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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Accumulated Photon Echo Spectroscopy of Ordered (CaF2) and Disordered (CaF2-YF3) crystals with Nd3+ ions

Keith W. Ver Steeg, R. J. Reeves, V.V. Fedorov, Alexander Ya. Karasik, Tasoltan T. Basiev, Richard C. Powell

Published Jan 1, 1994• 0 citations
Publisher

Abstract

Numerous experimental investigations of homogeneous line broadening (Γh) of RE3+ ions in crystals and glasses in frequency and time domain [1] have shown that Γh for glasses exceed those for crystals by more than one order of magnitude at low temperatures (T) for the same ions and transitions. Discrepancies between theory and experimental results make it difficult to determine an influence of host disordering on the Γh in a wide temperature range. In this work we measured and compared Γh, values for ordered CaF2 and disordered CaF2-YF3 crystals doped with Nd3+ ions.

DOI
10.1364/shbs.1994.wd32

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Numerous experimental investigations of homogeneous line broadening (Γh) of RE3+ ions in crystals and glasses in frequency and time domain [1] have shown that Γh for glasses exceed those for crystals by more than one order of magnitude at low temperatures (T) for the same ions and transitions. Discrepancies between theory and experimental results make it difficult to determine an influence of host disordering on the Γh in a wide temperature range. In this work we measured and compared Γh, values for ordered CaF2 and disordered CaF2-YF3 crystals doped with Nd3+ ions.
Accumulated photon echoes have been used to investigate the mechanisms of optical dephasing in CaF2 crystals activated by Nd3+ ions. Tunable picosecond laser radiation, which permits the selective excitation of various Nd3+ optical centers in the 4 I 9/2→4 G 5/2, 2 G 7/2 transition, is used. The optical phase relaxation times measured at temperatures from 9 to 50 K permit determination of the homogeneous widths of the transitions between the low-lying 4 I 9/2 Stark level and three excited 4 G 5/2, 2 G 7/2 levels, and calculation of the constants of the inter-Stark relaxation transitions in the ground and excited multiplets for the rhombic N and M Nd3+ centers in CaF2 crystals. An analysis of the temperature dependence of the homogeneous linewidth of the transitions between low-lying Stark levels of the ground and excited states shows that the mechanism of optical dephasing in the crystals investigated is described well by direct relaxation processes with resonant inter-Stark absorption of one phonon in the ground and excited states. At T=9 K, the homogeneous linewidth Γh in CaF2 crystals is almost an order of magnitude smaller than Γh in disordered CaF2-YF3 crystals. This difference can be attributed to the significantly greater spectral phonon density of states in disordered crystals.
Accumulated photon echoes (APE) were used to measure the dephasing rates of Nd3+ in various inorganic glasses as a function of excitation wavelength, sample temperature, and laser power. Although dephasing processes of optical transitions in solids are of considerable interest, they are poorly understood, largely due to the lack of experimental data on femtosecond and picosecond time scales. The APE technique using sub-picosecond laser sources has made it possible to measure in the time domain dephasing rates of inhomogeneously broadened transitions in amorphous systems.1,2
Accumulated photon echoes were used to measure the dephasing time (T2{\mathit{T}}_{2}T2​) of the 4^{4}4I9/2{\mathit{I}}_{9/2}I9/2​${\ensuremath{\rightarrow}}^{4}$G5/2{\mathit{G}}_{5/2}G5/2​,2{,}^{2},2G7/2{\mathit{G}}_{7/2}G7/2​ transition of Nd3+{\mathrm{Nd}}^{3+}Nd3+ in highly disordered CaF2{\mathrm{CaF}}_{2}CaF2​-YF3{\mathrm{YF}}_{3}YF3​ crystals. T2{\mathit{T}}_{2}T2​ decreased from subnanosecond values for excitation of low-lying Stark levels to subpicosecond values for excitation of high-lying levels. From 9--100 K the measured temperature dependence of the homogeneous linewidth is described by a resonant single-phonon absorption process.