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Optics and Spectroscopy

Resonance Frequency Shift in Two-Photon Transitions

N. D. Voropaev, А. Н. Ораевский

Published Dec 1, 1968• 0 citations
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The interaction of a four-level atomic system with two electromagnetic radiations has been studied. The two intermediate levels are closely spaced such that a single radiation frequency can induce transitions from the ground state to both of them. In a cascade-type double resonance, the pump electric-field amplitude is much stronger than the amplitude of the signal field, which can induce transitions from both of the intermediate levels to the upper state. The 15 optical Bloch equations obtained from the Liouville equations are solved analytically to obtain the Doppler-free signal line shape. The computed signals, exhibiting two Lorentzian line profiles, are presented for different pump frequencies. In addition to these one-photon transitions, we obtain a weak two-photon resonance peak. The two-photon resonance becomes weaker when the detuning of the pump frequency from a resonance frequency is increased. When the pump frequency ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$ is intermediate between the pump resonance frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, the two-photon resonance is very weak and almost vanishes when ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$=(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$)/2. When the pump frequency is on resonance with one of the transition frequencies, the Rabi splitting of the signal shows asymmetry because of the presence of a close-lying transition which is pumped off resonance. The intensity-dependent shifts of the transitions are such that they repel each other more and more as the intensity of the pump field is increased. These shifts arise from the nonresonant interaction between the atom and the field.
We investigate the phenomenon that a Berry phase evolving linearly in time induces a frequency shift of the resonance transition between two eigenstates, regardless of whether or not they are superposed. Using the magnetic-field-insensitive two-photon microwave---radio-frequency transition, which is free of any other dynamical frequency shift, we demonstrate that the frequency shift caused by a uniform rotation of the magnetic field corresponds to the derivative of the Berry phase with respect to time and depends on the direction of rotation of the magnetic field.