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Optics Letters

Time-resolved subnatural-width spectroscopy

Harold J. Metcalf, William D. Phillips

Published Dec 1, 1980• 29 citations
Publisher

Abstract

Spectra that are narrower than the natural width of decaying states can be achieved by beginning the observation of signals at a fixed delay time after excitation rather than immediately afterward. These signals are weaker (and noisier) than the full, time-unresolved signals. Applications of this line-narrowing technique to precision spectroscopy are discussed, and the properties of the resulting signals are studied. Numerical simulations demonstrate that time-resolved line narrowing is highly desirable in a large number of cases.

DOI
10.1364/ol.5.000540

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Spectra that are narrower than the natural width of decaying states can be achieved by beginning the observation of signals at a fixed delay time after excitation rather than immediately afterward. These signals are weaker (and noisier) than the full, time-unresolved signals. Applications of this line-narrowing technique to precision spectroscopy are discussed, and the properties of the resulting signals are studied. Numerical simulations demonstrate that time-resolved line narrowing is highly desirable in a large number of cases.
The resolution of a quantum-beat experiment, which is basically limited by the atomic natural linewidth, has been improved by observing the fluorescence only from those atoms which have survived in excited states after some time delay. The resulting narrowing enables one to resolve previously overlapping lines in beam-foil quantum-beats experiments using $\mathrm{H}\ensuremath{\alpha}$ and 4He^{4}\mathrm{He}4He ii (4\ensuremath{\rightarrow}3) deexcitation.
A single photon, emitted in a transition between two states, has a frequency distribution of intensity that is given by a Lorentzian if the transition is only naturally broadened and the period of observation TTT is long compared to the lifetime T1{T}_{1}T1​ of the excited state. However, when the observation time TTT is short or comparable to T1{T}_{1}T1​, the frequency spectrum is appreciably broadened. If only the delayed part of the emitted radiation field is detected, then the radiation spectrum does not change. However, if the radiation field is transmitted through a resonant absorber and then detected, the transmission spectrum of the delayed radiation field is narrowed. We show that this narrowing is due to the interference of the spectral components of the incident and coherently scattered fields. Experimental spectra of absorption of M\"ossbauer radiation, obtained by the coincidence technique, confirm this conclusion.
Summary form only given. Spectral narrowing by recurrent use of free-decay signal in magnetic resonance has been proposed and demonstrated in the ground state of Rb atoms. In the present report we apply this technique to the measurement of the hyperfine frequency in the excited state. This is a sublevel spectroscopy with recurrent excitation where the atomic response is iteratively used as the next excitation. The hyperfine spectra of the excited state /sup 2/P/sub 3/2/ of the D/sub 2/ transition in /sup 85/Rb atoms, the line widths of which are much narrower than the natural width, were observed and the hyperfine constants of the excited state were determined precisely.
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: