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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

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

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

Published Jan 1, 1991• 0 citations
Publisher

Abstract

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

DOI
10.1364/pshb.1991.sa3

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It is important to compare dephasing mechanisms for ordered and disordered systems with a small and large inhomogeneous line broadening, respectively. We studied dephasing processes in crystals with Nd3+ ions by using the accumulated photon echo (APE) technique. Ordered (CaF2) and disordered (CaF2–YF3) crystals were chosen for investigations.

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Since the first observation of accumulated photon echoes by Hesslink and Wiersna [1], nearly transform-limited mode-locked pulse trains have been used as the excitation source, and the resolution times have been limited by the widths of the pulses. In this paper we show theoretically and experimentally that the time resolution of the accumulated photon echoes is determine not by the pulse width but by the correlation time of the excitation field [2]. This indicates that it is possible to obtain a sub-picosecond resolution in accumulated photon echoes Sven by using a cw laser (non-mode-locked), if the laser output has a sufficiently broad and smooth spectrum.

International Conference on Ultrafast Phenomena•Jan 1, 1984•0 citations

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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.

Journal of Experimental and Theoretical Physics•Jan 1, 1998•17 citations

Picosecond accumulated photon echo in Nd-doped optical fiber

Naoshi Uesugi, Makoto Shimizu, Masaharu Mitsunaga

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Quantum Electronics and Laser Science Conference•May 10, 1992•1 citation
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
The long-lived stimulated photon echo is put forward as a powerful technique to probe structural dynamics in glasses and other amorphous solids. We present results of optical dephasing measurements on several doped organic glasses (deuterated ethanol, toluene, and triethylamine) and polymers (polystyrene, polyvinylbutyral, and polymethylmethacrylate). Using a stochastic analysis within the so-called two-level-system model, we can extract from these measurements the distribution function of fluctuation rates over a huge range of time scales, varying from picoseconds to hundreds of milliseconds. We show that the dynamics, which lies at the origin of spectral diffusion, is very dependent on the glass structure and can be described by two separate hyperbolic distribution functions of fluctuation rates. From longitudinal photon echo measurements in the population dimension, we find evidence for structural dynamics which is not accounted for in the standard two-level-system model and which is related to a spatially inhomogeneous distribution of fluctuation centers.
Since the first observation of accumulated photon echoes by Hesslink and Wiersna [1], nearly transform-limited mode-locked pulse trains have been used as the excitation source, and the resolution times have been limited by the widths of the pulses. In this paper we show theoretically and experimentally that the time resolution of the accumulated photon echoes is determine not by the pulse width but by the correlation time of the excitation field [2]. This indicates that it is possible to obtain a sub-picosecond resolution in accumulated photon echoes Sven by using a cw laser (non-mode-locked), if the laser output has a sufficiently broad and smooth spectrum.
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.