Advances in Chemical Physics, Vol. 74 by Ilya Prigogine, Stuart A. Rice

By Ilya Prigogine, Stuart A. Rice

This precious sequence is dedicated to supporting the reader receive basic information regarding a wide selection of subject matters in chemical physics, which box the editors interpret very commonly. Their rationale is to have specialists current finished analyses of topics of curiosity and to motivate the expression of person issues of view.

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1. The Vibron Model a. Molecular Vibronic States. In Fig. 2, the nuclear potentials for the ground and the excited states are different. For the normal coordinate Q, let us denote by xL0) and x:) the vibrational states in the ground and the excited electronic states, with n and m quanta of vibration, respectively. 35) In the crude Born-Oppenheimer approximations, the oscillator strength of the 0-n vibronic transition is proportional to (F;)’. Furthermore, the FranckCondon factor is analytically calculated in the harmonic approximation.

32) where b + b' is given its classical significance. 33) This problem is that of diagonal disorder (see Section IV). 34) Applying the results of Section IV,we find the two well-known limit results: At high temperature, A >> B, the excitonic coherence is thermalized; the lattice is an assembly of incoherent molecules with a response consisting of localized excitations with gaussian shape. C)in terms of the absorption of excitonic states, momentarily trapped in a lattice thermal fluctuation, when local interactions are not strong enough to create self-trapped excitons.

Raman resonant scattering or vibron fission), necessitate the explicit treatment of the molecular and lattice vibrations. In compact molecular crystals, such as anthracene, it is possible to distinguish lattice modes, with block motion of many molecules as a solid, from intramolecular modes, the vibrational excitons,’ whose motion is essentially intramolecular but in phase. In what follows, we call them phonons and vibrations, respectively. In the study of the coupling to the lattice, we have to consider an initial thermal population of phonons, while for our usual SURFACE AND BULK SPECTROSCOPY OF A MOLECULAR CRYSTAL 35 temperatures (kT

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