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Physical Review A

Recoil-induced resonances in pump-probe spectroscopy

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

Published May 1, 1995• 13 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.51.3947

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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 \ensuremathωk{\mathrm{\ensuremath{\omega}}}_{\mathit{k}}\ensuremathωk​ 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 \ensuremathωk{\mathrm{\ensuremath{\omega}}}_{\mathit{k}}\ensuremathωk​>\ensuremath{\Gamma}. If \ensuremathωk{\mathrm{\ensuremath{\omega}}}_{\mathit{k}}\ensuremathωk​, one of the doublets can be resolved provided that \ensuremathωk{\mathrm{\ensuremath{\omega}}}_{\mathit{k}}\ensuremathωk​>\ensuremathΓA{\mathrm{\ensuremath{\Gamma}}}_{\mathit{A}}\ensuremathΓA​, where \ensuremathΓA{\mathrm{\ensuremath{\Gamma}}}_{\mathit{A}}\ensuremathΓA​ 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.
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.
We analyze the fluorescence and absorption spectra of a two-level atom driven by a bichromatic field with frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, separated by ${\mathrm{\ensuremath{\omega}}}_{2}$-${\mathrm{\ensuremath{\omega}}}_{1}$=2\ensuremath{\delta}, and Rabi frequencies (at resonance) 2${\mathrm{\ensuremath{\Omega}}}_{1}$ and 2${\mathrm{\ensuremath{\Omega}}}_{2}$ such that their ratio \ensuremath{\alpha}=${\mathrm{\ensuremath{\Omega}}}_{2}$/${\mathrm{\ensuremath{\Omega}}}_{1}$1. We focus on the case of ${\mathrm{\ensuremath{\omega}}}_{1}$ close to the atomic frequency ${\mathrm{\ensuremath{\omega}}}_{0}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$ near the Rabi sideband frequency ${\mathrm{\ensuremath{\omega}}}_{1}$+2${\mathrm{\ensuremath{\Omega}}}_{1}$; the detunings are denoted by ${\mathrm{\ensuremath{\Delta}}}_{1}$=${\mathrm{\ensuremath{\omega}}}_{0}$-${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\Delta}}}_{2}$=${\mathrm{\ensuremath{\omega}}}_{1}$+2${\mathrm{\ensuremath{\Omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$. We find that the spectra depend critically on the detuning ${\mathrm{\ensuremath{\Delta}}}_{2}$: For large ${\mathrm{\ensuremath{\Delta}}}_{2}$, the fluorescence spectrum consists of the well known Mollow triplet, centered at ${\mathrm{\ensuremath{\omega}}}_{1}$; for smaller (but nonzero) ${\mathrm{\ensuremath{\Delta}}}_{2}$, the spectrum is composed of a triplet at ${\mathrm{\ensuremath{\omega}}}_{1}$ together with doublets near the sideband frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2${\mathrm{\ensuremath{\Omega}}}_{1}$. However, when ${\mathrm{\ensuremath{\Delta}}}_{2}$=0 (and \ensuremath{\alpha}\ensuremath{\ll}1), the spectrum consists of a doublet centered at ${\mathrm{\ensuremath{\omega}}}_{1}$ and triplets at ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2${\mathrm{\ensuremath{\Omega}}}_{1}$: there is then no fluorescence at ${\mathrm{\ensuremath{\omega}}}_{1}$. As \ensuremath{\alpha} increases, additional triplet structures appear in the spectrum at frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2n${\mathrm{\ensuremath{\Omega}}}_{1}$ with intensities proportional to ${\mathrm{\ensuremath{\alpha}}}^{2(\mathit{n}\mathrm{\ensuremath{-}}1)}$, n\ensuremath{\gtrsim}1, and a line reappears at ${\mathrm{\ensuremath{\omega}}}_{1}$, with intensity proportional to ${\mathrm{\ensuremath{\alpha}}}^{4}$. The absorption by the system of a weak probe beam is also strongly dependent on the detuning, and the spectrum is composed of emission-dispersion-absorption features located near ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{1}$\ifmmode\pm\else\textpm\fi{}2n${\mathrm{\ensuremath{\Omega}}}_{1}$. An analysis in the dressed-atom picture is presented which explains the physical origin of all these features, in both fluorescence and absorption. \textcopyright{} 1996 The American Physical Society.
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.
