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Physical Review A

Recoil-induced resonances in nonlinear spectroscopy

Jingzhong Guo, P. R. Berman, B. Dubetsky, G. Grynberg

Published Aug 1, 1992• 129 citations
Publisher

Abstract

It is shown that, as a result of the atomic recoil associated with the absorption and emission of radiation, resonances can appear in nonlinear spectroscopy. The theory is illustrated by calculating the line shapes associated with nearly degenerate four-wave mixing and pump-probe spectroscopy when laser fields interact with an ensemble of two-level atoms. The recoil-induced resonances should be observable for atoms cooled below the Doppler limit of laser cooling, and the line shapes may provide a means for measuring the velocity distribution of these cooled atoms.

DOI
10.1103/physreva.46.1426

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It is shown that, as a result of the atomic recoil associated with the absorption and emission of radiation, resonances can appear in nonlinear spectroscopy. The theory is illustrated by calculating the line shapes associated with nearly degenerate four-wave mixing and pump-probe spectroscopy when laser fields interact with an ensemble of two-level atoms. The recoil-induced resonances should be observable for atoms cooled below the Doppler limit of laser cooling, and the line shapes may provide a means for measuring the velocity distribution of these cooled atoms.
A theory of pump-probe spectroscopy is developed in which optical fields drive two-photon Raman transitions between ground states of an ensemble of three-level atoms. Effects related to the recoil the atoms undergo as a result of their interactions with the fields are fully accounted for in this theory. The linear absorption coefficient of a weak probe field in the presence of two pump fields of arbitrary strength is calculated. For subrecoil cooled atoms, the spectrum consists of eight absorption lines and eight emission lines. In the limit that ${\ensuremath{\chi}}_{1}\ensuremath{\ll}{\ensuremath{\chi}}_{2},$ where ${\ensuremath{\chi}}_{1}$ and ${\ensuremath{\chi}}_{2}$ are the Rabi frequencies of the two pump fields, one recovers the absorption spectrum for a probe field interacting with an effective two-level atom in the presence of a single pump field. However, when ${\ensuremath{\chi}}_{1}\ensuremath{\gtrsim}{\ensuremath{\chi}}_{2},$ new interference effects arise that allow one to selectively turn on and off some of these recoil-induced resonances.
Theoretical calculations are presented for the probe absorption spectra of atoms having magnetically degenerate ground states which are subjected to weak pump fields that produce spatial polarization gradients. Apart from the Raman resonance contribution to the spectrum which has been observed experimentally, we predict that additional resonant structures should appear as a result of the atomic recoil that occurs during the absorption or emission of radiation by the atoms. The width of the atomic recoil resonances is directly related to the Doppler width associated with the driven transition. For sub-Doppler cooled atoms, the width can be much narrower than the optical pumping rate that determines the width of the Raman signal.
Recoil-induced resonances (RIR) can be detected in experiments involving light-atom interaction where atomic external degrees of freedom play an important role. In pump-probe experiments the recoil of atoms due to absorption and emission of radiation is responsible for the amplification and attenuation of the probe beam under certain circumstances, resulting in a disperse and narrow (of the order of 10 kHz) feature in the spectrum of the probe beam. Backward four-wave mixing (BFWM) signals, via recoil-induced resonances, using cold atoms as nonlinear medium were also extensively studied during the past years. In this work it will be presented a systematic study of forward four-wave mixing (FFWM) via RIR. It will be also presented a simple theoretical model that allowed us to predict the lineshapes of the observed signals and to better understand the phenomenon studied. The model is also compared with results that are already known in order to verify its validity and predict the possibility of measure the velocity distribution of the atomic cloud in a future experiment.
When a pump field and probe field simultaneously drive an electronic-state atomic transition, the probe field absorption spectrum can consist of an absorption peak centered near \ensuremath{\Delta}'=0 and amplification peak centered near \ensuremath{\Delta}'=2\ensuremath{\Delta} (\ensuremath{\Delta} and \ensuremath{\Delta}' are the pump and probe field detunings from the atomic transition frequency, respectively). This type of spectrum is seen in the limit \ensuremath{\Vert}\ensuremath{\Delta}\ensuremath{\Vert}\ensuremath{\gg}\ensuremath{\chi}\ensuremath{\gg}\ensuremath{\Gamma}, where \ensuremath{\chi} is the Rabi frequency associated with the pump field and 2\ensuremath{\Gamma} is the homogeneous width associated with the atomic transition. For atoms cooled below the recoil limit of laser cooling, the qualitative nature of the probe absorption spectrum can undergo a dramatic change. Provided that the recoil splitting ${\mathrm{\ensuremath{\omega}}}_{\mathit{k}}$ is larger than the homogeneous decay rate (as might occur in the case of a forbidden transition), the absorption and amplification features each split into an absorption-amplification doublet. In addition, structure is found in the probe absorption spectrum near \ensuremath{\Delta}'=\ensuremath{\Delta}; this structure consists of two absorption-amplification doublets. Both doublets can be resolved if ${\mathrm{\ensuremath{\omega}}}_{\mathit{k}}$>\ensuremath{\Gamma}. If ${\mathrm{\ensuremath{\omega}}}_{\mathit{k}}$, one of the doublets can be resolved provided that ${\mathrm{\ensuremath{\omega}}}_{\mathit{k}}$>${\mathrm{\ensuremath{\Gamma}}}_{\mathit{A}}$, where ${\mathrm{\ensuremath{\Gamma}}}_{\mathit{A}}$ is some effective atomic ground state width in the problem. The positions, widths, and relative weights of all the components are readily predicted using a dressed-atom theory in which quantization of the center-of-mass momentum is included. An analytical expression for the probe field spectrum is obtained for a simple case in which spontaneous decay to the lower level is neglected. Validity criteria for the results are discussed.
The review systematizes the experimental material and reports the fundamental theoretical results on the study of nonlinear resonance effects in spectra of atomic systems situated in the radiation field of lasers. The theoretical part explains the topics of greatest importance and significance for understanding of the experimental studies: the Stark effect in an optical field; the nonequilibrium velocity distribution of the atoms; the shape of the spectral line for a transition adjacent to a transition combining with a strong field; the simultaneous manifestation of the Stark effect and of Doppler broadening in the form of a very sharp structure on the line contour; a brief mention of the influence of collisions, recoil, and other factors on the sharp structure in spectra. The experimental part reports the results of experiments on the observation of the Stark effect in the optical region of the spectrum, the fine structure of the profile of a Doppler-broadened line and its properties, namely the dependence on the observation direction, the anisotropy in the field of a standing wave, the polarization properties, etc. in spectra of spontaneous or stimulated emission, absorption, and generation.