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Chinese Physics Letters

Fluorescence-Detected Ultrafast Free-Induction Decay in Powdered Rare Earth Solids

Qi Luo, De-chang Dai, Xiangyang Yu, Zhiren Qiu, Jianying Zhou, Chun‐Hua Yan, Zhi-da Chen

Published Feb 1, 2000• 6 citations
Publisher

Abstract

Fluorescence interferometry is developed and applied to study ultrafast amplitude and phase dynamics for free-induction decay in powdered rare earth solids. The time-resolved phase dynamics of free-induction decay through-out the decaying process is accurately determined by using a novel dual-channel correlation technique and subpicosecond dephasing time is measured for Nd 3+ solids at room temperature. The phase dynamics is well simulated with linear coherent polarization theory.

DOI
10.1088/0256-307x/17/2/009

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Physical Review A•Apr 1, 1978•65 citations
Fluorescence interferometry is developed and applied to study ultrafast amplitude and phase dynamics for free-induction decay in powdered rare earth solids. The time-resolved phase dynamics of free-induction decay through-out the decaying process is accurately determined by using a novel dual-channel correlation technique and subpicosecond dephasing time is measured for Nd 3+ solids at room temperature. The phase dynamics is well simulated with linear coherent polarization theory.
Coherent dynamic property of neodymium yttrium aluminum garnet (Nd:YAG) crystal at 77 K is studied via the conventional absorption, the femtosecond fringe-resolved wave packet interferometry, and the related difference-phase spectrum. The recorded interferogram exhibits beatings in subpicosecond time scale arising from the interferences among various weakly split 4f-electronic states and the coupled vibronic optical phonon sidebands. The electron–phonon coupling in Nd:YAG can be well described by multiple Brownian oscillators model involving in each individual electronic transition. The parameters for characterizing material coherence and relaxation are determined via the theoretical modelings of both the frequency and the time-domain experimental signals.
I. A new technique utilizing the electro-optic frequency switching of a single mode ( 6 Mhz) dye laser was used to observe free induction decay and optical nutation in iodine gas and optical nutation in an organic mixed crystal (pentacene in p-terphenyl) at low temperature. A new technique, incoherent resonance decay (IRO) was also developed. These experiments allow one to determine T_1 and T_2, the longitudinal and transverse relaxation times of the excited ensemble, in analogy with magnetic resonance. For I_2(g) at O∙C; T_l = 2.3 x 10^(-7) sec, T_2 ≃ 1 x 10^(-7) sec. These techniques are limited to a time scale > 10 nsec. II. The construction and characterization of cw, mode-locked dye laser capable of putting out a continuous train of reproducible sub-picosecond pulses is described. Experiments utilizing this laser for the measurement of picosecond coherent transients and time resolved absorption spectroscopy are proposed.
Femtosecond free induction decay (FID) beats were observed for the 4F3/2 - 4I9/2 transition of Nd3+ ions doped in Y3Al5O12 (YAG) crystal at room temperature using a mode-locked Ti3+:Al2O3 laser. This is the first observation of room-temperature dephasing processes in the time domain for rare-earth ion doped materials. The FID beat signal shows a dip structure produced by the interference between the pump pulse and the FID signal, and a quantum beat. The FID signal became large and comparable to the pump pulse as the crystal length was increased. The FID intensity evolution due to the pulse propagation is explained well by phenomenological equations.
Ultrafast phase dynamics of free-induction decay for carriers in bulk GaAs is studied with differential-phase spectroscopy. The instantaneous phase shifts of the free-induction decay with respect to the excitation pulses are extracted from simultaneously recorded laser pulse autocorrelation and free-induction decay in GaAs. Ultrafast phase dynamics during and immediately after the femtosecond pulse excitation are numerically evaluated with optical Bloch equations using pump pulse and semiconductor exciton parameters as input. Good agreement of the theory with experiment is obtained.
A simple method for observing coherent optical-transient phenomena is described. Effects such as photon echoes and free induction decay (FID) should allow studies of the dynamic properties of atoms, molecules, and solids on a time scale ranging from milliseconds to \ensuremath{\sim} 50 ps. The frequency of a cw dye laser is switched with an intracavity electro-optic modulator, producing in an external sample coherent transients which are detected in the forward beam. Measurements of long dephasing times are possible, as in FID, because the laser can oscillate indefinitely at the new frequency following a step-function switching pulse. Measurements of short decay times are also practical because the switching time is not restricted by the laser gain or cavity ringing time. In addition, the dye's dephasing time of a few picoseconds or less is too rapid to interfere with these observations. Since the pulse sequence can be preselected, the entire class of coherent optical transients is accessible. The method thus incorporates all of the advantages inherent in Stark switching, including heterodyne detection and high sensitivity, without being restricted to Stark-tunable systems. Laser frequency switching is discussed also in terms of a theoretical model which exposes the time-dependent properties of a phase-modulated cavity mode. Dephasing studies have been carried out thus far in atomic and molecular gases and low-temperature solids containing inorganic impurity ions or large organic molecules. The utility of the FID effect is emphasized where precise dephasing times are obtained from time-frequency Fourier transformation of FID signals using a digital computer. The first quantitative and detailed test of FID theory is provided by these experimental techniques.