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Journal of the Physical Society of Japan

Line Narrowing Effect in Fully Resonant Four Wave Mixing Spectroscopy in Solids

Hirotoshi Souma

Published Sep 1, 1983• 2 citations
Publisher

Abstract

We explain the utility of third-order nonlinear susceptibility, χ (3) (ω 2 ; ±ω 1 , \({\mp}\omega_{1}\), ω 2 ), for the observation of resonances with homogeneous widths from inhomogeneously broadened distributions in three-level systems related to Raman or two-photon allowed electronic transitions. The line narrowing and high resolution capabilities are demonstrated theoretically using a model for inhomogeneous distributions of transitions in which we regard an absorption spectrum as the composition of some inhomogeneously broadened substructures. The experimental methods to separate a signal having frequency ω 2 from ingoing beam at the same frequency are outlined.

DOI
10.1143/jpsj.52.3225

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We explain the utility of third-order nonlinear susceptibility, χ (3) (ω 2 ; ±ω 1 , ({\mp}\omega_{1}), ω 2 ), for the observation of resonances with homogeneous widths from inhomogeneously broadened distributions in three-level systems related to Raman or two-photon allowed electronic transitions. The line narrowing and high resolution capabilities are demonstrated theoretically using a model for inhomogeneous distributions of transitions in which we regard an absorption spectrum as the composition of some inhomogeneously broadened substructures. The experimental methods to separate a signal having frequency ω 2 from ingoing beam at the same frequency are outlined.
Three wave mixing is investigated with respect to its spectroscopic applications under fully resonant conditions. A theoretical study of the appropriate second order susceptibility χ(2) reveals interesting features both for sum and difference frequency generation. For difference frequency generation two different mechanisms are possible one of which allows the observation of resonances between excited states and the study of dephasing induced coherent emission. The coherence decay rate between the two excited states may be measured and also its pure dephasing rate. The line-narrowing characteristics of the fully resonant χ(2) are studied with respect to correlation between the inhomogeneous distribution for different levels. The line-narrowing capabilities are found to be partly complementary for the sum—and the two difference frequency resonance configurations. This leads to the suggestion of new line-narrowing techniques which could provide information about type and amount of correlation in inhomogeneously broadened systems.
Four-wave mixing processes with double and triple resonances are discussed in detail. Explicit expressions for the resonant nonlinear susceptibilities of various cases are derived. It is shown that in some cases, four-wave mixing can yield a spectrum with reduced inhomogeneous broadening. Possible applications of multiresonant four-wave mixing as a spectroscopic technique are considered. They include high-resolution spectroscopy, deduction of transition matrix elements, study of transitions between excited states, measurement of longitudinal relaxation times, distinction between resonant Raman scattering and resonant fluorescence, etc. Selective polarization arrangement allows us to suppress the nonresonant background, separately measure the real and imaginary parts of the resonant nonlinear susceptibility, minimize the effects of absorption and laser intensity fluctuations, and greatly enhance the signal-to-noise ratio.
A method is introduced to calculate for a model set of molecular levels the spectral line shapes expected for a variety of conventional laser experiments including absorption, hole burning, fluorescence line narrowing, and Raman scattering. The method allows the incident laser field to have arbitrary intensity. Furthermore, the effects of model Gaussian or Lorenzian inhomogeneous distributions are readily incorporated. Earlier results for a two-level system are easily obtained and new results are presented for inhomogeneously broadened two and three level systems, and for the effects of pure dephasing on the strong field spectra. In particular we have described the differences between fluorescence and Raman in strong fields, and the effect of strong fields on the spontaneous emission of inhomogeneously broadened transitions. Some predictions are made regarding line narrowing experiments in the strong-field limit.
In this article, we analyse a new sensitive spectroscopic technique in which a sample cell is irradiated by a two-frequency pump beam (ω + Δ ± δ/2) and a counter-propagating probe beam (ω). The phase-conjugate fields re-emitted at frequencies ω ± δ, via four-wave mixing processes, are detected through their heterodyne beating with the probe field. The properties of the heterodyne beat signal are studied by means of a perturbation calculation of the nonlinear response of the medium, carried out to the third order in the incident fields. In resonant gas media, the emission lineshape exhibits a Doppler-free doublet structure [frequency splitting 3 δ/2 for single-photon resonances, and δ/2 for two-photon transitions]. By using a phase-sensitive detection of the beat signal, one can separately analyse real (dispersion) or imaginary parts (absorption) of the nonlinear susceptibility. For single-photon transitions, the signal phase shift is related to the atomic levels lifetime and allows one to study the relaxation dynamics in gas phase (like quenching collisions, velocity diffusion, etc...). This is particularly interesting for cross-over resonances, in which only the common level contributes. In three-level systems, one also predicts a selective resonant enhancement of the phase-conjugate emission through Raman-type two-photon processes. Most of these predictions have been experimentally verified.
The advent of lasers has revolutionized the methods and possibilities of spectroscopy. Their monochromaticity permits the study of extremely narrow spectral features which would not have been resolved using classical techniques. Moreover, their extreme spectral power density, in giving rise to the field of nonlinear optics, which will be studied in Chapter 7, has resulted in the development of new and powerful spectroscopic techniques. These techniques, of which we describe briefly some examples in this complement, have as their basis the fact that an atom does not respond linearly when subjected to a very intense light field. First of all we shall describe the broadening mechanisms that explain the fact that the experimentally measured widths of atomic or molecular resonances are larger than those that would be observed if the atoms were isolated and at rest. We shall introduce in Section 3G.1 the concept of homogeneous width, which can be considered as the intrinsic width of a transition, and inhomogeneous width which concerns the variation of the frequency of a given transition that occurs because of the state of motion of the atom, or because of factors in its environment. We shall explain why it is possible, using nonlinear optical techniques to eliminate the effects of inhomogeneous broadening on recorded spectra, resulting in an improvement over the resolution of conventional techniques. We shall then concentrate more specifically on Doppler broadening , which is the most commonly encountered source of inhomogeneous broadening, describing two nonlinear optical techniques, saturated absorption spectroscopy (in Section 3G.2) and two-photon spectroscopy (in Section 3G.3), which enable it to be overcome.
The influence of the high-pump-field intensity saturation and dynamic Stark effects on the resonant nearly degenerate four-wave-mixing signal (${\mathrm{\ensuremath{\omega}}}_{3}$=2${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$) is studied in a frequency space defined by the pump- and probe-field frequencies, ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, respectively. Variable inhomogeneous widths have been considered ranging from extremely narrow (homogeneous distribution) to extremely wide. Remarkable differences between nearly homogeneously broadened systems and extreme inhomogeneous ones are exhibited. It is shown, for the situation of homogeneous broadening, that the spectra carried on with fixed probe and fixed pump frequency values have substantial differences in shape. These differences disappear in the situation of extreme inhomogeneous broadening. Fixed-pump-frequency resonant and fixed-probe-frequency nonresonant spectra are proposed as very convenient tools to yield useful evidence about the width of the inhomogeneous molecular distribution.