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Shenyang Gongye Daxue xuebao

Research of hole width and depth on laser duration in spectral hole burning

Quan Shan

Published Jan 1, 2001• 0 citations
OpenAlex

Abstract

With the transient solutions of optical Bloch equation the dependences of hole width and depth on the burning pulse duration have been discussed in spectral hole burning of two level system.With a strong and short π pulse ,a deep hole can be burnt mode which width is much narrower than the steady state one predicted by optical bloch equation safficient.

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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).

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In this paper, the physical mechanism of the interaction between electromagnetic wave and spectral-hole burning crystal material is investigated in detail. In the small signal regime, a perturbation theory model is used to analyze the mechanism of spectral-hole burning. By solving the Liouville equation, three-order perturbation results are obtained. From the theoretic analysis, spectral-hole burning can be interpreted as a photon echo of the zero-order diffraction echo when the first optical pulse and the second optical pulse are overlapped in time. According to the model, the spectral-hole width is dependent on the chirp rate of the reading laser. When the chirp rate is slow with respect to the spectral features of interest, the spectral hole is closely mapped into time domain. For a fast chirp rate, distortions are observed. The results follow Maxwell—Bloch model and they are also in good agreement with the experimental results.

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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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The Journal of Chemical Physics•Feb 15, 1991•53 citations
With the transient solutions of optical Bloch equation the dependences of hole width and depth on the burning pulse duration have been discussed in spectral hole burning of two level system.With a strong and short π pulse ,a deep hole can be burnt mode which width is much narrower than the steady state one predicted by optical bloch equation safficient.
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).
In this paper, the physical mechanism of the interaction between electromagnetic wave and spectral-hole burning crystal material is investigated in detail. In the small signal regime, a perturbation theory model is used to analyze the mechanism of spectral-hole burning. By solving the Liouville equation, three-order perturbation results are obtained. From the theoretic analysis, spectral-hole burning can be interpreted as a photon echo of the zero-order diffraction echo when the first optical pulse and the second optical pulse are overlapped in time. According to the model, the spectral-hole width is dependent on the chirp rate of the reading laser. When the chirp rate is slow with respect to the spectral features of interest, the spectral hole is closely mapped into time domain. For a fast chirp rate, distortions are observed. The results follow Maxwell—Bloch model and they are also in good agreement with the experimental results.
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.
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 number of limitations to hole burning in the liquid phase are identified. As spectral diffusion becomes more rapid, a point is reached where the narrowest hole width no longer measures the homogeneous linewidth. Spectral congestion of the solute is also shown to limit the fastest detectable spectral diffusion rate. An optimal pulse length is found which allows observation of the most rapid spectral diffusion. In addition, the coherence effect observed when the pulses overlap is shown to have resonances at both the excited and ground state vibrational spacings. The coherence effect greatly resembles the hole burning spectrum, but contains no dynamical information. Because of these limitations, hole burning may not be observed even when the homogeneous spectrum is well resolved and spectral diffusion is slow. Experimental confirmation is found in the hole burning spectrum of iodine in hexane, which shows no hole burning despite having a narrow homogeneous linewidth.