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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Primary Formation Dynamics of Peroxynitrite Following Photolysis of Nitrate
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Primary Formation Dynamics of Peroxynitrite Following Photolysis of Nitrate

机译：硝酸盐光解后过亚硝酸盐的初生动力学

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The photolysis of nitrate, in D20 solution has been investigated by femtosecond infrared spectroscopy.In accordance with previous investigations, we observe that the peroxynitrite ion, ON00-, is the dominantphotochemical product following the excitation of nitrate at 200 nm. Moreover, we are able to identify thecis/trans isomers of peroxynitrite and the dynamics of their formation in solution. We observe that the trans-ONOO~- isomer is formed directly and solely from the excited NO_3~- ion within the firsttwopicoseconds afterexcitation. Subsequently, about half of the trans-ONOO~- isomerizes to cis-ONOO~- in 25 ps; thereafter, theratio between the two isomers remains constant for the 300 ps duration of the experiment. The observedvibrational frequencies of the terminal O=N bonds are at 1515 and 1580 cm~(-1)fortrans-and cis-peroxynitrite,respectively. The detailed analysis of the infrared bands of cis- and trans-peroxynitrite is facilitated by electronicstructure calculations on the conformers in a cluster of 11 D_2Omolecules and by steady-state infraredspectroscopy of ONOO~- in D_2O.In addition to the formation of ONOO~-, experiments also reveal aslow-50 ps formation of NO_2following the photolysis of nitrate.
机译：飞秒红外光谱法研究了D20溶液中硝酸盐的光解作用。根据先前的研究，我们观察到在200 nm硝酸盐激发后，过氧亚硝酸盐离子ON00-是主要的光化学产物。此外，我们能够确定过氧亚硝酸盐的顺/反异构体及其在溶液中形成的动力学。我们观察到，反式-ONOO-异构体是在激发后的前两个皮秒内直接且仅由被激发的NO 3-离子形成的。随后，约有一半的反式-ONOO-在25 ps内异构化为顺式-ONOO-。此后，两个异构体之间的热值在实验的300 ps时间内保持恒定。对于反式和顺式过氧亚硝酸盐，观察到的末端O = N键的振动频率分别为1515和1580 cm〜（-1）。通过对11个D_2分子簇中的构象异构体进行电子结构计算，以及通过D_2O中ONOO〜-的稳态红外光谱，可以方便地详细分析顺式和反式过氧亚硝酸盐的红外波段。 ，实验还揭示了硝酸盐的光解后，NO_2的形成速率低至50 ps。

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