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Semiclassical many-mode Floquet theory. II. Non-linear multiphoton dynamics of a two-level system in a strong bichromatic field

Tak-San Ho and Shih-I Chu

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For pt.I see Chem. Phys. Lett. vol.96, p.464 (1983). The non-linear multiphoton excitation dynamics of two-level systems under the influence of two strong linearly polarised monochromatic fields is studied exactly for the first time along the semiclassical many-mode Floquet theory. The present approach relaxes the restrictions of the conventional generalised rotating-wave approximation (GRWA) and allows correct treatment of various non-linear features such as power broadening, resonance shift, asymmetry in absorption lineshape, etc. By extending the nearly degenerate perturbative method of Salwen (1955), approximate analytical expressions for transition probabilities are obtained for multiphoton resonance processes for which (n+1) photons of one field are absorbed, whereas n photons of the other field are emitted, where n is an arbitrary integer. Detailed comparison of the analytical, the GRWA and the numerically exact results is given. Also presented is a case study of the time evolution of spin 1/2 systems in multi-quantum NMR transitions driven by pulsed bichromatic radiofrequency fields.


PACS

31.15.xg Semiclassical methods

33.70.Jg Line and band widths, shapes, and shifts

33.70.Ca Oscillator and band strengths, lifetimes, transition moments, and Franck-Condon factors

33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states)

Subjects

Atomic and molecular physics

Computational physics

Dates

Issue 10 (28 May 1984)



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