Optics Letters

Measurement of optical homogeneous linewidths in a glass with picosecond accumulated photon echoes

Robert M. Shelby

Published Feb 1, 1983• 66 citations

Abstract

Picosecond accumulated photon echoes have been used to study optical dephasing in the (4)I(9/2)?(2)G(7/2), (4)G(5/2) transition of Nd(3+) in silicate glass. The homogeneous width exhibited a T(2.2)temperature dependence similar to that of other rare-earth systems previously studied by fluorescence line narrowing. The wavelength dependence of the echo-decay curves shows that relaxation among crystal-field states takes place in a few picoseconds.

DOI: 10.1364/ol.8.000088

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Optics Letters

Measurement of optical homogeneous linewidths in a glass with picosecond accumulated photon echoes

Robert M. Shelby

Published Feb 1, 1983• 66 citations

Publisher

Abstract

DOI: 10.1364/ol.8.000088

Related papers

Accumulated photon echoes as a probe of radiationless relaxation processes in Nd-doped glasses

Keith W. Ver Steeg, Roger J. Reeves, Richard C. Powell

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.1,2Accumulated 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

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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 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.

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Ryuzi Yano, Naoshi Uesugi

Measurements of the homogeneous width of the $^{4}$ ${\mathrm{G}}_{5\mathrm{/}2}$ , $^{2}$ ${\mathrm{G}}_{7\mathrm{/}2}$ ${\mathrm{\ensuremath{-}}}^{4}$ ${\mathrm{I}}_{9\mathrm{/}2}$ transition of ${\mathrm{Nd}}^{3+}$ in a silicate glass fiber at low temperatures by the technique of accumulated photon echoes show that the dephasing processes are one-phonon processes between the Stark levels of ${\mathrm{Nd}}^{3+}$ . These dephasing processes differ from the commonly observed processes of rare-earth ion-doped glasses: the local-configurational-change-induced dephasing process and the Raman process with low-frequency modes. The densely distributed Stark levels of the $^{4}$ ${\mathrm{G}}_{5\mathrm{/}2}$ and $^{2}$ ${\mathrm{G}}_{7\mathrm{/}2}$ states are responsible for one-phonon processes. The transition-wavelength dependences of the homogeneous widths ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (4.2 K) and ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (T\ensuremath{\rightarrow}0) are explained by using the one-phonon process model.Measurements of the homogeneous width of the $^{4}$ ${\mathrm{G}}_{5\mathrm{/}2}$ , $^{2}$ ${\mathrm{G}}_{7\mathrm{/}2}$ ${\mathrm{\ensuremath{-}}}^{4}$ ${\mathrm{I}}_{9\mathrm{/}2}$ transition of ${\mathrm{Nd}}^{3+}$ in a silicate glass fiber at low temperatures by the technique of accumulated photon echoes show that the dephasing processes are one-phonon processes between the Stark levels of ${\mathrm{Nd}}^{3+}$ . These dephasing processes differ from the commonly observed processes of rare-earth ion-doped glasses: the local-configurational-change-induced dephasing process and the Raman process with low-frequency modes. The densely distributed Stark levels of the $^{4}$ ${\mathrm{G}}_{5\mathrm{/}2}$ and $^{2}$ ${\mathrm{G}}_{7\mathrm{/}2}$ states are responsible for one-phonon processes. The transition-wavelength dependences of the homogeneous widths ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (4.2 K) and ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (T\ensuremath{\rightarrow}0) are explained by using the one-phonon process model.

Physical review. B, Condensed matterMar 1, 19976 citations

The temperature-dependent homogeneous width of the

^{5}

${\mathit{D}}_{0\mathrm{\ensuremath{-}}}^{7}$

{\mathit{F}}_{0}

transition of

{\mathrm{Eu}}^{3+}

in a pure silicate glass fiber has been measured by accumulated photon echoes between 1.6 and 44 K. The temperature dependence of the homogeneous width shows a crossover from T-linear (T7 K) to

{\mathit{T}}^{2}

(T>7 K). The whole temperature dependence of the homogeneous width between 1.6 and 44 K can be explained by the configurational changes of the glass which is modeled by two-level systems (TLS's) and a Raman process involving low-frequency vibrational modes of the silicate glass (the rotations of

{\mathrm{SiO}}_{4}

tetrahedra). The T-linear temperature dependence is attributed to the TLS process. The anomalous

{\mathit{T}}^{2}

dependence down to 10 K cannot be explained by only one process, but can be explained by the contributions of both the TLS process and the Raman process. Above 40 K, the Raman process becomes the dominant dephasing mechanism.

Measurements of the homogeneous width of the

^{4}

{\mathrm{G}}_{5\mathrm{/}2}

^{2}

{\mathrm{G}}_{7\mathrm{/}2}

${\mathrm{\ensuremath{-}}}^{4}$

{\mathrm{I}}_{9\mathrm{/}2}

transition of

{\mathrm{Nd}}^{3+}

in a silicate glass fiber at low temperatures by the technique of accumulated photon echoes show that the dephasing processes are one-phonon processes between the Stark levels of

{\mathrm{Nd}}^{3+}

. These dephasing processes differ from the commonly observed processes of rare-earth ion-doped glasses: the local-configurational-change-induced dephasing process and the Raman process with low-frequency modes. The densely distributed Stark levels of the

^{4}

{\mathrm{G}}_{5\mathrm{/}2}

and

^{2}

{\mathrm{G}}_{7\mathrm{/}2}

states are responsible for one-phonon processes. The transition-wavelength dependences of the homogeneous widths ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (4.2 K) and ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (T\ensuremath{\rightarrow}0) are explained by using the one-phonon process model.