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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Optical spectroscopy of Tm 3+ in organic matrices for hole-burning storage applications

Alexey V. Turukhin, Agnes V. Carpenter, A.A. Gorokhovsky, R. R. Alfano, Ting-Yi Chu, Yoshiyuki Okamoto

Published Nov 5, 1998• 2 citations
Publisher

Abstract

The optical properties of four Tm3+ chelates, specifically (beta) -diketone tris chelates of thulium, in a poly(methyl methacrylate) matrix are presented. Samples under investigation were the Tm3+ complexes formed using thulium chloride (TmCl3 (DOT) 6H2O) with thenoyltrifluoroacetylacetone (TTFA), 1,1,1-trifluoro-2,4- pentanedione (TFD), 1-phenyl-1,3-butanedione (PBD), and 1,3- diphenyl-1,3-propanedione (DBM) ligands. These materials are interesting from the point of view of potential applications for optical hole-burning frequency and time-domain storage and processing. Optical absorption, steady state and time-resolved photoluminescence, and spectral hole-burning at the transition between 3H6(1) and 3H4(1) crystal-field levels were studied at temperatures between 1.4 and 300 K.

DOI
10.1117/12.330415

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The optical properties of four Tm3+ chelates, specifically (beta) -diketone tris chelates of thulium, in a poly(methyl methacrylate) matrix are presented. Samples under investigation were the Tm3+ complexes formed using thulium chloride (TmCl3 (DOT) 6H2O) with thenoyltrifluoroacetylacetone (TTFA), 1,1,1-trifluoro-2,4- pentanedione (TFD), 1-phenyl-1,3-butanedione (PBD), and 1,3- diphenyl-1,3-propanedione (DBM) ligands. These materials are interesting from the point of view of potential applications for optical hole-burning frequency and time-domain storage and processing. Optical absorption, steady state and time-resolved photoluminescence, and spectral hole-burning at the transition between 3H6(1) and 3H4(1) crystal-field levels were studied at temperatures between 1.4 and 300 K.
Abstract : The optical properties of four Tm(3+) ion - organic ligand chelate complexes in a poly(methyl methacrylate) matrix were studied. These materials are interesting for potential applications of optical hole-burning frequency and time-domain storage and processing. Optical absorption, steady state and time-resolved photoluminescence, and spectral hole-burning at the transition between 3-H6 (1) and 3-H4 (1) crystal-field levels were studied at temperatures between 1.4 and 300 K. The heterodyne grating-generated scan interferometric technique has been demonstrated for the real time detection of the femtosecond data signal.
The zero-phonon line (ZPL) between the two excited-state manifolds 3F4 and 3H4 of the trivalent thulium ion in yttrium aluminum perovskite (Tm3+:YAlO3) lies within the telecom E-band at around 1451 nm and exhibits an optical coherence time of a few μs at cryogenic temperatures. To improve this time in view of potential applications, e.g. single-photon sources and optical quantum memory, we characterized the magnetic properties of the lowest Stark levels of these two manifolds. Varying the external magnetic field amplitude and orientation, we measured the enhanced nuclear Zeeman splitting by probing the field-dependent frequency detuning of side holes created by means of spectral hole burning, and we characterized the inhomogeneous line shift caused by the quadratic Zeeman interaction. Together, this allowed us to establish the spin Hamiltonians for the lowest Stark level of the 3F4 and 3H4 manifolds, and to predict optical clock transitions for particular orientations and magnitudes of the magnetic field
Spectral hole burning is reported for the trivalent thulium ion with measurements on the (3)H(6)(1) ? (3)H(4)(1) transition of LaF(3):Tm(3+) and two sites (A and B) of CaF(2):Tm(3+) at 1.5 K. Hole burning occurs by population storage in the metastable (3)F(4) level. The holes were scanned by an electric-field ramp applied directly to the sample, the frequency being calibrated by burning multiple holes with a frequency-modulated laser. This yielded the hole widths as well as the Stark coefficients for the transition studied, which are 8.3 kHz/V cm(-1) parallel to the C(2) axis (LaF(3):Tm(3+)) and for CaF(2):Tm(3+) are 25 kHz/V cm(-1) (site A), and 4.6 kHz/V cm(-1) (site B) for fields along the (001) direction. From the polarization behavior of the holes, the sites in CaF(2) are assigned to the F(-)-compensated C(4nu) and C(3nu) sites, respectively.
One very exciting application of laser spectroscopy would be to use the high-resolution capabilities of today’s lasers and the phenomenon of persistent spectral hole-burning to form a frequency domain optical storage system.1 In such a system, bits of information would be stored by locally modifying (in the frequency domain) the shape of an inhomogeneously broadened absorption line of an absorber in a solid at low temperatures. Because typical homogeneous widths are 1000X (or more) narrower than typical inhomogeneous widths, as many as 1000 bits could be written in one diffraction-limited 1-μm spot In a sample, yielding the impressive storage density of 1011 bits/cm2.
Over the report period, an optical laboratory for characterization materials for frequency domain optical storage was upgraded. Spectral and spectral hole burning properties were studied for several free-based and metallo-naphthalocyanine derivatives in polymer hosts. These materials exhibit a strong 0-0 absorption band and persistent hole burning in the region 800 nm. Hole burning parameters were determined for eight materials; in particular, the hole burning kinetics was analyzed and the quantum efficiencies were determined to be between 0.1% and 1%. Holograms (data pages) in the transmission geometry were successfully recorded in the materials studied using single frequency laser diodes. A photoluminescence of five natural diamonds (type Ia) implanted with Xe ions with dose range 1x10(exp 13) - 5x10(exp 14) /sq cm was investigated as a function of thermal annealing at temperatures between 300 and 1400 C.