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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Narrowing of the homogeneous two-photon absorption line width in two-level dipolar system

Aleksander K. Rebane, Mikhail A. Drobizhev, Nikolay S. Makarov

Published Jan 8, 2008• 1 citation
Publisher

Abstract

We study narrowing of nonlinear two photon absorption line shape in system with non-zero permanent dipole moment difference between the ground- and excited state. The temperature-induced broadening of one photon absorption (1PA) and two photon absorption (2PA) line shapes is modeled by subjecting the resonance transition frequency to random fluctuations of varying amplitude and by solving numerically the corresponding two-level density matrix equation of motion. We show that under conditions, when 1PA and 2PA transitions are both far from saturation, the 2PA homogeneous line width may be as much as 25% narrower than the corresponding 1PA line width. This offers novel possibilities for reducing the temperature-induced dephasing in quantum computing, quantum memory and other applications based on coherent multi-photon interactions.

DOI
10.1117/12.761400

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We study narrowing of nonlinear two photon absorption line shape in system with non-zero permanent dipole moment difference between the ground- and excited state. The temperature-induced broadening of one photon absorption (1PA) and two photon absorption (2PA) line shapes is modeled by subjecting the resonance transition frequency to random fluctuations of varying amplitude and by solving numerically the corresponding two-level density matrix equation of motion. We show that under conditions, when 1PA and 2PA transitions are both far from saturation, the 2PA homogeneous line width may be as much as 25% narrower than the corresponding 1PA line width. This offers novel possibilities for reducing the temperature-induced dephasing in quantum computing, quantum memory and other applications based on coherent multi-photon interactions.
We calculate the third-order nonlinear absorption and dispersion (self-phase-modulation and cross-phase modulation) of a homogeneously broadened two-level molecular system with permanent dipole moments interacting with (1) an optical field of frequency \ensuremath{\omega}, and (2) two optical fields of frequency ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, i.e., the susceptibilities ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) and ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{1}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{2}$). Sharp features in the nonlinear absorption and dispersion appear whenever one- or two-photon resonance conditions are met. Only features corresponding to one-photon resonance arise if the difference between the permanent dipole moments of the levels, \ensuremath{\Delta}\ensuremath{\mu}, vanishes. The ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) spectrum has two features, one at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$ dominated by contributions proportional to ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{4}$, where ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$ is the transition dipole moment of the two levels with transition frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and the other at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$/2 dominated by contributions proportional to (\ensuremath{\Delta}\ensuremath{\mu})2{)}^{2})2${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{2}$. Sharp features in ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{2}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{1}$) appear when ${\mathrm{\ensuremath{\omega}}}_{2}$ is near ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$,${\mathrm{\ensuremath{\omega}}}_{1}$,${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and \ensuremath{\Vert}${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$\ensuremath{\Vert}.
The physics of the two-photon absorption process is investigated for a three-state system. The density-matrix equations for the two-photon interaction are solved in the steady-state limit assuming that the pump laser radiation is monochromatic. Collisional broadening, saturation, and Stark shifting of the two-photon resonance are investigated in detail by numerical solution of the steady-state density-matrix equations. Analytical expressions for the saturation intensity and the Stark shift are derived for the case where the single-photon transitions between the intermediate state and the initial and final states are far from resonance with the pump laser. For this case, it is found that the direction of the Stark shift is dependent on the relative magnitudes of the dipole-moment matrix elements for the single-photon transitions that couple the intermediate state with the initial and final states. Saturation and Stark shifting are also investigated for the case where the single-photon transitions between the intermediate state and the initial and final states are close to resonance with the pump laser.
In this paper, two-photon absorption resonance has been investigated . We studied this phenomenon in three-level system with common upper level, two lower long-life levels and two quasi-resonant laser fields with different frequency spectrum. It has been shown that, the absorption coefficient in the far distance from absorption line at the frequency of two-photon resonance has considerable amplitude and narrow width. Frequency difference between two lower levels is transition frequency for optical clocks. This resonance is much less sensitive to the effects of noise components and probing fields compared with electromagnetically induced transparency. Stark shift of the two-photon resonance can be offset and reduced by the changes in the probing field amplitude. We recommended to use an additional laser with narrow line to stabilize the frequency at optical clock to get a line in sub-Hertz range.
The line shape of a Doppler-broadened transition is dramatically altered by the presence of a laser field resonating with a second Doppler-broadened transition sharing a common level: Two narrow resonances of different widths appear superimposed upon the broad background signal at frequencies symmetrically located about the corresponding line center. The effect has already found application in a number of seemingly different though intimately related studies, including high-resolution hfs and isotope-shift determinations. The theory of the effect is developed with reference to these applications. The treatment is formulated in terms of transition rates induced by two classical fields resonantly interacting with a pair of coupled Doppler-broadened transitions of arbitrary frequencies. The perturbation approach adopted is valid for one field fully saturating its transition; the resulting line-shape expression exhibits important power-broadening effects. This approach is equivalent to the familiar density-matrix formulation, which is also presented. Various features of the resulting expression are discussed in detail as they apply to two precision spectroscopic applications, mode crossing and spontaneous emission line narrowing. The connection with previous work is also discussed.
A weak excitation transit-time resolution limited analytic line shape is derived for a Doppler broadening-free degenerate two-photon transition from a standing wave with a TEM00 transverse profile. This approximation is appropriate when the collisional mean free path is much larger than the transverse width of the TEM00 beam. It is considerably simpler than the two-photon absorption line shape previously published, Bordé, C. R. Hebd. Seances Acad. Sci., Ser. B 282, 341–344 (1976), which was derived for more general experimental conditions. The case of a saturating field, with an intensity-dependent shift of the resonance frequency, is treated and expressed in reduced units. Numerical calculations are presented for the line shape for a range of the reduced intensity and light intensity shifts values.
Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.