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Optics Letters

Spectral hole burning in the trivalent thulium ion

R. M. Macfarlane

Published May 15, 1993• 25 citations
Publisher

Abstract

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.

DOI
10.1364/ol.18.000829

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•Oct 8, 1999•0 citations
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.
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.
4fn ⇒ 4fn transitions of trivalent rare earth ions doped in crystals frequently give sharp spectral lines. The transitions associated with the higher levels of a multiplet can be relatively sharp, 10-1000 GHz, where the width is determined by the decay rate of the levels by spontaneous phonon emission to lower levels. The transitions and their linewidth can be determined using conventional absorption or excitation techniques. On the other hand the transitions associated with the meta-stable lower levels typically give much sharper features with linewidths of 1 - 100 GHz and the widths are determined by the inhomogeneities of the crystal field. These inhomogeneous linewdths can be obtained by conventional spectroscopic techniques but the homogeneous linewidth requires more innovative techniques such as optical holeburning or photon echoes. The time domain photon echo measurements do not requiring a high resolution source and have frequently been used to establish that the homogeneous linewidth of such transitions. The lines can be very narrow down to the kHz regime [1,2]. Should complimentary measurements be attempted in the frequency domain utilising holeburning a special frequency stabilised lasers is required and one has been developed in association with the current work [3].
Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of Eu2+{\mathrm{Eu}}^{2+}Eu2+ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable 4f65d{4f}^{6}5d4f65d excited state to the conduction band followed by electron transport to Eu3+{\mathrm{Eu}}^{3+}Eu3+ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the Eu2+{\mathrm{Eu}}^{2+}Eu2+ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.
We report what is believed to be the first demonstration of laser frequency stabilization directly to persistent spectral holes in a solid-state material. The frequency reference material was deuterated CaF(2): Tm(3+) prepared with 25-MHz-wide persistent spectral holes on the H(6)(3)?H(4)(3) transition at 798 nm. The beat frequency between two lasers that were independently locked to persistent spectral holes in separate crystal samples showed typical root Allan variances of 780+/-120Hz for 20-50-ms integration times.
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.