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Journal of Physics B Atomic Molecular and Optical Physics

Theory of two-step pulsed photoburning of limiting narrow spectral holes

Inna Rebane

Published Aug 14, 1989• 2 citations
Publisher

Abstract

One-step (0 to 1) spectral hole burning (SHB) is widely used as a method of eliminating inhomogeneous broadening of spectra: the minimal width of the hole in the inhomogeneous distribution function (IDF) of the transition frequency Omega 01 is obtained by SHB with monochromatic light and is determined by the homogeneous linewidth sigma 0 = gamma 1 + Gamma (where gamma 1 and Gamma are the constants of the energetic and the phase relaxation of the (first) excited level respectively). Two-step (0 to 1 to 2) SHB is considered where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. If the selective pulse is a coherent and single-sided exponential then, in the case of an extremely short fixing pulse ( delta pulse), on the increase of the time delay T between the selective and fixing pulses, a monotonic narrowing of the spectral hole in the IDF of the frequency Omega 01 takes place up to the limit width Gamma + mod gamma 1 - Delta mod (where Delta is the spectral width of the selective pulse).

DOI
10.1088/0953-4075/22/15/016

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Annual Review of Physical Chemistry•Jan 1, 1989•230 citations
One-step (0 to 1) spectral hole burning (SHB) is widely used as a method of eliminating inhomogeneous broadening of spectra: the minimal width of the hole in the inhomogeneous distribution function (IDF) of the transition frequency Omega 01 is obtained by SHB with monochromatic light and is determined by the homogeneous linewidth sigma 0 = gamma 1 + Gamma (where gamma 1 and Gamma are the constants of the energetic and the phase relaxation of the (first) excited level respectively). Two-step (0 to 1 to 2) SHB is considered where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. If the selective pulse is a coherent and single-sided exponential then, in the case of an extremely short fixing pulse ( delta pulse), on the increase of the time delay T between the selective and fixing pulses, a monotonic narrowing of the spectral hole in the IDF of the frequency Omega 01 takes place up to the limit width Gamma + mod gamma 1 - Delta mod (where Delta is the spectral width of the selective pulse).
Abstract A two‐step spectral hole burning (SHB) is considered, where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. It is shown that in a three‐level system excited by two consecutive pulses, the kinetics of the forming spectral hole differs essentially from the one on stationary irradiation. In the case of a short second pulse the shape of the hole in the inhomogeneous distribution function (IDF) of the purely electronic line frequency Ω01 is dependent on the time interval T between the first and second excitation steps and under certain conditions a hole can be obtained which is narrower than in the one‐step SHB with monochromatic light. It is considered how the hole in IDF is manifested in the absorption and two‐step pulse excitation spectra. It is shown that the hole in the absorption spectrum may be narrower than 2γ1 and in the two‐step pulse excitation, −γ1 (γ1 is the energy relaxation constant of the first excited level).
A theory of spectral hole burning (SHB) by light pulses of an arbitrary shape and duration is proposed. One- and two-step (photon-gated) SHB processes induced by laser pulses in two-, three- and four-level systems are theoretically considered. It is shown that for two-step SHB there exists a possibility of obtaining spectral holes which are narrower than in the one-step SHB with monochromatic light. In case of one- and two-step SHB the dependence of the shape of the hole on the duration of the burning pulse is considered (on two-step SHB the second pulse is Δ-pulse).
The two-step persistent spectral hole burning (PSHB) of a hole in the inhomogeneous distribution function (IDF) of the optical transition frequencies in a three-level system by two successive light pulses, in the case of an exponentially increasing and decreasing first coherent pulse and an infinitely short second pulse is calculated. The compensation effect of the natural linewidth of the first excited level and the parameter describing the exponential decrease of the intensity of the first burning pulse is shown. The time-dependent zero-phonon line (ZPL) in luminescence spectrum in the recording scheme containing the time gate in front of the spectrometer with high resolution in the case of exponential opening and closing of the time gate is calculated. The effect of the compensation of the natural linewidth of the excited level and the parameter describing the exponential increase of the transparency of the time gate is shown.
Abstract The shape of the spectral hole in an inhomogeneous distribution function of centres over the transition frequency is calculated for the case of a quasimonochromatic burning light pulse which characteristic duration time is comparable to the relaxation times of the excited electronic level. Two‐step spectral hole‐burning in the cases of three‐ and four‐level systems as well as one‐step processes are considered. The temporal responses of the spectral holes as spectral filters on δ‐pulse of light are found.
Zero-phonon lines in impurity optical spectra and their inhomogeneous broadening are discussed. Photoburning of persistent spectral holes is not only an effective method to eliminate the inhomogeneous broadening and perform high resolution spectroscopy, but it serves also as a powerful tool to control by means of illumination the absorption coefficient and refractive index of the matter. It opens new horizons for frequency-selective optical memories, data storage and data processing. Hole burning by picosecond pulses and the time-and space-domain holography based on it are discussed and the results of the experiments described.
The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2: