Regulation of nonadiabatic processes in the photolysis of some carbonyl compounds

Physical Chemistry Chemical Physics : PCCP
King-Chuen Lin

Abstract

Carbonyl compounds studied are confined to acetyl halide (CH3COCl), acetyl cyanide (CH3COCN), acetyl sulfide (CH3COSH), acetaldehyde (CH3CHO), and methyl formate (HCOOCH3). They are asymmetrically substituted, but do not follow the well-known Norrish type I reactions. Each compound ejected in an effusive beam at about 300 K is commonly excited to the (1)(n, π*)CO lower state; that is, a nonbonding electron on O of the C[double bond, length as m-dash]O group is promoted to the antibonding orbital of π*CO. The photolysis experiments are conducted in the presence of Ar gas and the corresponding fragments are detected using time-resolved Fourier-transform Infrared (FTIR) emission spectroscopy. The enhancement of the collision-induced internal conversion or intersystem crossing facilitates the dissociation channels via highly vibrational states of the ground singlet (So) or triplet (T1) potential energy surfaces. In this manner, an alternative nonadiabatic channel is likely to open yielding different products, even if the diabatic coupling strength is strong between the excited state and the neighboring state. For instance, the photodissociation of CH3COCl at 248 nm produces HCl, CO, and CH2 fragments, in contrast to the supersonic ...Continue Reading

References

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Jan 13, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Chia-Yun LiuKing-Chuen Lin
Mar 15, 2011·Physical Chemistry Chemical Physics : PCCP·Meng-Hsuan ChaoKing-Chuen Lin
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Mar 28, 2012·Physical Chemistry Chemical Physics : PCCP·L Rubio-LagoL Bañares
Mar 14, 2014·Physical Chemistry Chemical Physics : PCCP·King-Chuen Lin, Po-Yu Tsai

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Citations

Feb 18, 2016·The Journal of Physical Chemistry. a·Paul L HoustonJoel M Bowman
Mar 25, 2014·Journal of Magnetic Resonance·Mitsuhiro TakedaMasatsune Kainosho
Aug 20, 2016·Physical Chemistry Chemical Physics : PCCP·A B StephansenT I Sølling
Oct 6, 2017·Chemical Society Reviews·Joel M Bowman, Paul L Houston
Jul 12, 2017·Physical Chemistry Chemical Physics : PCCP·Yong-Chang HanKing-Chuen Lin

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