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IBM Journal of Research and Development

Subnanosecond Optical Free-Induction Decay

Ralph G. DeVoe, Richard G. Brewer

Published Sep 1, 1979• 1 citation
Publisher

Abstract

A novel form of laser frequency switching is devised that extends coherent optical transient studies to a 100-picosecond time scale, the measurements being performed in real time. Free-induction decay (FID) on a subnanosecond time scale reveals new features, such as a first-order FID that dephases with the inhomogeneous dephasing time T2* and interferes with the well-known nonlinear FID. A complete analytical expression for optical FID is derived and supports our FID observations for the sodium D1transition.

DOI
10.1147/rd.235.0527

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Journal of Physics D Applied Physics•Dec 14, 1990•4 citations
A novel form of laser frequency switching is devised that extends coherent optical transient studies to a 100-picosecond time scale, the measurements being performed in real time. Free-induction decay (FID) on a subnanosecond time scale reveals new features, such as a first-order FID that dephases with the inhomogeneous dephasing time T2* and interferes with the well-known nonlinear FID. A complete analytical expression for optical FID is derived and supports our FID observations for the sodium D1transition.
A novel form of laser frequency switching is devised which extends coherent optical transient studies to a 100-psec time scale. The technique incorporates a traveling-wave electro-optic element which imposes with unit efficiency a uniform time-varying phase and thus a frequency shift on a cw laser beam. In contrast to earlier optical traveling-wave modulators which are driven by a microwave oscillator, here the optical phase change is induced rapidly and easily by a dc electric field pulse that propagates in a microwave guide either parallel or antiparallel to the light wave. This advance enables optical free-induction decay (FID) studies on a subnanosecond time scale and reveals such new features as a rapid first-order FID that dephases with the inhomogeneous dephasing time T2∗{T}_{2}^{*}T2∗​. The well-known nonlinear FID can interfere with the first-order component at short times and decays over the much longer period $\frac{{T}_{2}}{[1+{(1+{\ensuremath{\chi}}^{2}{T}_{1}{T}_{2})}^{\frac{1}{2}}]}$, where $\ensuremath{\chi}$ is the Rabi frequency. A complete analytical expression is derived for optical FID of a transition subject to homogeneous and inhomogeneous broadening and supports detailed observations of the sodium D1{D}_{1}D1​ line.
By extending the laser-frequency-switching technique to a 100-psec time scale, we have observed for the Na D1{D}_{1}D1​ line the first-order free-induction decay, its inhomogeneous dephasing time T2∗{{T}_{2}}^{*}T2​∗, its interference with the nonlinear free-induction decay, and a 1.8-GHz interference beat of the ground-state hfs. Detailed theoretical predictions of these new coherence effects are faithfully observed.
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.
A new feature of optical free induction decay (FID) is observed in a coherently prepared sample of 13CH^{13}\mathrm{CH}13CH3F_{3}\mathrm{F}3​F by the method of Stark switching. The preparative phase is due to the resonant steady-state excitation by a cw laser beam, and is followed by FID upon sudden application of a dc Stark field that switches the molecular sample out of resonance. The emission is not observed as a simple decay but instead appears as a train of sharp pulses regularly spaced in time as a result of a repetitive interference. This situation arises because an entire set of infrared transitions within the Stark split manifold are initially prepared, in contrast to our previous study of a nondegenerate transition. The emission, which beats with the laser, produces a heterodyne beat spectrum, consisting of a set of regularly spaced frequencies, that is the Fourier transform of the slowly decaying pulse progression observed. We thus demonstrate what is the optical analog of the well-known NMR method of high-resolution pulse Fourier spectroscopy. The detailed behavior of the pulse train agrees well with an FID theory that assumes the transitions to be uncoupled. The subtle behavior of FID near the time origin is explored also by approximate analytic expressions that reveal either a near zero amplitude or sizable amplitude depending on the degree of saturation in the preparative stage. The experimental technique discussed offers an attractive way for obtaining high-resolution optical spectra without Doppler broadening, and for generating an optical pulse train whose time scale can be compressed by simply increasing the Stark field.
Using the time-dependent perturbation treatment of the density matrix, the authors report the occurrence of first-order free induction decay (FID) in narrow direct-gap semiconductors. The analysis deals with the interaction of a near resonant, ultrashort, moderate power laser pulse with the bulk semiconductor sample. Numerical estimates have been made for intrinsic InSb of micrometre size at 77 K irradiated by a frequency doubled 10.6 mu m CO 2 laser with pulse duration in the picosecond domain. The results reveal oscillations, around the background values, in the decay profiles of both the refractive index as well as the absorption coefficient. The transient transmitted intensity has been found to decay in a time comparable to the inhomogeneous Doppler broadening time, which is much shorter that the dephasing time. The analytical behaviour reported here is in very good agreement with the experimental observations of first-order FID in the atomic caesium vapour systems.