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Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia

MPS-Authors
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Moshammer,  Robert
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Pfeifer,  Thomas
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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2012.15374.pdf
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Citation

Belsa, B., Amini, K., Liu, X., Sanchez, A., Steinle, T., Steinmetzer, J., et al. (2021). Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia. Structural Dynamics, 8(1): 014301. doi:10.1063/4.0000046.


Cite as: https://hdl.handle.net/21.11116/0000-0008-A3B6-2
Abstract
Visualizing molecular transformations in real-time requires a structural
retrieval method with {\AA}ngstr\"om spatial and femtosecond temporal atomic
resolution. Imaging of hydrogen-containing molecules additionally requires an
imaging method that is sensitive to the atomic positions of hydrogen nuclei,
with most methods possessing relatively low sensitivity to hydrogen scattering.
Laser-induced electron diffraction (LIED) is a table top technique that can
image ultrafast structural changes of gas-phase polyatomic molecules with
sub-{\AA}ngstr\"om and femtosecond spatiotemporal resolution together with
relatively high sensitivity to hydrogen scattering. Here, we image the umbrella
motion of an isolated ammonia molecule (NH$_3$) following its strong field
ionization. Upon ionization of a neutral ammonia molecule, the ammonia cation
(NH$_3^+$) undergoes an ultrafast geometrical transformation from a pyramidal
($\Phi_{HNH} = 107 ^\circ$) to planar ($\Phi_{HNH}=120^\circ$) structure in
approximately 8 femtoseconds. Using LIED, we retrieve a near-planar
($\Phi_{HNH}=117 \pm 5^\circ$) field-dressed NH$_3^+$ molecular structure
$7.8-9.8$ femtoseconds after ionization. Our measured field-dressed NH$_3^+$
structure is in excellent agreement with our calculated equilibrium field
dressed structure using quantum chemical ab initio calculations.