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Bloch-Siegert effects in two-photon excitations: Fixed laser-molecule configurations versus orientational averaging
1Department of Chemistry, University of Western Ontario, London, Ontario N6A 5B7, Canada.
Abstract:
The two-level rotating wave approximation for two-photon excitations in dipolar molecules is modified to include the effects of the Bloch-Siegert shift in the two-photon resonance energy. The resulting analytical results are used to establish a criterion for when Bloch-Siegert effects are important and the relevance of these effects are compared for fixed laser-molecule configurations versus orientationally averaged results. Two-level model molecules, with parallel permanent and transition dipoles, are used in this work and the effects of Bloch-Siegert shifts are discussed for resonance profiles, time-dependent populations of the excited state, and time-averaged excitation rates. Bloch-Siegert shifts can have pronounced effects on resonance energies and the shape of resonance profiles and, for example, on the magnitudes and the temporal locations of the maxima in the temporal evolution of the time-dependent properties of the system.
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