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physica status solidi (b)

Theory of Two‐Step Spectral Hole Burning by Pulses

Inna Rebane

Published Feb 1, 1988• 7 citations
Publisher

Abstract

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).

DOI
10.1002/pssb.2221450241

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

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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).

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Possibility of spectral holes narrower than those determined by natural linewidth

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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.

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PHOTON GATED HOLE BURNING IN THE7F0?5D2ABSORPTION OF BaCIF : Sm2+

J. C. Vial, R. M. Macfarlane

Spectral hole burning in solids is a selective bleaching of a small portion of an inhomogeneously broadened optical transition by a laser. In the photon gated holeburning process spectral holes are burned in two steps. The first is provided by a narrow band laser resonant with the inhomogeneously broadened transition and the second (gating) can be initiated by a broad band light source. Photon gated spectral hole burning was reported recently in 7F0→5D0 and 7F0→5D1 absorption lines of Sm2+ in BaClF(1). In this poster we report on the spectral holeburning behaviour of 1F0→5D2 transition. We found that even in absence of additional light source for gating, permanent holes can be burned. This self gating behaviour is consistent with the observation that the optimum frequency following 5D0 excitation is ≈ 22 000cm-1 so that two photons of energy 5D2 - 7F0 are sufficient to produce photoionisation. We have analysed the light intensity dependance of hole area and a simple model indicate that the electron transfer following the photoionisation is strongly dependant on the ion - electron trap distance.

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Femtosecond hole burning storage by two-photon absorption

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Summary form only given. Spectral hole burning (SHB) is a promising technique for optical recording of information with a potential to store in excess of 10/sup 4/-10/sup 5/ bits per /spl lambda//sup 3/ volume (Moerner, 1988). Highest storage capacity is achieved when frequency- or time-domain addressing is combined with addressing in three spatial dimensions by using a bulk SHB medium. However, so far both bit-by-bit and holographic SHB storage experiments were restricted to two spatial dimensions. This is because focusing a laser beam to a small volume inside the SHB medium is hindered by one-photon absorption in SHB material layers. We propose that this problem may be overcome by burning holes via two-photon absorption (TPA) (Demtro/spl uml/der, 1982; Takeda et al, 2000). TPA has been used earlier for conventional spectrally nonselective recording in photo-chromic materials by focusing two perpendicularly directed laser beams (with photon energies /spl planck//spl omega//sub 1/ and /spl planck//spl omega//sub 2/) on to one spot (Parthenopoulos and Rentzepis, Science, vol. 245, pp. 843-845, 1989). Since the sample is transparent for each beam separately, TPA occurs only at the beam intersection point. In this paper, we investigate frequency-selective SHB by TPA in organic dye-doped polymers at low temperature. In our experiments, the SHB medium is essentially transparent for the writing beams, which allows unrestricted penetration and focusing in the depth of the sample.

Conference on Lasers and Electro-Optics•Jan 1, 2001•1 citation
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).
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).
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).
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.
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.
Spectral hole burning in solids is a selective bleaching of a small portion of an inhomogeneously broadened optical transition by a laser. In the photon gated holeburning process spectral holes are burned in two steps. The first is provided by a narrow band laser resonant with the inhomogeneously broadened transition and the second (gating) can be initiated by a broad band light source. Photon gated spectral hole burning was reported recently in 7F0→5D0 and 7F0→5D1 absorption lines of Sm2+ in BaClF(1). In this poster we report on the spectral holeburning behaviour of 1F0→5D2 transition. We found that even in absence of additional light source for gating, permanent holes can be burned. This self gating behaviour is consistent with the observation that the optimum frequency following 5D0 excitation is ≈ 22 000cm-1 so that two photons of energy 5D2 - 7F0 are sufficient to produce photoionisation. We have analysed the light intensity dependance of hole area and a simple model indicate that the electron transfer following the photoionisation is strongly dependant on the ion - electron trap distance.
Summary form only given. Spectral hole burning (SHB) is a promising technique for optical recording of information with a potential to store in excess of 10/sup 4/-10/sup 5/ bits per /spl lambda//sup 3/ volume (Moerner, 1988). Highest storage capacity is achieved when frequency- or time-domain addressing is combined with addressing in three spatial dimensions by using a bulk SHB medium. However, so far both bit-by-bit and holographic SHB storage experiments were restricted to two spatial dimensions. This is because focusing a laser beam to a small volume inside the SHB medium is hindered by one-photon absorption in SHB material layers. We propose that this problem may be overcome by burning holes via two-photon absorption (TPA) (Demtro/spl uml/der, 1982; Takeda et al, 2000). TPA has been used earlier for conventional spectrally nonselective recording in photo-chromic materials by focusing two perpendicularly directed laser beams (with photon energies /spl planck//spl omega//sub 1/ and /spl planck//spl omega//sub 2/) on to one spot (Parthenopoulos and Rentzepis, Science, vol. 245, pp. 843-845, 1989). Since the sample is transparent for each beam separately, TPA occurs only at the beam intersection point. In this paper, we investigate frequency-selective SHB by TPA in organic dye-doped polymers at low temperature. In our experiments, the SHB medium is essentially transparent for the writing beams, which allows unrestricted penetration and focusing in the depth of the sample.