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Journal of Luminescence

Long-delay engraving and recovery of chirped femtosecond pulses by spectro-temporal holography in spectral hole-burning molecular solids

Jean‐Pierre Galaup, A.A. Gorokhovsky

Published Mar 5, 2007• 0 citations
Publisher
DOI
10.1016/j.jlumin.2007.02.043

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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.

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Spatio-temporal holography using persistent spectral hole-burning in dye molecules embedded in plastic films is promising for applications such as femtosecond pulse shaping, data storage or phase conjugation. In addition to the common 2 spatial dimensions of classical holograms, each point in the sample plane can be used to store spectral informations such as the shape of a femtosecond pulse. On each point of the sample, spectral interferences between a reference pulse and an object pulse (for example chirped) are recorded via spectral hole-burning in the absorption band of the dye molecule. As early as 1983, photon echo and time-reversal experiments using persistent spectral hole-burning were performed in porphyrazine styrol solutions at 630 nm [1]. Then several developments, like the reconstruction of the polarization state of object pulses [2], time and space holography [3,4], image holograms using a single pair of femtosecond pulses [5] were demonstrated in different photosensitive media.

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We apply Fourier-transform spectral interferometry to complete phase and intensity characterization of a chirped filter engraved in a persistent spectral hole-burning (PSHB) material. The conjugated transfer function of a grating pair compressor is stored in a PSHB material as an accumulated spectral hologram that behaves as a pulse stretcher. By directing the diffracted pulse back through the compressor, we verified that the PSHB stretcher’s transfer function is indeed conjugated to that of the grating pair compressor. We have extended the spectral phase analysis to regions where the engraved structure is much narrower than the spectrometer’s resolution.

Journal of the Optical Society of America B•Mar 1, 2003•2 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.
Spatio-temporal holography using persistent spectral hole-burning in dye molecules embedded in plastic films is promising for applications such as femtosecond pulse shaping, data storage or phase conjugation. In addition to the common 2 spatial dimensions of classical holograms, each point in the sample plane can be used to store spectral informations such as the shape of a femtosecond pulse. On each point of the sample, spectral interferences between a reference pulse and an object pulse (for example chirped) are recorded via spectral hole-burning in the absorption band of the dye molecule. As early as 1983, photon echo and time-reversal experiments using persistent spectral hole-burning were performed in porphyrazine styrol solutions at 630 nm [1]. Then several developments, like the reconstruction of the polarization state of object pulses [2], time and space holography [3,4], image holograms using a single pair of femtosecond pulses [5] were demonstrated in different photosensitive media.
We apply Fourier-transform spectral interferometry to complete phase and intensity characterization of a chirped filter engraved in a persistent spectral hole-burning (PSHB) material. The conjugated transfer function of a grating pair compressor is stored in a PSHB material as an accumulated spectral hologram that behaves as a pulse stretcher. By directing the diffracted pulse back through the compressor, we verified that the PSHB stretcher’s transfer function is indeed conjugated to that of the grating pair compressor. We have extended the spectral phase analysis to regions where the engraved structure is much narrower than the spectrometer’s resolution.