Dynamics of excess electron localization in liquid helium and neon

Michael Rosenblit, Joshua Jortner*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

48 Scopus citations

Abstract

In this paper, we address the relations between the structure, electronic level structure, energetics, and localization dynamics of an excess electron in a bubble in liquid 4He, 3He, and Ne. Our treatment of the dynamics of formation for the electron bubble rests on a quantum mechanical Wigner-Seitz description of the excess electron in conjunction with a hydrodynamic picture for the liquid. The dynamics of electron localization is described in terms of the initial formation of an incipient bubble of radius 3.3-3.5 Å followed by adiabatic bubble expansion in the ground electronic state. The hydrodynamic model for bubble expansion considers the expansion of a spherical cavity in an incompressible liquid with the energy dissipation being due to the emission of sound waves. This model predicts the bubble expansion time (τDb) in liquid 4He to be τDb = 8.5 ps at P = 0, exhibiting a marked pressure dependence (decreasing by a numerical factor of 4 at P = 16 atm) and revealing a small isotope effect of τDb(4He)/τD b(3He) = 0.83 in liquid 3He, while for liquid Ne, τDb ≅ 1 ps. The collapse times of the empty bubble formed by vertical photoionization of the electron bubble are τc = 19.8 ps for 4He and τc = 34 ps for 3He, with τc being considerably longer than τdb, reflecting the effect of the kinetic electron energy on the fast electron bubble expansion. The interrogation of the electron bubble localization dynamics by femtosecond absorption spectroscopy is explored by the analysis of the temporal evolution of the electronic excitation energies.

Original languageEnglish
Pages (from-to)751-757
Number of pages7
JournalJournal of Physical Chemistry A
Volume101
Issue number4
DOIs
StatePublished - 23 Jan 1997

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