Observation of photochemical C-N bond cleavage in CH3N3: a new photochemical route to cyclic N3

The Journal of Physical Chemistry. a
Christopher LarsonAlec M Wodtke

Abstract

We report VUV-photoionization based photofragmentation-translational spectroscopy data, providing a comprehensive study of the collision free photochemistry of methyl azide (CH3N3) at 193 nm. We report the first observation of the production of methyl and the N3 radical and derive the translational energy release distribution of this reaction. The most probable translation energy is only 8%, and the maximum translational energy is only 60% of the available energy, taking CH3 + linear N3 as the zero of energy. However, the maximum translational energy release is quantitatively consistent with production of the higher energy isomer cyclic N3. Threshold photoionization of the N3 fragment using tunable synchrotron radiation shows results consistent with theoretical predictions of the cyclic N3 ionization potential. The secondary dissociation of N3 --> N(2D) + N2 is also observed and its translational energy release is derived. This distribution peaks at approximately 6 and extends to 11 kcal/mol as would be expected from the size of the exit channel barrier for spin-allowed dissociation of cyclic N3 (7 kcal/mol) and, furthermore, inconsistent with the barrier height of the spin-allowed dissociation of linear N3 (3 kcal/mol). A larg...Continue Reading

References

Apr 25, 2006·Physical Chemistry Chemical Physics : PCCP·Jianyang ZhangAlec M Wodtke
Jul 15, 2006·The Journal of Physical Chemistry. a·Ming-Liang Zhang, Eli Pollak
Aug 2, 2006·Physical Chemistry Chemical Physics : PCCP·Peter C SamartzisAlec M Wodtke
Feb 9, 2007·The Journal of Chemical Physics·Peter C SamartzisAlec M Wodtke
Jul 7, 2007·Physical Chemistry Chemical Physics : PCCP·Peter C Samartzis, Alec M Wodtke

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Citations

Dec 20, 2012·The Journal of Chemical Physics·B R L GalvãoA J C Varandas
Aug 24, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Yan Hong LiangQian Shu Li
Aug 16, 2017·The Journal of Chemical Physics·Alfredo Quinto-HernandezAlec M Wodtke
Jul 15, 2018·Scientific Reports·Yuanzheng ChenHui Wang
Oct 21, 2020·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Qingguo Feng
Sep 2, 2009·The Journal of Physical Chemistry. a·Lin JinYi-hong Ding
Sep 6, 2011·Journal of the American Chemical Society·Jien-Lian Chen, Wei-Ping Hu
Sep 21, 2011·The Journal of Physical Chemistry. a·B R L Galvão, A J C Varandas
Feb 11, 2015·The Journal of Physical Chemistry. B·U Geiger, Y Haas

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