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61.
Simpson CD Brand JD Berresheim AJ Przybilla L Räder HJ Müllen K 《Chemistry (Weinheim an der Bergstrasse, Germany)》2002,8(6):1424-1429
In this paper we present the synthesis and characterization of the so far largest polycyclic aromatic hydrocarbon (PAH), containing 222 carbon atoms or 37 separate benzene units. First a suitable three-dimensional oligophenylene precursor molecule is built up by a sequence of Diels-Alder and cyclotrimerization reactions and then planarized in the final step by oxidative cyclodehydrogenation to the corresponding hexagonal PAH. Structural proof is based on isotopically resolved MALDI-TOF mass spectra and electronic characteristics are studied by UV/Vis spectroscopy. 相似文献
62.
On the basis of a pyrrolidine tweezer 1, a library of peptidosulfonamide tweezers (15a-e, 16a-e) was synthesized on the solid phase. This library was screened in a simultaneous substrate screening procedure for the ability to enantioselectively catalyze the Ti(O-i-Pr)(4)-mediated addition of diethylzinc to aldehydes. One of the best solid-phase tweezer catalyst (i.e., 16d, giving an ee of 32% in solid-phase catalysis) was resynthesized in solution (compounds 20 and 21). The now homogeneous solution-phase catalysis showed even better enantioselectivity (i.e., up to 66%). 相似文献
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67.
Brungart DS Simpson BD Darwin CJ Arbogast TL Kidd G 《The Journal of the Acoustical Society of America》2005,117(1):292-304
Recent results have shown that listeners attending to the quieter of two speech signals in one ear (the target ear) are highly susceptible to interference from normal or time-reversed speech signals presented in the unattended ear. However, speech-shaped noise signals have little impact on the segregation of speech in the opposite ear. This suggests that there is a fundamental difference between the across-ear interference effects of speech and nonspeech signals. In this experiment, the intelligibility and contralateral-ear masking characteristics of three synthetic speech signals with parametrically adjustable speech-like properties were examined: (1) a modulated noise-band (MNB) speech signal composed of fixed-frequency bands of envelope-modulated noise; (2) a modulated sine-band (MSB) speech signal composed of fixed-frequency amplitude-modulated sinewaves; and (3) a "sinewave speech" signal composed of sine waves tracking the first four formants of speech. In all three cases, a systematic decrease in performance in the two-talker target-ear listening task was found as the number of bands in the contralateral speech-like masker increased. These results suggest that speech-like fluctuations in the spectral envelope of a signal play an important role in determining the amount of across-ear interference that a signal will produce in a dichotic cocktail-party listening task. 相似文献
68.
Busacca CA Grossbach D Campbell SJ Dong Y Eriksson MC Harris RE Jones PJ Kim JY Lorenz JC McKellop KB O'Brien EM Qiu F Simpson RD Smith L So RC Spinelli EM Vitous J Zavattaro C 《The Journal of organic chemistry》2004,69(16):5187-5195
The Boehringer-Ingelheim phosphinoimidazoline (BIPI) ligands were applied to the formation of chiral quaternary centers in the asymmetric Heck reaction. Several different substrates were examined in detail, using more than 70 members of this new ligand class. Hammett relationships were determined through systematic variation of the ligand electronics. All substrates showed essentially the same Hammett behavior, where enantioselectivity increased as the ligands were made more electron-deficient. Ligand optimization has led to catalysts which give the highest enantioselectivities reported to date for these difficult systems. 相似文献
69.
Simpson HJ Houston BH Liskey SW Frank PA Berdoz AR Kraus LA Frederickson CK Stanic S 《The Journal of the Acoustical Society of America》2003,114(3):1281-1290
Acoustic bottom penetration experiments were carried out in a medium-grain sandy bottom at a site in St. Andrews Bay, Florida. These investigations used a new buried, vertical, one-dimensional synthetic array system where a small hydrophone was water-jetted into the sediment to a depth of approximately 2 m. Once buried, this hydrophone was mounted to a vertical robotics stage that translated the hydrophone upward in 1-cm increments. A broadband (3 to 80 kHz) spherical source, positioned 50 cm above the sediment-water interface, was used to insonify the sediment. Measurements were made with insonification angles above and below the critical angle by changing the horizontal distance of the source relative to the insertion point. This new measurement system is detailed, and results are presented that include temporal, frequency, and wavenumber analysis for natural and roughened interfaces. The measured compressional sound speed and attenuation are shown to be self-consistent using the Kramers-Kronig relation. Furthermore, only a single fast compressional wave was observed. There was no observation of a second slower compressional wave as predicted by some applications of the Biot model to unconsolidated water-saturated porous media. 相似文献
70.
Souchkov AB Simpson JR Quijada M Ishibashi H Hur N Ahn JS Cheong SW Millis AJ Drew HD 《Physical review letters》2003,91(2):027203
We have measured the optical conductivity of single crystal LuMnO3 from 10 to 45000 cm(-1) at temperatures between 4 and 300 K. A symmetry allowed on-site Mn d-d transition near 1.7 eV is observed to blueshift ( approximately 0.1 eV) in the antiferromagnetic state due to Mn-Mn superexchange interactions. Similar anomalies are observed in the temperature dependence of the TO phonon frequencies which arise from spin-phonon interaction. We find that the known anomaly in the temperature dependence of the quasistatic dielectric constant epsilon(0) below T(N) approximately 90 K is overwhelmingly dominated by the phonon contributions. 相似文献