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Angewandte Chemie International Edition in English

Spectral Hole Burning at Room Temperature and with a Single Molecule: Two New Perspectives

Christoph Bräuchle

Published Apr 1, 1992• 9 citations
Publisher

Abstract

En route to real molecular electronics the “spectral hole burners” among physical chemists have come a long way. Two developments which foster these ambitions are discussed herein: 1. For the first time holes with sufficient thermal stability could be burned in experiments at room temperature by using the 4f electron transitions of Sm in substitutionally disordered microcrystals of SrFCl0.5Br0.5 or Mg0.5Sr0.5FCl0.5 doped with Sm2+. 2. The manipulation of single molecules necessary for real molecular electronics was possible on a perylene‐doped polyethylene film. At T = 1.5 K, spectral hole burning could be carried out selectively several times in succession with a single perylene molecule.

DOI
10.1002/anie.199204261

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Spectral Hole-Burning Between 2 K and Room Temperature in Sm2+ Doped Substitutionally Disordered Microcrystals

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Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations

Room-Temperature Persistent Spectral Hole Burning in Sm2+:SrFCl0.5Br0.5

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Electron transition process of 5D2→7F0 of Sm2+ in spectral hole-burning

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Materials of MyM’1-yFClxBr1-x:Sm2+ have been widely applied in spectral hole-burning since the first observation of persistent spectral hole-burning in BaFCl:Sm2+ at 2K was reported by A. Winnaker, etc. in 1985[1]. From then on, hole-burning in BaFCl0.5Br0.5:Sm2+ at 77K[2] in SrFCl and Mg0.5Sr0.5FCl0.5Br0.5:Sm2+ at room temperature[3, 4] were reported. Room temperature hole-buring of Sm2+ in fluorohafnate glasses[5,6] were reported in recent years also. These materials are of potential use in high temperature hole- burning. But comparing to organic materials, they have lower hole- burning efficiency and narrower inhomogenous line width. In order to apply spetral hole- buring in frequency domain optical storage, it is important to improve these materials.

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Two-photon persistent hole burning is observed at T = 296 K in 5 D 1 – 7 F 0 and 5 D 0 – 7 F 0 transitions of Sm 2+ ions in substitutionally disordered SrFCl 1/2 single crystals, showing the ratio of inhomogeneous to homogeneous linewidth of 20 ÷ 25. The minimum hole widths of 3.5 cm -1 and 2.6 cm -1 , respectively, were determined for these transitions. In fact, the applicability of persistent spectral hole burning, known as a low-temperature high-resolution spectroscopic method and a potential basis for the use of a new–spectral–dimension in optical data storage and processing, is demonstrated for the first time at room temperature in inorganic materials.

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We measured the temperature dependence of the fluorescence of Sm 2+ ions doped into a Mg 0.5 Sr 0.5 FCl 0.5 Br 0.5 mixed crystal and observed the persistent spectral hole burning at 90 K and 300 K. The electrons appearing at the 5 D 0 → 7 F 0 transition mostly come via the 4f5d→ 5 D 1 → 5 D 0 → 7 F 0 route but some of the electrons come directly from the 4f5d band. At 90 K, persistent spectral hole burning was achieved much more efficiently by the photon-gated spectral hole-burning process than by the one-photon hole-burning process, while the one-photon hole-burning process is much more efficient at 300 K.

Journal of Physics Condensed Matter•Mar 15, 2001•0 citations
En route to real molecular electronics the “spectral hole burners” among physical chemists have come a long way. Two developments which foster these ambitions are discussed herein: 1. For the first time holes with sufficient thermal stability could be burned in experiments at room temperature by using the 4f electron transitions of Sm in substitutionally disordered microcrystals of SrFCl0.5Br0.5 or Mg0.5Sr0.5FCl0.5 doped with Sm2+. 2. The manipulation of single molecules necessary for real molecular electronics was possible on a perylene‐doped polyethylene film. At T = 1.5 K, spectral hole burning could be carried out selectively several times in succession with a single perylene molecule.
Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.
Materials of MyM’1-yFClxBr1-x:Sm2+ have been widely applied in spectral hole-burning since the first observation of persistent spectral hole-burning in BaFCl:Sm2+ at 2K was reported by A. Winnaker, etc. in 1985[1]. From then on, hole-burning in BaFCl0.5Br0.5:Sm2+ at 77K[2] in SrFCl and Mg0.5Sr0.5FCl0.5Br0.5:Sm2+ at room temperature[3, 4] were reported. Room temperature hole-buring of Sm2+ in fluorohafnate glasses[5,6] were reported in recent years also. These materials are of potential use in high temperature hole- burning. But comparing to organic materials, they have lower hole- burning efficiency and narrower inhomogenous line width. In order to apply spetral hole- buring in frequency domain optical storage, it is important to improve these materials.
Two-photon persistent hole burning is observed at T = 296 K in 5 D 1 – 7 F 0 and 5 D 0 – 7 F 0 transitions of Sm 2+ ions in substitutionally disordered SrFCl 1/2 single crystals, showing the ratio of inhomogeneous to homogeneous linewidth of 20 ÷ 25. The minimum hole widths of 3.5 cm -1 and 2.6 cm -1 , respectively, were determined for these transitions. In fact, the applicability of persistent spectral hole burning, known as a low-temperature high-resolution spectroscopic method and a potential basis for the use of a new–spectral–dimension in optical data storage and processing, is demonstrated for the first time at room temperature in inorganic materials.
We measured the temperature dependence of the fluorescence of Sm 2+ ions doped into a Mg 0.5 Sr 0.5 FCl 0.5 Br 0.5 mixed crystal and observed the persistent spectral hole burning at 90 K and 300 K. The electrons appearing at the 5 D 0 → 7 F 0 transition mostly come via the 4f5d→ 5 D 1 → 5 D 0 → 7 F 0 route but some of the electrons come directly from the 4f5d band. At 90 K, persistent spectral hole burning was achieved much more efficiently by the photon-gated spectral hole-burning process than by the one-photon hole-burning process, while the one-photon hole-burning process is much more efficient at 300 K.