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Femtosecond energy- and angle-resolved photoelectron spectroscopy

Arasaki, Yasuki and Takatsuka, Kazuo and Wang, Kwanghsi and McKoy, Vincent (2000) Femtosecond energy- and angle-resolved photoelectron spectroscopy. Journal of Chemical Physics, 112 (20). pp. 8871-8884. ISSN 0021-9606.

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We present a formulation of energy- and angle-resolved photoelectron spectra for femtosecond pump–probe ionization of wave packets and results of its application to the ^1Σ^+_u double-minimum state of aligned Na_2. 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 pump–probe 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 molecule and polarization of the probe pulse are also seen to be potentially useful for real-time monitoring of molecular rotation.

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Additional Information:© 2000 American Institute of Physics. (Received 10 January 2000; accepted 28 February 2000) This work has been supported by a grant from the Ministry of Education, Science, and Culture (Japan), and the National Science Foundation (U.S.).
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Ministry of Education, Culture, Sports, Science and Technology (MEXT)UNSPECIFIED
Issue or Number:20
Record Number:CaltechAUTHORS:20151027-154130546
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Official Citation:Femtosecond energy- and angle-resolved photoelectron spectroscopy Arasaki, Yasuki and Takatsuka, Kazuo and Wang, Kwanghsi and McKoy, Vincent, The Journal of Chemical Physics, 112, 8871-8884 (2000), DOI:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:61611
Deposited By: George Porter
Deposited On:28 Oct 2015 15:06
Last Modified:03 Oct 2019 09:09

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