A theory of pump-probe spectroscopy is developed in which optical fields drive two-quantum, Raman-like transitions between ground-state sublevels. Three fields are incident on an ensemble of atoms. Two of the fields act as the pump field for the two-quantum transitions. The absorption or gain of an additional probe field is monitored as a function of its detuning from one of the fields which constitutes the pump field. Although the probe absorption spectrum displays features common to those found in pump-probe spectroscopy of single-quantum transitions, new interference effects are found to modify the spectrum. Many of these features can be explained within the context of a dressed-atom picture.
We examine the radiative properties of a two-level atom driven by a strong bichromatic field with frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$=${\mathrm{\ensuremath{\omega}}}_{0}$-${\mathrm{\ensuremath{\delta}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$=${\mathrm{\ensuremath{\omega}}}_{0}$+${\mathrm{\ensuremath{\delta}}}_{2}$, which can be asymmetrically placed about the atomic transition frequency ${\mathrm{\ensuremath{\omega}}}_{0}$ and can have different Rabi frequencies ${\mathrm{\ensuremath{\Omega}}}_{1}$ and ${\mathrm{\ensuremath{\Omega}}}_{2}$. Applying the optical Bloch equations for the bichromatic excitation, we derive an infinite set of equations of motion for the time evolution of the atomic variables. The equations are solved numerically by matrix inversion and Laplace transforms. Using the quantum regression theorem, we then solve for the steady-state total fluorescence intensity, and the resonance-fluorescence and absorption spectra. The spectra are found to depend on the frequency difference 2\ensuremath{\delta}=${\mathrm{\ensuremath{\delta}}}_{1}$+${\mathrm{\ensuremath{\delta}}}_{2}$, the average detuning \ensuremath{\Delta}=${\mathrm{\ensuremath{\omega}}}_{0}$-1/2(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$), and the Rabi frequencies of the driving fields. For ${\mathrm{\ensuremath{\Omega}}}_{1}$=${\mathrm{\ensuremath{\Omega}}}_{2}$=\ensuremath{\Omega}, the total fluorescent intensity displays a series of maxima for \ensuremath{\Delta}=\ifmmode\pm\else\textpm\fi{}n\ensuremath{\delta}\ensuremath{\mp}${\mathrm{\ensuremath{\Omega}}}^{2}$/4\ensuremath{\delta}, where the n are the odd integers. The intensity-dependent shift from the resonances n\ensuremath{\delta} is explained as an analog of the generalized Bloch-Siegert shift. The resonance-fluorescence spectrum for \ensuremath{\Delta}\ensuremath{\ne}0 appears to contain more peaks than that for \ensuremath{\Delta}=0.This is due to the splitting of the central peak and the even sidebands into doublets. The absorption spectrum of a weak-probe beam for \ensuremath{\Delta}=0 and equal Rabi frequencies consists of a symmetric series of dispersionlike sidebands separated from ${\mathrm{\ensuremath{\omega}}}_{0}$ by integer multiples of \ensuremath{\delta}, together with a central absorption peak at ${\mathrm{\ensuremath{\omega}}}_{0}$, whose amplitude oscillates with \ensuremath{\Omega}. For \ensuremath{\Delta}\ensuremath{\ne}0 and/or ${\mathrm{\ensuremath{\Omega}}}_{1}$\ensuremath{\ne}${\mathrm{\ensuremath{\Omega}}}_{2}$, the odd sidebands remain dispersionlike, while the central peak and the even sidebands split into absorption-emission doublets. A simple physical interpretation of the spectral features is given in terms of the dressed-atom model.
The emission spectrum is calculated for a system of two identical atoms, having relative coordinate r. Initially one atom is in an excited state and the other in its ground state. Both atom and field variables are fully quantized, so that the calculation automatically includes effects related to both retardation and atomic recoil on the absorption or emission of radiation. It is shown that for k0{\mathrm{k}}_{0}k0​r\ensuremath{\gg}:1 (where k0{\mathrm{k}}_{0}k0​=2\ensuremath{\pi}/\ensuremath{\lambda} and \ensuremath{\lambda} is the wavelength associated with the resonant excited- to ground-state transition), the emission spectrum can consist of a triplet. The frequency separation between the components of the triplet can be interpreted in terms of the recoil the atoms undergo individually on emitting or absorbing radiation. For k0{\mathrm{k}}_{0}k0​r\ensuremath{\ll}1, the atoms emit as a composite system and the recoil (while not resolvable) is that associated with a ``molecule'' of mass 2m, where m is the mass of one of the atoms.