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Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle.

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Harding,  D. J.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Neugebohren,  J.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Grütter,  M.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Schmidt-May,  A. F.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Auerbach,  D. J.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Kitsopoulos,  T. N.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Wodtke,  A. M.
Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society;

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Citation

Harding, D. J., Neugebohren, J., Grütter, M., Schmidt-May, A. F., Auerbach, D. J., Kitsopoulos, T. N., et al. (2014). Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle. The Journal of Chemical Physics, 141(5): 054201. doi:10.1063/1.4891469.


Cite as: https://hdl.handle.net/11858/00-001M-0000-0023-C070-F
Abstract
We present a new photo-fragment imaging spectrometer, which employs a movable repeller in a single field imaging geometry. This innovation offers two principal advantages. First, the optimal fields for velocity mapping can easily be achieved even using a large molecular beam diameter (5 mm); the velocity resolution (better than 1%) is sufficient to easily resolve photo-electron recoil in (2 + 1) resonant enhanced multiphoton ionization of N2 photoproducts from N2O or from molecular beam cooled N2. Second, rapid changes between spatial imaging, velocity mapping, and slice imaging are straightforward. We demonstrate this technique's utility in a re-investigation of the photodissociation of N2O. Using a hot nozzle, we observe slice images that strongly depend on nozzle temperature. Our data indicate that in our hot nozzle expansion, only pure bending vibrations – (0, v 2, 0) – are populated, as vibrational excitation in pure stretching or bend-stretch combination modes are quenched via collisional near-resonant V-V energy transfer to the nearly degenerate bending states. We derive vibrationally state resolved absolute absorption cross-sections for (0, v 2 ≤ 7, 0). These results agree well with previous work at lower values of v2, both experimental and theoretical. The dissociation energy of N2O with respect to the O(1D) + N2 Σg+1 asymptote was determined to be 3.65 ± 0.02 eV.