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It has been shown by Heller that a nonstationary wave packet resulting from a Franck–Condon transition evolves on the potential energy surface of the final electronic state and propagates through phase space at a rate which can be determined from the autocorrelation function ↓C(t)↓2=↓〈(0)‖(t)〉↓2. Since C(t) can be obtained by Fourier transformation of an optical spectrum S(E), i.e., from an observable quantity, it is possible to derive from an experimental measurement information concerning the density operator of a so‐called dynamical statistical ensemble (DSE). This density operator, denoted ρav, represents a statistical mixture of the eigenstates of the system with weights determined by the dynamics of the system. It becomes diagonal after a so‐called break time TB. Its measure, according to a definition due to Stechel, can be interpreted as an effective number of states (denoted N) that significantly contribute to the dynamics. The break time TB represents the finite period of time allowed to expand i...

the journal of chemical physics

Intramolecular vibrational energy relaxation seen as expansion in phase space. I. Some experimental results for H2O+(X̃ 2B1), C2H+4(X̃ 2B3), and HCN+(B̃ 2∑+)