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Tunneling dynamics of the NH3(Ã) state observed by time-resolved photoelectron and H atom kinetic energy spectroscopies
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Yu, Hui, Evans, Nicholas L., Chatterley, Adam S., Roberts, Gareth M., Stavros, Vasilios G. and Ullrich, Susanne (2014) Tunneling dynamics of the NH3(Ã) state observed by time-resolved photoelectron and H atom kinetic energy spectroscopies. The Journal of Physical Chemistry A, Volume 118 (Number 40). pp. 9438-9444. doi:10.1021/jp507201a ISSN 1089-5639.
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Official URL: http://dx.doi.org/10.1021/jp507201a
Abstract
We have investigated the effects of quantum tunneling on the photodissociation dynamics of ammonia, following below and above barrier photoexcitation of low-lying levels of the ν2′ umbrella mode of the NH3 à state (NH3 (Ã)). This barrier separates the local minimum of the vertical Franck–Condon region from the NH3 (Ã)/NH3 (X̃) conical intersection (CI) which can be accessed along the N–H stretch coordinate. Two complementary techniques, time-resolved photoelectron spectroscopy (TR-PES) and time-resolved total kinetic energy release spectroscopy (TR-TKER), have been utilized to directly measure, for the first time, vibrational level dependent excited state lifetimes and N–H dissociation time scales as well as photoproduct final energy distributions. Interestingly, ν2′ even/odd dependencies are observed in the measured time constants and NH2 internal energy spectra, which are attributed to tunneling through a barrier, whose magnitude is dependent on the planarity of NH3 in the à state and direct versus indirect dissociation at the NH3 (Ã)/NH3 (X̃) conical intersection.
Item Type: | Journal Article | ||||
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||
Journal or Publication Title: | The Journal of Physical Chemistry A | ||||
Publisher: | American Chemical Society | ||||
ISSN: | 1089-5639 | ||||
Official Date: | 5 September 2014 | ||||
Dates: |
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Volume: | Volume 118 | ||||
Number: | Number 40 | ||||
Page Range: | pp. 9438-9444 | ||||
DOI: | 10.1021/jp507201a | ||||
Status: | Peer Reviewed | ||||
Publication Status: | Published | ||||
Access rights to Published version: | Restricted or Subscription Access |
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