2015
DOI: 10.1103/physreva.91.031403
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Understanding the modulation mechanism in resonance-enhanced multiphoton probing of molecular dynamics

Abstract: Time-resolved spectroscopy on isolated molecules gives fundamental insight into the conversion of light energy to other degrees of freedom. Probing of the photoinduced dynamics can be accomplished by ionization, via a single-photon or multiphoton transition. In this Rapid Communication we directly contrast transient spectra on the molecule perylene obtained with multiphoton ionization (MPI) to single-photon ionization (SPI). The photoinduced nuclear geometry relaxation modulates the MPI transient with a decay … Show more

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Cited by 14 publications
(15 citation statements)
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“…Femtosecond laser pulses in this energy range can be obtained from high-order harmonic generation [20]. The related high probe-only background can be superimposed on the excited-state signal, leading to significant spectral distor-tions [19,20]. The presented Bayesian approach can be adapted to such experimental conditions and will lead to similar improvements as presented in the present work.…”
Section: Discussionmentioning
confidence: 96%
“…Femtosecond laser pulses in this energy range can be obtained from high-order harmonic generation [20]. The related high probe-only background can be superimposed on the excited-state signal, leading to significant spectral distor-tions [19,20]. The presented Bayesian approach can be adapted to such experimental conditions and will lead to similar improvements as presented in the present work.…”
Section: Discussionmentioning
confidence: 96%
“…eV probe [28], we find that WFI near threshold and SFI provide qualitatively similar results (see later), although only WFI can be compared quantitatively with calculations of the excited state dynamics. It can be shown analytically that the first-order one-photon ionization probability is directly proportional to the norm of the Dyson orbital formed by projecting the N-1 electron wave function of the final (ionic) state onto the N electron wave function of the initial (neutral) state of the molecule [29,30]:…”
Section: Fig 1 Cartoons Showing the Excited State Dynamics In A)mentioning
confidence: 52%
“…the difference in the measurements comes from the different sensitivities that WFI and SFI have to the excited state dynamics. We believe that this longer decay in the SFI CH 2 I 2 pumpprobe signal is due to a multiphoton resonance which enhances the ion yield as the molecule dissociates [19][20][21][22][23][24][25]28]. As the wavepacket dissociates on the neutral excited state, the molecular structure can be such that n-photons (n < IP/hν) from the strong field probe can come into resonance with an intermediate state, between the excited state and the continuum, increasing the ionization rate.…”
Section: Fig 1 Cartoons Showing the Excited State Dynamics In A)mentioning
confidence: 98%
“…However, the observed value of “n” is found to be 3 (Table 1), which indicates there are intermediates resonant states 64 in the photoionization process. These states could be valence or SAMO excited states because they both are optically active (Table 2) and can therefore be transiently populated during the pulse.…”
Section: Introductionmentioning
confidence: 97%