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Physics and chemistry of materials with low-dimensional structures. Series C, Molecular structures

Spectral Hole-Burning in Crystalline and Amorphous Organic Solids. Optical Relaxation Processes at Low Temperature

Silvia Volker

Published Jan 1, 1989• 40 citations
Publisher
DOI
10.1007/978-94-009-0863-5_4

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Aspects of hole burning and spectro-temporal holography in molecular doped solids (Review)

Jean‐Pierre Galaup

The persistent spectral hole-burning (PSHB) phenomenon has been known since 1974. It is still an important research area for the study of the intimacy of complex molecular systems in the solid state, revealing high-resolution spectra, photophysics, photochemistry, and dynamics of molecular doped amorphous media, organic as well as inorganic. From another point of view, PSHB allows the engraving of any spectral structures in the inhomogeneous absorption band profile of molecular doped amorphous hosts or ion doped crystals cooled down to liquid helium temperatures. Therefore, a PSHB material is programmable in the spectral domain and consequently it can be transformed in an optical processor capable of achieving user-defined optical functions. Some aspects of both fields are illustrated in the present paper. Concerning the search for efficient PSHB materials, the hole-burning performances and the photophysics of polymer and xerogel based systems are compared. The problem of high-temperature persistent spectral hole-burning materials and the search for new frequency selective photosensitive systems for fast optical pulse processing at 800nm are considered. Regarding the points treated, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, by combining inorganic and organic capabilities or by grafting organic species to the host, hybrid xerogels have not yet revealed all possibilities. Also, the interest of two-photon materials for engraving spectral features with near-infrared or infrared light is developed. As an introduction to possible applications of PSHB material, the basics of spectro-temporal holography are remembered and a demonstrative experiment using a naphthalocyanine-doped polymer film is described, proving that the temporal aberration free recompression of ultrashort light pulses is feasible, therefore opening a way for applications in ultrashort light pulse shaping. Aspects for a comparison between cw hole-burning and femtosecond spectro-temporal experiments are considered, and prospects for coherent control of light fields or photochemical processes are also evoked.

Low Temperature Physics•Nov 1, 2006•1 citation

Laser Hole Burning Spectroscopy: A High Resolution Probe of Molecular Environments.

R. M. Macfarlane, Robert M. Shelby

Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.

Final Report•Jun 1, 1981•0 citations
The persistent spectral hole-burning (PSHB) phenomenon has been known since 1974. It is still an important research area for the study of the intimacy of complex molecular systems in the solid state, revealing high-resolution spectra, photophysics, photochemistry, and dynamics of molecular doped amorphous media, organic as well as inorganic. From another point of view, PSHB allows the engraving of any spectral structures in the inhomogeneous absorption band profile of molecular doped amorphous hosts or ion doped crystals cooled down to liquid helium temperatures. Therefore, a PSHB material is programmable in the spectral domain and consequently it can be transformed in an optical processor capable of achieving user-defined optical functions. Some aspects of both fields are illustrated in the present paper. Concerning the search for efficient PSHB materials, the hole-burning performances and the photophysics of polymer and xerogel based systems are compared. The problem of high-temperature persistent spectral hole-burning materials and the search for new frequency selective photosensitive systems for fast optical pulse processing at 800nm are considered. Regarding the points treated, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, by combining inorganic and organic capabilities or by grafting organic species to the host, hybrid xerogels have not yet revealed all possibilities. Also, the interest of two-photon materials for engraving spectral features with near-infrared or infrared light is developed. As an introduction to possible applications of PSHB material, the basics of spectro-temporal holography are remembered and a demonstrative experiment using a naphthalocyanine-doped polymer film is described, proving that the temporal aberration free recompression of ultrashort light pulses is feasible, therefore opening a way for applications in ultrashort light pulse shaping. Aspects for a comparison between cw hole-burning and femtosecond spectro-temporal experiments are considered, and prospects for coherent control of light fields or photochemical processes are also evoked.
Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.