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- W2038494691 abstract "We adopt the theory of intramolecular dynamics to explore charge separation and recombination in two classes of ‘isolated’ solvent-free molecular systems: (A) Supermolecules containing bridged electron donor and electron acceptor, where electron transfer occurs on a spatial scale of ≈︁ 10 Å. (B) Ultrahigh molecular Rydberg excitations with a principle quantum number n ≃ 50−300 and spatial dimensions of ≈︁ 104 Å, where relaxation processes, e.g., electron-core recombination via internal conversion or predissociation, and charge separation by autoionization, are manifested. The molecular limit for photoinduced long-range ET in isolated supermolecules [class (A)] is treated on the basis of the statistical limit for interstate radiationless transitions, which involve either a direct or a mode-selective mediated coupling. The level structure, optical excitation modes and dynamics of high molecular Rydbergs [class (B)] interrogated by time-resolved ZEKE (zero-electron kinetic energy) spectroscopy, are treated by the effective Hamiltonian formalism. We pursue the formal analogy between the coupling, accessibility and decay of ultrahigh Rydbergs in an external weak (F = 0.01−1.0 V/cm) electric field and intramolecular (interstate and intrastate) relaxation in a bound level structure. Model calculations for the field-induced (l) mixing reveal that the Rydberg dynamics is characterized by two distinct (≈︁ ns and ≈︁μs) time scales. Up to date, long time-resolved (10 μs − 100 ns time scales) nonexponential decay of ZEKE Rydbergs was experimentally documented, in accord with our analysis. The predicted existence of the short decay times (1 − 10 ns) was not yet subjected to an experimental test." @default.
- W2038494691 created "2016-06-24" @default.
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- W2038494691 date "1995-03-01" @default.
- W2038494691 modified "2023-09-23" @default.
- W2038494691 title "B. Electron Motion in Highly Excited States and Radiationless Transitions. General Dynamical Theory and Experiment. Intramolecular Dynamics and Charge Separation in Large Systems" @default.
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- W2038494691 doi "https://doi.org/10.1002/bbpc.19950990310" @default.
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