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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Spectral and Temporal Dynamics of Nonequilibrium Phonons in YAG:Pr3+

Xiaojun Wang, William M. Dennis

Published Jan 1, 1991• 0 citations
Publisher

Abstract

We have investigated the spectral and temporal dynamics associated with phonon decay in the YAG:Pr3+ system at a range of temperature between 9 and 25 K. Nonequilibrium phonons were generated using defect induced one phonon absorption (DIOPA) of far infrared (FIR) radiation1. Phonon detection was achieved optically using a variation of absorption vibronic sideband phonon spectroscopy2.

DOI
10.1364/pshb.1991.fc3

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We have investigated the spectral and temporal dynamics associated with phonon decay in the YAG:Pr3+ system at a range of temperature between 9 and 25 K. Nonequilibrium phonons were generated using defect induced one phonon absorption (DIOPA) of far infrared (FIR) radiation1. Phonon detection was achieved optically using a variation of absorption vibronic sideband phonon spectroscopy2.
The temporal evolution of nonequilibrium phonon populations in LaF3{\mathrm{LaF}}_{3}LaF3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+ is investigated at low temperatures (1.8 K) utilizing pulsed, tunable, monochromatic generation and time-resolved, tunable, narrow-band detection. High occupation number, narrow-band phonon populations are generated via far-infrared pumping of defect-induced one-phonon absorption. Time-resolved, frequency-selective detection is provided by optical sideband absorption. Nonequilibrium phonon decay times are measured and attributed to anharmonic decay.
We have investigated the spectral and temporal dynamics associated with the interaction between monochromatic and thermal phonon distributions in YAG:Pr3+{\mathrm{Pr}}^{3+}Pr3+. Using defect-induced one-phonon absorption to generate a monochromatic phonon distribution at 43.3 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, we measure a ${\mathit{T}}^{\mathrm{\ensuremath{-}}3}$ dependence of the monochromatic phonon lifetime in the temperature range 9 to 25 K. We observe the evolution of additional broadband phonon distributions which do not occur at low temperatures.
Defect-induced one-phonon absorption1 of far-infrared radiation is used to generate monochromatic nonequilibrium phonon populations in LaF3:Pr3+ at a range of frequencies throughout the acoustic band. The pump source for this generation mechanism is a transversely excited atmospheric-pressure CO2-laser-pumped superradiant cell. Phonon occupation numbers of order 10 are generated. Phonons are optically detected in a time-resolved frequency-selective manner by using the anti-Stokes absorption sideband of the 3P0 state of Pr3+. The lifetime of these phonons is determined and is found to obey the ω-5 dependence as predicted by the isotropic dispersionless model for anharmonic decay of acoustic phonons.2 The spectral dynamics associated with the decay of these phonons is also investigated and is compared with a rate-equation analysis that includes backfeeding of the decay products. The production of double-frequency phonons by a three-phonon confluence process is also demonstrated.
Defect-induced one-phonon absorption is used to generate high-occupation-number narrow-band nonequilibrium phonon populations at a range of frequencies in LaF3{\mathrm{LaF}}_{3}LaF3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. The spectral and temporal dynamics associated with the return to equilibrium of these phonons is observed. Processes that dominate the spectral evolution are shown to be narrow-band phonon confluence, anharmonic decay, and the broadband confluence of anharmonic decay products. The experimental data are shown to be in good agreement with a phonon-occupation-number rate-equation analysis that incudes the above processes.
A number of optical techniques have been developed in recent years which have been applied to study the dynamics of high frequency phonons. Monoenergetic phonons were generated by spin-lattice relaxation between two electronically excited states of an impurity ion. Resonant trapping provided the means to detect these phonons with good temporal resolution. VSPS was used to detect high frequency phonons over a wide frequency range with excellent temporal, spectral and spatial resolution. The life-time of a monoenergetic non-equilibrium distribution of phonons was determined by the observation of optical dephasing, using free induction decay(FID), which results from phonon induced coherence loss(PICOLO). Non-resonant fluorescence line narrowing(FLN) techniques provided a means to determine the spectral distribution of non-equilibrium phonons generated by spin lattice relaxation. Keywords: Phonons; Phonon decay; Coherent phonon generation; Phonon spectroscopy; High frequency phonons and Monoenergetic phonons.