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Physical Review A

Overtone absorption in a two-overtone frequency field

Munir Hasan Nayfeh, J. M. Shobaki

Published Jul 1, 1984• 3 citations
Publisher

Abstract

We examine the third-overtone absorption of diatomic molecules in the presence of a tunable field in near-third-overtone resonance using a one-dimensional anharmonic-oscillator model. We find that the tunable mode causes modulation of the absorption as a result of an intensity-induced quenching effect. At high intensities the absorption diminishes accompanied with the disappearance of the modulation. Our investigations also show that these effects are insensitive to the dephasing of the interaction.

DOI
10.1103/physreva.30.295

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•Jan 1, 1998•0 citations
We examine the third-overtone absorption of diatomic molecules in the presence of a tunable field in near-third-overtone resonance using a one-dimensional anharmonic-oscillator model. We find that the tunable mode causes modulation of the absorption as a result of an intensity-induced quenching effect. At high intensities the absorption diminishes accompanied with the disappearance of the modulation. Our investigations also show that these effects are insensitive to the dephasing of the interaction.
We demonstrate that vibrational overtone (second-harmonic) absorption must be treated as a resonance in the presence of vibrational two-exciton band excitations, as outlined earlier by two of us (T.H. and R.O.) in a manuscript with Luiz C. Scavarda do Carmo and Fritz L\"uty. Explicit calculations are made for a three-dimensional body-centered cubic and a one-dimensional lattice. The behavior of the position and intensity of the overtone absorption with exciton bandwidth and vibrational anharmonicity is studied in detail. Substantial cooperative vibrational absorption intensity is seen to be inconsistent with significant overtone splitting on the scale of the cooperative vibrational absorption bandwidth. Because no extrinsic impurity is required to provide a matrix element for two-exciton absorption, we suggest that the exciton band absorption associated with overtone absorption may be a very clean technique to observe exciton dispersion in solids.
Resonant interactions of a coherent field with an anharmonic oscillator are classified based on the established analogy with multiphoton interactions of light with atoms. It is shown that interference interactions in which the absorption of a single coherent field quantum induces a multiphoton transition in the anharmonic oscillator are superpositions of resonances of the “cascade” and “lambda-V” types, and a general description of these resonances is given. For the third- and fourth-order nonlinearities, the general expressions are applicable to a resonant process with the absorption of a single photon and the double excitation of the oscillator. Resonant processes of the second harmonic generation and “rectification” of radiation are predicted and described; experimental investigation of these processes will provide information about anharmonicity parameters in the proposed model.
Infrared (ir) radio-frequency (rf) double-resonance spectroscopy was carried out on the vibrational-overtone band of methyl iodide molecules (CH3I). An optical Fabry-Perot cavity was employed as an absorption cell to record saturated ir spectral lines even by a small-power extended-cavity diode laser with a high sensitivity and a wide tunability in the presence of a rf field. These features allowed investigation of molecules strongly coupled with monochromatic and bichromatic rf fields, or dressed molecules, at various rf power levels and detuning frequencies for a variety of ir and rf transitions. At appropriate energy-level schemes, quantum-interference effects were observed. All resultant spectra showed good agreement with dressed-state theoretical calculations, indicating that the present spectrometer is valid for precise investigation of dressed molecules.
We have investigated the interaction between bichromatic optical fields and atomic transitions. We have considered both the interaction of a saturating bichromatic field in the form of a 100% amplitude-modulated field resonantly interacting with a single atomic transition as well as the interaction of a pair of 100% amplitude-modulated fields with two coupled atomic transitions. In our studies of a single atomic transition resonantly excited by a 100% amplitude-modulated field we have used a fully quantum-electrodynamical analysis to model the Autler-Townes effect induced by a bichromatic optical field. We find that the effect induced by a bichromatic field is markedly different from the effect produced by a monochromatic exciting field. We have derived analytic expressions for the bichromatic Autler-Townes absorption spectrum. The absorption spectrum consists of equally spaced lines spaced by the modulation frequency. The linewidths of neighboring lines alternate as functions of the field strength. Experimentally, we observed this spectrum for both resonant and detuned 100% amplitude-modulated driving fields by monitoring the absorption of a weak monochromatic field as it was tuned about the resonance frequency of the 3²P₃/₂(F = 3, mF = 3) ↔ 4²D₅/₂(F = 4, mF = 4) transition while driving the 3²S₁/₂(F = 2, mF = 2) ↔ 3²P₃/₂(F = 3, mF = 3) transition with a saturating 100% amplitude-modulated field. We found excellent agreement between our predicted and measured spectra. We then investigated the resonant interaction between a pair of 100% amplitude-modulated fields and two atomic transitions sharing a common atomic level. We considered both a three-level atomic cascade system and a three-level atomic lambda system. We examined the effect that the relative phase between the two modulations has on the rate at which the modulated fields are absorbed. We find that the saturated time-averaged field absorption exhibits parametric resonances in both the cascade and lambda systems. The time-averaged absorption is strongly dependent upon the relative phase of modulation between the two fields and for certain phase differences the time-averaged absorption can be enhanced over the maximum saturated absorption experienced by cw fields of the same time-averaged intensities. We also find that the stationary atomic response exhibits periodic oscillations and for the cascade system periodic two-photon inversions of up to 40% can be achieved. We further find dark absorption resonances as a function of phase in the lambda system. We analyze the results from the point of view of semi-classical adiabatic dressed states.