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Coherent Phonon Generation and High Frequency Phonon Spectroscopy.

John E. Rives, Richard S. Meltzer, David Paul Landau

Published Mar 18, 1986• 0 citations
OpenAlex

Abstract

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.

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Quantum Electronics and Laser Science Conference•Jan 1, 2000•0 citations
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.
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 study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:
Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter.This is especially true for high frequency heat carrying phonons, which are intrinsic lattice vibrations experiencing many decoherence events with the environment, and are thus generally assumed to be incoherent.Two photon interference techniques, especially coherent population trapping (CPT) and electromagnetically induced transparency (EIT), have led to extremely sensitive detection, spectroscopy and metrology.Here, we propose the use of two photon interference in a three-level system to sense coherent phonons.Unlike prior works which have treated phonon coupling as damping, we account for coherent phonon coupling using a full quantum-mechanical treatment.We observe strong asymmetry in absorption spectrum in CPT and negative dispersion in EIT susceptibility in the presence of coherent phonon coupling which cannot be accounted for if only pure phonon damping is considered.Our proposal has application in sensing heat carrying coherent phonons effects and understanding coherent bosonic multi-pathway interference effects in three coupled oscillator systems.Phonons are packets of vibrational energy that shares many similarities with its bosonic cousin photons.Advances in nanofabrication has enabled many parallels between the development of photon and phonon control.Parallel developments in passive control techniques include photonic [1] versus phonoic crystals [2], optical [3] versus acoustic metamaterials [4] etc. Development in active manipulation of electromagnetic waves through light-matter interaction have led to creation of nanoscale optical emitters [5] and gates [6] and similar progress have been made in controlling phonons using their interaction with matter especially in the realms of optomechanics [7] and phononic devices [8,9].Phonons span a vast frequency range and while techniques to control and sense lower frequency coherent phonons have been well-developed [10-19], heat carrying coherent terahertz acoustic phonons have been harder to measure directly due to the small wavelength and numerous scattering mechanism at these small wavelengths [20].In the past, THz crystal phonons have been generated and detected in low temperature experiments with defect doped crystals [21-24], with experimental evidence of coherent phonon generation [25][26][27].At the same time, interpretation of non-equilibrium phonon transport, with the advancement of nanoscale electrical heating and ultrafast optical pump-probe techniques, have allowed us to infer phonon coherence from broadband thermal conductivity measurements [28][29][30][31][32].There have been also interest of using defect-based techniques as a thermal probe using perturbation to energy levels due to changes in temperature [33].Furthermore, surface deflection techniques with ultrafast optics have also been used to generate phonons close to THz frequencies in materials [34][35][36][37].Defect-based techniques are attractive compared to both thermal conductivity measurement and deflection techniques due to its ability to directly access atomic length scales where THz phonon wavelength resides.Also, the energy levels in the excited state [21,38,39] and ground state [25,40] electron manifold of these defects can match the phonon energy precisely, resulting in a narrow band phonon detector.In light of the success of defect-based optical absorption techniques in coupling directly to high frequency phonons, we propose the use of two photon interference to measure the coherence properties of these phonons.
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.
Summary form only given. If resonantly excited the effect of the longitudinal phonon mode is dominant resulting in an effective three-wave interaction. Photons are down converted between the optical waves while creating a coherent phonon emission via difference frequency mixing. If a phonon background is present and a single optical pulse is injected, a new down-shifted wave is generated. In any case a mutual locking of the two optical pulses can be observed although their group velocities are different. In the coherent case a subsequent up and down conversion occurs, where an equilibrium state of the field distribution is readily obtained for incoherent phonons. In the latter case the resulting rather stable bound state. The created pulses can be used to detect the density and spectral properties of the phonon background.