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Optics Letters

Spectral hole burning in thulium-doped glass ceramics

R. M. Macfarlane, Matthew J. Dejneka

Published Apr 1, 2001• 21 citations
Publisher

Abstract

We have used spectral hole burning to measure the homogeneous linewidth of the (3)H(6)(1)- (3)F(3)(1) transition of Tm(3+) ions doped into oxyfluoride glass ceramics consisting of nanocrystals of LaF(3) in an aluminosilicate glass matrix. From the magnitude of the hole width in the nanocrystals and its dependence on temperature, we propose that excitation of tunneling modes in the adjacent glassy phase as well as of confined mechanical modes in the nanocrystals is responsible for the broadening.

DOI
10.1364/ol.26.000429

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Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1992•0 citations
We have used spectral hole burning to measure the homogeneous linewidth of the (3)H(6)(1)- (3)F(3)(1) transition of Tm(3+) ions doped into oxyfluoride glass ceramics consisting of nanocrystals of LaF(3) in an aluminosilicate glass matrix. From the magnitude of the hole width in the nanocrystals and its dependence on temperature, we propose that excitation of tunneling modes in the adjacent glassy phase as well as of confined mechanical modes in the nanocrystals is responsible for the broadening.
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 observation of statistical absorption fluctuations of an inhomogeneously broadened optical transition in a glass is reported. Frequency modulation spectroscopy in a 10-ppm Nd3+{\mathrm{Nd}}^{3+}Nd3+-doped-silica optical fiber has also revealed spectral holes that persist for days at 4.2 K. Homogeneous linewidths ${\ensuremath{\Gamma}}_{h}$ measured using hole burning and fluctuations are in good mutual agreement but are significantly larger than those inferred from photon echo decays in the same system. This difference confirms recent predictions of a time-dependent ${\ensuremath{\Gamma}}_{h}$(t) arising from the tunneling dynamics of the glass.
Optical dephasing of Pr3+ and Tm3+ ions doped in transparent oxyfluoride glass ceramics was studied with the two-pulse photon echo technique. It was found that the dephasing time of rare earth ions is dramatically less in nanocrystals embedded in a glass matrix than in bulk crystals. A quasi-linear temperature dependence obtained at low temperatures proved that the long-range interaction of the ions inside the nanocrystals with the two level systems of the glass matrix dominates the optical dephasing. The local thermal effect in glass ceramics containing nanocrystals elevates the local temperature, which results in the reduction of optical dephasing time. For Tm(3+)-doped glass ceramics, the elevation of local temperature induced by the irradiation of excitation laser even quenched the photon echo signals in the experimental study.
Persistent spectral hole burning is observed in Sm(2+)-doped glasses at room temperature. The holes are burned in the (7)F(0) ? (5)D(0), (5)D(1) lines of the Sm(2+) ions in three kinds of fluoride glass. The dependence of the burning efficiency on the sample and on the burning intensity is measured. The intensity dependence is approximately linear, and no antihole is observed around the burned hole. The hole-burning mechanism is discussed. The temperature dependence of the homogeneous width is also measured.
Persistent spectral hole burning (PSHB) in the ${}^{7}{F}_{0}{\ensuremath{-}}^{5}{D}_{0}$ transition and the electron excitation in the ${}^{7}{F}_{0}\ensuremath{-}4f5d$ transition of Sm2+{\mathrm{Sm}}^{2+}Sm2+ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses were studied from the measurements of hole burning efficiency and the refilling of the burnt hole. The PSHB at low temperature is attributed to the optically activated rearrangement of OH bonds surrounding Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions. On the other hand, the PSHB at high temperature is attributed to one-step electron tunneling in the excitation state. The barrier heights for hole filling corresponding to the two mechanisms were determined to be \ensuremath{\sim}0.27 and \ensuremath{\sim}0.90 eV, respectively. Thermal depth of the trap that captures electrons by two-step ionization via the 4f5d4f5d4f5d state was determined to be \ensuremath{\sim}0.35 eV below the conduction band. A model was proposed for describing the PSHB and electron excitation of Sm2+{\mathrm{Sm}}^{2+}Sm2+ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses. In addition, the dependence of hole burning efficiency on the Al2O3{\mathrm{Al}}_{2}{\mathrm{O}}_{3}Al2​O3​ concentration, temperature, and burning wavelength was also studied.