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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Vibrational Modes of the Vinyl and Deuterated Vinyl Radicals
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Vibrational Modes of the Vinyl and Deuterated Vinyl Radicals

机译：乙烯基和氘代乙烯基自由基的振动模式

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Following the initial report of the detection of fundamental transitions of all nine vibrational modes of thevinyl radical [Letendre, L.; Liu, D.-K.; Pibel, C. D.; Halpern, J. B.; Dai, H.-L. J. Chem. Phys. 2000, 112,9209] by time-resolved IR emission spectroscopy, we have re-examined the assignments of the vibrationalmodes through isotope substitution. Precursor molecules vinyl chloride-d_3, vinyl bromide-d_and 1,3-butadiene-d_6 are used for generating vibrationally excited vinyl-d_3through 193 nm photolysis. The nondeuterated versionsof these molecules along with vinyl iodide and methyl vinyl ketone are used as precursors for the productionof vinyl-h_3. IR emission following the 193 nm photolysis laser pulse is recorded with nanosecond time and～8 cm~(-1)frequency resolution. A room-temperature acetylene gas cell is used as a filter to remove thefundamental transitions of acetylene, a photolysis product, in order to reduce the complexity of the emissionspectra. Two-dimensional cross-spectra correlation analysis is used to identify the emission bands from thesame emitting species and improve the S/Nof the emission spectra. Isotope substitution allows the identificationof several low-frequency vibrational modes. For C_2H_3, the assigned modes are thev_4(CC stretch) at 1595,v_5(2symmetric 1401,6(2asymmetric + α-CH bend) at 1074, v_8 (CH_2+ symmetricout-of-plane (oop) bend) at 944, and v_9(CH_2+ α-CH asymmetric oop bend) at 897 cm~(-1). For C_2D_3, themodes are the v_5(CD_2symmetric bend) at 1060, v_6 (2asymmetric + α-CD 820, and 8(2 α-CD symmetric oop bend) at 728 cm~(-1).
机译：在有关检测乙烯基自由基的所有九种振动模式的基本转变的初步报告之后[Letendre，L .; Liu D.-K .; Pibel，C。D .; Halpern，J. B .;戴慧玲J.化学物理2000，112,9209]通过时间分辨红外发射光谱学，我们已经通过同位素置换重新检查了振动模态的分配。前体分子氯乙烯-d_3，溴乙烯-d_和1,3-丁二烯-d_6用于通过193 nm光解产生振动激发的乙烯基-d_3。这些分子的非氘代形式与碘乙烯和甲基乙烯基酮一起被用作生产乙烯基-h_3的前体。记录193 nm光解激光脉冲后的IR发射，时间为纳秒，频率分辨率约为8 cm〜（-1）。室温乙炔气室用作过滤器，以去除乙炔（一种光解产物）的基本转变，以降低发射光谱的复杂性。二维互谱相关分析用于识别相同发射物种的发射带，并提高发射光谱的信噪比。同位素替代可以识别几种低频振动模式。对于C_2H_3，分配的模式为1595处的v_4（CC拉伸），v_5（1074处的2对称1401、6（2不对称+α-CH弯曲），v_8（CH_2 +对称面外（oop）弯曲）和944_v （CH_2 +α-CH不对称弯头）在897 cm〜（-1）。对于C_2D_3，模式为1060的v_5（CD_2对称弯头），v_6（2个不对称+α-CD820和8（2α-CD对称弯头）弯曲）在728厘米〜（-1）处。

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