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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Spectral Hole-Burning and Holography in a Y2SiO5:Pr3+ Crystal

Keith Holliday, Mauro Croci, Eric Vauthey, Urs P. Wild

Published Jan 1, 1992• 4 citations
Publisher

Abstract

Plane wave holography is a method of producing and detecting weak spectral holes with very low background [1]. Its success relies upon hole-burning materials of excellent optical quality with strongly absorbing zero phonon lines such as dye doped polymers which have been extensively studied [2 and references therein]. Through an extension of this technique, image storage [3] and data manipulation [4] have been demonstrated in such materials. Here, we report the application of plane wave holography to a crystalline material, Y2SiO5:Pr3+, for the first time. Spectroscopic measurements of Y2SiO5:Pr3+ have not previously been reported.

DOI
10.1364/shbl.1992.tua4

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Plane wave holography is a method of producing and detecting weak spectral holes with very low background [1]. Its success relies upon hole-burning materials of excellent optical quality with strongly absorbing zero phonon lines such as dye doped polymers which have been extensively studied [2 and references therein]. Through an extension of this technique, image storage [3] and data manipulation [4] have been demonstrated in such materials. Here, we report the application of plane wave holography to a crystalline material, Y2SiO5:Pr3+, for the first time. Spectroscopic measurements of Y2SiO5:Pr3+ have not previously been reported.
Holeburning holography is an ultrahigh density image storage technique. Since the memory capacity is governed by the ratio of the inhomogeneous-to-homogeneous linewidths, 103~106 images can be recorded in a single sample spot. An extensive study on holebuming holography has been carried out by Wild et.al for organic dye-doped polymer samples1-4. On the other hand, holeburning holography has not been carried out for crystal samples, because there are few crystals exhibiting persistent holes. We have performed holeburning holography to record images for Eu3+:Y2SiO5 crystal which has been known for exhibiting persistent holes. Moreover, Eu3+:Y2SiO5 has other unique features5,6 such as narrow holewidth and high holeburning quantum efficiency. By using this crystal, we have also succeeded in real-time recording of a moving object.
Holographic detection of spectral holes is demonstrated in a crystalline host material with signal-to-noise ratios of up to 104{10}^{4}104. Hole burning occurs in two Pr3+{\mathrm{Pr}}^{3+}Pr3+ sites in the Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ lattice, in both cases due to population redistribution between the ground-state quadrupole levels. The signal contains contributions due to a resonant hole and several side holes and antiholes, a phenomenon not previously observed using the holographic technique. The diffracted spectrum is modeled in two ways. In the first case the transmission spectrum is used to determine the population gratings and thus the diffraction efficiency. In the second case the transition probabilities between ground- and excited-state Kramer's doublets are used to model the population gratings. The technique is applied to pseudo-Stark-effect measurements from which the crystallographic sites as determined by x-ray analysis are matched to the spectroscopic data presented here. The time decay of the diffracted signal is used to study nuclear spin-lattice relaxation. It is shown that at 1.6 K temperature-dependent phonon-induced processes make no contribution to this decay. The nonexponential time decay of the population upon radio-frequency irradiation resonant with a ground-state quadrupole splitting is attributed to Pr-Pr cross relaxation.
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.
The use of holography is attractive for optical data storage due to its poten­tial for implementing page oriented data storage systems. However, multiplexed recording using Bragg selective materials has not provided a large enough stor­age capability to justify the expense of these systems. Persistent spectral hole burning holography allows multiplexed recording using much smaller wavelength separations between the holograms, and hence dramatically increases the storage capacity possible in holographic memory systems [1]. A comparison between the wavelength selectivity obtained for transmission gratings recorded using hole burning in a dye doped polymer film versus Bragg selectivity in a 1 cm thick iron-doped lithium niobate crystal is shown in Fig. (1).
Time-and-space-domain holography [1,2] can be regarded as an extension of a conventional holographic process, where, in addition to the spatial image, the hologram plays back the time dependence of an event. The play-back of events is possible because we are using highly frequency-selective inhomogeneously broadened absorbers as recording material. This technique has a variety of potential applications in optical data storage and processing. In the present paper we consider the basic physical principle of time-and-space-domain storage in frequency-selective materials which exploit the effect of spectral hole burning [3]. In particular we will show that organic dye-doped spectral hole burning materials allow recording and playback of pi- co- and femtosecond time-scale events.