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Physics of the Solid State

Doppler spectroscopy of zero-phonon lines

Karl K. Rebane

Published Jan 1, 2007• 1 citation
Publisher

Abstract

Narrow profiles of purely electronic zero-phonon lines open up attractive possibilities for spectral investigation with the use of the Doppler effect (Doppler spectroscopy). It is established that, for a 10-MHz-wide zero-phonon line to shift to a new position, the velocity of motion of a receiver with respect to a source needs to be only ∼10 m/s. It is shown that the narrower the line or the spectral hole (its negative image), the more efficient the Doppler spectroscopy. The possibility of measuring the shape of spectral holes with the use of Doppler spectroscopy is demonstrated, and the potentialities of supersensitive Doppler spectroscopy are considered. The specific feature revealed in the frequency modulation by Doppler spectroscopy is that it occurs without a perturbation of the internal states of the emitter and absorber. The conclusion is drawn that there is a need to study the interference of a photon with itself when the frequency of “one-half of it” changes with the use of Doppler spectroscopy.

DOI
10.1134/s1063783407010155

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Narrow profiles of purely electronic zero-phonon lines open up attractive possibilities for spectral investigation with the use of the Doppler effect (Doppler spectroscopy). It is established that, for a 10-MHz-wide zero-phonon line to shift to a new position, the velocity of motion of a receiver with respect to a source needs to be only ∼10 m/s. It is shown that the narrower the line or the spectral hole (its negative image), the more efficient the Doppler spectroscopy. The possibility of measuring the shape of spectral holes with the use of Doppler spectroscopy is demonstrated, and the potentialities of supersensitive Doppler spectroscopy are considered. The specific feature revealed in the frequency modulation by Doppler spectroscopy is that it occurs without a perturbation of the internal states of the emitter and absorber. The conclusion is drawn that there is a need to study the interference of a photon with itself when the frequency of “one-half of it” changes with the use of Doppler spectroscopy.
A pure-electronic zero-phonon line, which represents an optical analog of the Mössbauer γ-resonance line, is a cornerstone of three remarkable areas of spectroscopy and optics of impurity solids, namely, ultrahigh-resolution spectroscopy, persistent hole-burning spectroscopy, and spectroscopy of single impurity molecules. In recent experiments made by the photon echo technique, a zero-phonon line width as small as 78 Hz was achieved (with the Q -factor, i.e., the ratio of the transition frequency to the line width being 2×10 14 :78≈ 10 12 ), which is several tenfold lower than the frequency shift of the vibronic spectrum caused by the momentum of the absorbed or emitted photon of optical range. We estimate the position, intensity, and width of zero-phonon lines under conditions when these characteristics, as well as properties of the phonon wing, are determined not only by Stokes losses but also by the photon recoil effect. It is shown that the latter effect, within the approximation used, does not lead to strong and easily detectable phenomena. They, however, take place, and their study is becoming more topical with improving accuracy and sophistication of the experimental technique (in the photon echo configurations, etc.).
A few examples of recent progress in the study and applications of purely electronic zero-phonon line (ZPL) and its offshoots are briefly considered: new experimental values of the narrowest ZPL; time-and-space-domain holography in the femtosecond domain, and the realization of a femtosecond Taffoli gate by it; single-impurity-molecule spectroscopy, its relation to single-photon interference and to the realization of quantum computing; the promises of quantum computing compared to what has already been done in holography.
Fluorescence—line—narrowing, spectral hole—burning and single molecule spectroscopy are methods of selective spectroscopy using zero-phonon lines (ZPL) to make selection in molecular ensemble. However if electron-phonon coupling is strong or sample temperature is near to room temperature, ZPL are absent and the optical band consists of electron-phonon transitions which are called phonon-side-band (PSB). In these cases the above mentioned methods of selective spectroscopy do not work. Can we get an information concerning a homogeneous optical band from inhomogeneously broadened bands in these cases? The answer is yes if we use femtosecond photon echo.
A theory of the influence of binary collisions on the line shapes associated with Doppler-free spectroscopy is presented. The specific calculation is for two-photon absorption through a real or virtual intermediate state, but the extension of the results to alternative level schemes is included. Collisions are treated quite generally at first, but, ultimately, a simple but reasonable collision model is adopted to properly account for both the "phase-interrupting" and "velocity-changing" aspects of collisions. It is shown that collisional processes can be used to distinguish between the "two-quantum" and "stepwise" contributions to the two-photon excitation rate. Moreover, it is demonstrated that systematic experimental line-shape investigations, in addition to providing tests of current collision theories, can lead to values for collision broadening and shift parameters, excitation transfer rates, magnetic substate relaxation rates, velocity-changing collision rates, and collision kernels. Consequently, Doppler-free spectroscopy can provide a new and important probe of collision effects in atomic and molecular systems.
Spectroscopies of matrix isolated species and impurity activated solids are close relatives. Both are among the well developing chapters of solid state spectroscopy and optics. In this paper I am trying to give very brief overview what has been achieved in science and applications of impurity activated solids based on zero-phonon lines (ZPLs) in optical data storage and processing. I would like to show that the latter comprises via persistent spectral hole burning time-and-space domain holography in a certain meaning also the "stopping of light". ZPLs are beginning to play a role in the approaches to optical quantum computing.