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Physical Review Letters

Observation of Two-Photon Optical Nutation and Free-Induction Decay

M. M. T. Loy

Published Jun 14, 1976• 79 citations
Publisher

Abstract

The observation of two-photon optical nutation and free-induction decay is reported. The experimental result, on a two-photon transition in N${\mathrm{H}}_{3}$ with all relevant parameters known, is shown to be in quantitative agreement with the prediction of the two-photon vector model.

DOI
10.1103/physrevlett.36.1454

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Optics Letters•Nov 1, 1978•7 citations
The observation of two-photon optical nutation and free-induction decay is reported. The experimental result, on a two-photon transition in NH3{\mathrm{H}}_{3}H3​ with all relevant parameters known, is shown to be in quantitative agreement with the prediction of the two-photon vector model.
The Stark-pulse technique of Brewer and Shoemaker allows one to observe phenomena such as optical free-induction decay, optical nutation, and two-photon superradiance. In this paper, we develop a theoretical treatment of these phenomena under the appropriate experimental conditions. The calculations of the free-induction decay and the corresponding optical nutation are shown to be in excellent agreement with experiment. We also discuss the two-photon superradiance phenomenon of Brewer and Shoemaker as a Raman effect appearing in first-order perturbation theory. The analysis illustrates the essential features of the experimental observation.
We present solutions for two-photon optical transients from a three-level system which include the effects of (a) direct spontaneous emission to and from the nonresonant intermediate state and (b) phase-interrupting collisions. These effects are, in general, expected to be important for electronic transitions in the visible or ultraviolet region relevant for many two-photon transient experiments on free atoms. The steady-state absorption profile shows power narrowing and desaturation due to spontaneous relaxation. The two-photon delayed optical nutation signal is obtained explicitly. A perturbative calculation of optical nutation shows intensity-dependent damping. We find that for a particular case, namely, when the upper level spontaneous decay rate is twice that of the intermediate level, transient signals have especially simple forms and can be usefully employed for experimental determination of decay constants. The paper is a direct but nontrivial generalization of Schenzle and Brewer's corresponding investigation on one-photon transients.
Density matrix formalism is used to model two-photon free-induction decay from a ladder-type, three-level scheme with a resonant intermediate state. Counterpropagating light beams are assumed. Only the upper transition is frequency shifted out of resonance with the injected field. Results indicate departure from single-photon behavior; in particular, there is a π phase shift in the oscillations when the Rabi frequencies associated with each transition are comparable in magnitude. The theory is applied to the 32S1/2 (F = 1) − 32P1/2 − 42D3/2 excitation scheme of sodium.