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Spectral dependence of photoemission in multiphoton ionization of NO 2 by femtosecond pulses in the 375-430 nm range
Ist Teil von
Physical chemistry chemical physics : PCCP, 2017-08, Vol.19 (33), p.21996-22007
Ort / Verlag
England: Royal Society of Chemistry
Erscheinungsjahr
2017
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
We investigate the multiphoton ionization of NO
using tunable (430-375 nm) femtosecond pulses and photoelectron-photoion coincidence momentum spectroscopy. In order to understand the complex electronic and nuclear photodynamics at play following absorption of three to five photons, we also report extended photoionization calculations using correlated targets and coupled channels. Exploring the multiphoton dissociative ionization (MPDI) and multiphoton ionization (MPI) processes over such a broad energy range enables us to lend further support to our work carried out around 400 nm of a femtosecond laser [S. Marggi Poullain et al., J. Phys. B: At., Mol. Opt. Phys., 2014, 47, 124024]. Two excitation energy regions are identified and discussed in terms of the proposed reaction pathways, highlighting the significant role of Rydberg states, such as the [R*(6a
)
, 3pσ] Rydberg state, in the NO
multiphoton excitation and photoionization. These new results support our previous assumption that different bent and linear geometries of the NO
(X
Σ
) ionic state contribute to the MPDI and MPI, consistent with the reported calculations which reveal an important vibronic coupling characterizing the photoemission. Remarkably, the strong anisotropy of the recoil frame photoelectron angular distribution (RFPAD) previously observed at 400 nm appears as a fingerprint across the whole explored photon energy range.