarsening of ~1 nm. Interestingly, when an analogous sample was pre-treated in H(2) at ~400 °C, a final size of ~5 nm was reached at 800 °C. The beneficial role of oxygen in the stabilization of small Pt NPs was also observed in situ during annealing treatments in O(2) at 450 °C for several hours. In particular, while NPs of 0.5 ± 0.1 nm initial average size did not display any significant sintering (0.6 ± 0.2 nm final size), an analogous thermal treatment in hydrogen leads to NP coarsening (1.2 ± 0.3 nm). The same sample pre-dosed and annealed in an atmosphere containing water only displayed moderate sintering (0.8 ± 0.3 nm). Our data suggest that PtO(x) species, possibly modifying the NP/support interface, play a role in the stabilization of small Pt NPs. Our study reveals the enhanced thermal stability of inverse micelle prepared Pt NPs and the importance of the sample pre-treatment and annealing environment in the minimization of undesired sintering processes affecting the catalytic performance of nanosized particles. 相似文献
957.
Gauss’s hypergeometric function gives periods of elliptic curves in Legendre normal form. Certain truncations of this hypergeometric function give the Hasse invariants for these curves. Here we study another form, which we call the Clausen form, and we prove that certain truncations of and in $\mathbb {F}_{p}[x]$ are related to the characteristic p Hasse invariants. 相似文献
958.
959.
Hiroshi Ono Mitsuru Kuzuwata Tomoyuki Sasaki Kohei Noda Nobuhiro Kawatsuki 《Applied physics. B, Lasers and optics》2014,114(4):567-571
The blazed vector grating possessing antisymmetric distributions of the birefringence were fabricated by exposing the line-focused linearly polarized ultraviolet light on the photosensitive polymer liquid crystals. The polarization states of the diffraction beams can be highly and widely controlled by designing the blazed structures, and the diffraction properties were well-explained by Jones calculus. 相似文献
960.
Hiroshi Ono Ryoya Hasebe Tomoyuki Sasaki Kohei Noda Nobuhiro Kawatsuki 《Applied Physics A: Materials Science & Processing》2014,114(4):1353-1360
This article presents effects of photocrosslinking on photorefractive properties in polymer-liquid crystal composites doped with fullerene (C60) as a photoconductive agent. The efficiency of the photorefraction was improved by crosslinking the polymer network and reached near to the theoretical limit for the thin phase grating. The carrier conduction in the composite films was investigated and the high-performance photorefractivity of the photocrosslinked mesogenic composite was explained by low dark current and high photocurrent. The firm crosslinked polymer network in the polymer-liquid crystal composite has also employed for the stable photorefractive diffraction at elevated temperature and under a static dc field applied the mesogenic composite film. 相似文献