The Photoelectron Angular Distribution as a Probe of Energetically Indistinguishable Channels in Photodetachment

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Radicals And Ions

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Photoelectron imaging measurements of I-\cdotCH3CN are presented from the lowest energy I(2P3/2)\cdotCH3CN channel threshold to 0.3 eV above the I(2P1/2)\cdotCH3CN threshold. Excitation of the cluster just below the latter threshold leads to competition between direct detachment and the production of a dipole-bound state [I(2P1/2)\cdotCH3CN]-. Subsequent relaxation of the I moiety (2P1/2→2P3/2) occurs via autodetachment of the dipole bound electron. However, the autodetached electrons are energetically equivalent to those directly detached via the 2P3/2 channel. While the photoelectron spectrum is insensitive to this phenomenon, the kinetic energy dependence of the photoelectron angular distribution (PAD) of the 2P3/2 channel reflects these dynamics. Dramatic changes are observed within a 100 meV window of the I(2P1/2)\cdotCH3CN threshold. Although previously unreported, further results are presented that show sharp changes in the PAD are relatively common in I-\cdotX cluster anions (X=polar molecule).

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