Fleisher Adam J, Bjork Bryce J, Bui Thinh Q, Cossel Kevin C, Okumura Mitchio, Ye Jun
†JILA, National Institute of Standards and Technology and University of Colorado, Department of Physics, 440 UCB, Boulder, Colorado 80309, United States.
‡Material Measurement Laboratory, National Institute of Standards and Technology, 100 Bureau Drive, Gaithersburg, Maryland 20899, United States.
J Phys Chem Lett. 2014 Jul 3;5(13):2241-6. doi: 10.1021/jz5008559. Epub 2014 Jun 16.
We demonstrate time-resolved frequency comb spectroscopy (TRFCS), a new broadband absorption spectroscopy technique for the study of trace free radicals on the microsecond timescale. We apply TRFCS to study the time-resolved, mid-infrared absorption of the deuterated hydroxyformyl radical trans-DOCO, an important short-lived intermediate along the OD + CO reaction path. Directly after photolysis of the chemical precursor acrylic acid-d1, we measure absolute trans-DOCO product concentrations with a sensitivity of 5 × 10(10) cm(-3) and observe its subsequent loss with a time resolution of 25 μs. The multiplexed nature of TRFCS allows us to detect simultaneously the time-dependent concentration of several other photoproducts and thus unravel primary and secondary chemical reaction pathways.
我们展示了时间分辨频率梳光谱技术（TRFCS），这是一种用于在微秒时间尺度上研究痕量自由基的新型宽带吸收光谱技术。我们应用TRFCS来研究氘代羟基甲酰基自由基反式-DOCO的时间分辨中红外吸收，反式-DOCO是OD + CO反应路径上一种重要的短寿命中间体。在化学前驱体丙烯酸-d1光解后，我们以5×10(10) cm(-3) 的灵敏度测量反式-DOCO产物的绝对浓度，并以25 μs的时间分辨率观察其随后的损耗。TRFCS的多路复用特性使我们能够同时检测其他几种光产物随时间变化的浓度，从而揭示一级和二级化学反应路径。
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