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Gap detection thresholds were measured by forced-choice procedure for conditions where the duration of a silent gap was varied adaptively between pairs of sinusoidal markers of the same or different frequency. Frequencies of the first sinusoid in a pair of markers ranged from F1 = 500 to 4000 Hz. Second-sinusoid marker frequencies F2 included F1 = F2, and usually frequencies 2%, 5%, 24%, and 50% higher than F1. In preliminary studies the role of presentation level (E/N0) on gap detection was considered. Preliminary data revealed confounding extraneous factors arising from gating transients and from overall stimulus (i.e., markers + gap) and/or masker duration cues. In the main experiments, the contributions of these extraneous cues were evaluated with experimental designs aimed at identifying and minimizing the confounding roles of these cues in gap detection. For conditions where extraneous gating transient cues were minimized (by presenting the sinusoidal markers in a continuous noise masker with random onset phase for the second sinusoid in every pair of markers) and overall stimulus duration cues were diminished (by randomizing the duration of each marker independently), gap detection thresholds increased from 5 to 90 ms as the frequency separation between F1 and F2 was increased by half an octave. When the gap detection thresholds were treated as filter attenuation values by normalizing and converting the data into decibels, the data were closely fit by the roex filter model. On average, the listeners' performances were modeled well by a constant-percentage (7%) bandwidth filter centered on F1. 相似文献
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3-Methyl-2-butenenitrile (1) cyclodimerised on treatment with lithium diisopropylamide in dimethoxyethane at temperatures between ?78°C and 0°C to 3-amino-4-cyano-1,5,5-trimethyl-1,3-cyclohexadiene (2) the structure of which was established by acid hydrolysis to the known 4-cyano-1,5,5-trimethyl-1-cyclohexene-3-one (3). 相似文献
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Graphene nanoflakes (GNFs) are predicted to possess novel magnetic, optical, and spintronic properties. They have recently been synthesized and a number of applications are being studied. Here we investigate the statistical properties of rippled GNFs (50–5,000 atoms) at $\text{ T}=300$ K. An adjacency matrix is calculated from the coordinates and we find that the free energy, enthalpy, entropy, and atomic displacement all show power law behavior. The vibrational energy versus the Wiener index also shows power law character. We distinguish between using Euclidean topographical indices and compare them to topological ones. These properties are determined from atomic coordinates using MATLAB routines. 相似文献
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T. Parker Maloney Alexander F. Dohoda Alec C. Zhu Forrest E. Michael 《Chemical science》2022,13(7):2121
Herein we report an intermolecular propargylic C–H amination of alkynes. This reaction is operationally convenient and requires no transition metal catalysts or additives. Terminal, silyl, and internal alkynes bearing a wide range of functional groups can be aminated in high yields. The regioselectivity of amination for unsymmetrical internal alkynes is strongly influenced by substitution pattern (tertiary > secondary > primary) and by relatively remote heteroatomic substituents. We demonstrate that amination of alkynes bearing α-stereocenters occurs with retention of configuration at the newly-formed C–N bond. Competition experiments between alkynes, kinetic isotope effects, and DFT calculations are performed to confirm the mechanistic hypothesis that initial ene reaction of a selenium bis(imide) species is the rate- and product-determining step. This ene reaction has a transition state that results in substantial partial positive charge development at the carbon atom closer to the amination position. Inductive and/or hyperconjugative stabilization or destabilization of this positive charge explains the observed regioselectivities.Selenium catalysis enables a general intermolecular propargylic C–H amination of alkynes. The concerted mechanism gives rise to high regioselectivity for the more electron-rich end of the alkyne and retention of the C–H propargylic stereocenter. 相似文献
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