TY - JOUR
T1 - N 1s photoelectron angular distributions from fixed-in-space NO2 molecules
T2 - Stereodynamics and symmetry considerations
AU - Yamazaki, Masakazu
AU - Adachi, Jun Ichi
AU - Kimura, Yasuyuki
AU - Stener, Mauro
AU - Decleva, Piero
AU - Yagishita, Akira
N1 - Funding Information:
The present work was supported by a Grant-in-Aid for Scientific Research from the Japanese Ministry of Education, Culture, Sports, Science and Technology. This work was partly supported by Grant-in-Aid for JSPS Fellows (No. 18•01229) from Japan Society for the Promotion of Science (JSPS). The experiments have been performed under the approval of the Photon Factory Program Advisory Committee (Project Nos. 2007G550 and 2009G560). M.Y. is grateful for the support by the JSPS Research Fellowships for Young Scientists.
PY - 2010/10/28
Y1 - 2010/10/28
N2 - Angular distributions of N 1s photoelectrons from fixed-in-space NO 2 molecules have been measured over the energy region of shape resonance and above. A multiple-coincidence velocity-map imaging technique for observation of molecular frame photoelectron angular distributions (MF-PADs) has been extended to nonlinear molecular targets. Density functional theory calculations have also been conducted to elucidate the photoionization dynamics and shape resonance in the N 1s photoionization of NO2. Results show that the N 1s MF-PADs exhibit strong shape variation as a function of both photoelectron kinetic energy and symmetries of final states, whereas asymmetry parameters of laboratory frame PADs show a local minimum around the shape resonance region and increase monotonically as the photon energy increases. Over the shape resonance, the spatial shape of the photoelectron wave function with b2 -symmetry closely resembles that of 5 b2 unoccupied molecular orbital of NO2, although the MF-PAD pattern for b2 -symmetry does not correspond directly to the 5 b2 orbital shape. At higher kinetic energy of 90 eV, MF-PADs become less structured, but still show a significant dependence on the symmetry of final states.
AB - Angular distributions of N 1s photoelectrons from fixed-in-space NO 2 molecules have been measured over the energy region of shape resonance and above. A multiple-coincidence velocity-map imaging technique for observation of molecular frame photoelectron angular distributions (MF-PADs) has been extended to nonlinear molecular targets. Density functional theory calculations have also been conducted to elucidate the photoionization dynamics and shape resonance in the N 1s photoionization of NO2. Results show that the N 1s MF-PADs exhibit strong shape variation as a function of both photoelectron kinetic energy and symmetries of final states, whereas asymmetry parameters of laboratory frame PADs show a local minimum around the shape resonance region and increase monotonically as the photon energy increases. Over the shape resonance, the spatial shape of the photoelectron wave function with b2 -symmetry closely resembles that of 5 b2 unoccupied molecular orbital of NO2, although the MF-PAD pattern for b2 -symmetry does not correspond directly to the 5 b2 orbital shape. At higher kinetic energy of 90 eV, MF-PADs become less structured, but still show a significant dependence on the symmetry of final states.
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U2 - 10.1063/1.3505549
DO - 10.1063/1.3505549
M3 - Article
C2 - 21033782
AN - SCOPUS:78149389182
VL - 133
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 16
M1 - 164301
ER -