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Le Journal de Physique Colloques

OPTICAL DEPHASING OF Pr3+ IONS BY NONEQUILIBRIUM PHONONS IN LaF3 AND YAlO3

R. M. Macfarlane, Richard S. Meltzer

Published Oct 1, 1985• 1 citation
Publisher

Abstract

We describe a new effect, phonon-induced coherence loss (PICOLO), whereby a monoenergetic nonequilibrium phonon distribution is responsible for the loss of optical coherence. The interaction of these phonons with the ions is monitored with the free induction decay or photon echo. We show how PICOLO can be used to study the electron-phonon interaction and the dynamics of phonons.

DOI
10.1051/jphyscol:1985746

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Low Temperature Physics•Sep 1, 1997•1 citation
We describe a new effect, phonon-induced coherence loss (PICOLO), whereby a monoenergetic nonequilibrium phonon distribution is responsible for the loss of optical coherence. The interaction of these phonons with the ions is monitored with the free induction decay or photon echo. We show how PICOLO can be used to study the electron-phonon interaction and the dynamics of phonons.
Phonon-induced coherence loss (PICL) is produced by a monoenergetic nonequilibrium distribution of phonons in LaF3{\mathrm{LaF}}_{3}LaF3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. The phonons are generated by relaxation between excited states of the Pr3+{\mathrm{Pr}}^{3+}Pr3+ ion after selective excitation with a pulsed, tunable dye laser. The optical dephasing is observed from the effect on the free-induction decay of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions whose excited-state level separation is resonant with the phonons. It is shown that PICL is a sensitive detector of monoenergetic phonons, and can be used to study phonon dynamics. The observed rate of optical dephasing is reduced relative to an equivalent occupation of 23-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ phonons produced thermally.
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.
The dephasing time of coherently prepared Pr3+{\mathrm{Pr}}^{3+}Pr3+ impurity ions in a La F3{\mathrm{F}}_{3}F3​ crystal is measured by optical free-induction decay. Above 4\ifmmode^\circ\else\textdegree\fi{}K, phonon processes severely shorten the decay time. Below 4\ifmmode^\circ\else\textdegree\fi{}K, we observe a temperature-independent decay time of 0.38 \ensuremath{\mu}sec. This is surprisingly short considering that there are no contributions from first-order hyperfine, phonon, or Pr3+{\mathrm{Pr}}^{3+}Pr3+-Pr3+{\mathrm{Pr}}^{3+}Pr3+ interactions.
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.
Experimental results on the investigation of low-temperature optical absorption spectra and temperature dependence of the photon echo (PE) amplitude signal in Y2SiO5:Pr3+ and LaF3:Pr3+ crystals at the transition H43(0)−3P0 of the Pr3+ ion are presented. It is shown that additional relaxation channels exist for PE in addition to the known phonon mechanisms. This is associated in a LaF3:Pr3+ crystal with the temperature variation of dipole moment at the Pr3+ ion transition. In a Y2SiO5:Pr3+ crystal, this is due to the thermally activated transitions for the Pr3+ ion between nonequivalent positions in the crystal lattice.