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Femtosecond energy-and angle-resolved photoelectron spectroscopy Yasuki Arasaki and Kazuo Takatsukaa)

Summary: Femtosecond energy- and angle-resolved photoelectron spectroscopy
Yasuki Arasaki and Kazuo Takatsukaa)
Department of Basic Science, Graduate School of Arts and Sciences, University of Tokyo, Komaba,
153-8902, Tokyo, Japan
Kwanghsi Wang and Vincent McKoy
Laboratory for Molecular Sciences, California Institute of Technology, Pasadena, California 91125
Received 10 January 2000; accepted 28 February 2000
We present a formulation of energy- and angle-resolved photoelectron spectra for femtosecond
pump­probe ionization of wave packets and results of its application to the 1
u double-minimum
state of aligned Na2. The formulation is well-suited for inclusion of the underlying dynamics of
molecular photoionization and its dependence on molecular geometry. Results are presented for
three typical pump laser energies selected so as to investigate qualitatively different patterns of the
spatio-temporal propagation of wave packets on the double-minimum potential curve and of their
associated photoelectron spectra. Photoelectron angular distributions are also reported for different
orientations of linearly polarized pump and probe pulses. The resulting photoelectron spectra
illustrate the importance of a proper description of the underlying photoionization amplitudes and
their dependence on geometry for unraveling wave packet dynamics from pump­probe
photoelectron signals in nonadiabatic regions where the electronic structure evolves rapidly with
geometry. The dependence of these photoelectron angular distributions on relative orientation of the


Source: Arasaki, Yasuki - Department of Basic Science, University of Tokyo


Collections: Physics