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Physical Review A

Theorem on coherent transients

Axel Schenzle, N. C. Wong, Richard G. Brewer

Published Aug 1, 1980• 44 citations
Publisher

Abstract

A fundamental theorem in nuclear magnetic resonance and quantum optics is derived for an atomic system subject to inhomogeneous broadening and coherent preparation by a pulsed electromagnetic field of arbitrary shape. We show that the coherent emission, free induction decay or echo, which follows is confined to an interval which precisely equals the duration of the applied pulse sequence. The theorem applies to two-level or multilevel transitions for which the inhomogeneous linewidth is infinitely broad and the sample is optically thin.

DOI
10.1103/physreva.22.635

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Physical Review A•Dec 1, 1972•312 citations
A fundamental theorem in nuclear magnetic resonance and quantum optics is derived for an atomic system subject to inhomogeneous broadening and coherent preparation by a pulsed electromagnetic field of arbitrary shape. We show that the coherent emission, free induction decay or echo, which follows is confined to an interval which precisely equals the duration of the applied pulse sequence. The theorem applies to two-level or multilevel transitions for which the inhomogeneous linewidth is infinitely broad and the sample is optically thin.
A general expression for coherent transients, free induction decay and echoes, of an atomic or spin two-level system excited by resonant laser or rf field in the form of two square pulses is given by using the Fourier-transform method. This expression interprets the main characteristics of the transient signals well. An analytic expression for the shapes of two-pulse echoes is derived by assuming infinite inhomogeneity and the same Rabi frequencies for the two pulses. Two-pulse echo shapes were numerically calculated for various combinations of pulse areas by using the analytic expression. Nuclear-magnetic-resonance experiment was carried out on an inhomogeneously broadened proton spin system. Experimental two-pulse echo shapes are compared with the calculated ones. Agreement between theory and experiment is quite excellent.
Large-amplitude oscillations are predicted in the free-induction decay (FID) of atomic or spin two-level quantum systems that are coherently prepared by a resonant electromagnetic field in the form of a square amplitude pulse of duration TTT. The effect should be detectable in nuclear magnetic resonance (NMR) or in optical resonance experiments when the transition line shape is inhomogeneously broadened (${T}_{2}^{*}\ensuremath{\ll}{T}_{2}$) and the applied field is intense enough that the pulse area $\ensuremath{\chi}T\ensuremath{\ge}2\ensuremath{\pi}$, where $\ensuremath{\chi}$ is the Rabi frequency. Physically, the effect is due to Rabi oscillations which are generated in the preparative stage and are then reproduced because of atomic memory in the radiative period which follows. The atomic polarization derived from the Bloch equations assumes the form of an integral over the inhomogeneous line shape, and can be evaluated numerically for arbitrary linewidth $\ensuremath{\sigma}$ or analytically when $\ensuremath{\sigma}\ensuremath{\rightarrow}\ensuremath{\infty}$. The characteristics of the oscillation are unusual since the oscillation frequency, which is of order $\ensuremath{\chi}$, increases with time while the oscillation envelope vanishes identically for times $t\ensuremath{\ge}2T$. Coherent emission is therefore confined to one pulse width TTT immediately following the pulse. Previous NMR and infrared FID experiments with small-area pulses ($\ensuremath{\chi}T\ensuremath{\le}4\ensuremath{\pi}$), interpreted erroneously in terms of an edge echo effect, support the oscillatory FID behavior described here. For the case $\ensuremath{\chi}T>4\ensuremath{\pi}$, an experimental test would be even more decisive, as the oscillations are more pronounced.
The dynamics of nuclear spins in atomic and molecular environments have been examined in exquisite detail over the past 27 years by the methods of pulsed nuclear magnetic resonance. The early discovery of the spin echo by Erwin Hahn and the transient nutation effect by Henry Torrey initiated the field by introducing coherent transient phenomena to radio-frequency spectroscopy. An entire class of coherent spin transients could be observed by a simple variation of the rf pulse sequence, and from the decay characteristics the various spin-dephasing mechanisms could be examined separately. In short, these methods allowed decomposition of the spin-transition linewidth into its broadening components, and also offered new and versatile ways for performing high-resolution rf spectroscopy.
Oscillatory free-induction decay (FID) theoretically predicted by Schenzle, Wong, and Brewer was observed by using NMR in an inhomogeneously broadened proton system. Oscillatory behaviors were also observed, in the same system, in two-pulse echoes generated by large-area pulses. These phenomena appear in a highly inhomogeneous-broadened atomic or spin two-level system driven by resonant laser or rf pulses with areas equal to or larger than $2\ensuremath{\pi}$. Detailed studies were made for spin-locked and notched echoes. Behaviors of the oscillatory FID and the oscillatory echoes were theoretically examined by solving the Bloch equations and numerically integrating the solution over the inhomogeneous broadening. Excellent agreement between experiment and theory was obtained. Analytic expressions for the shapes of the locked- and notched-type echoes are obtained, which interpret the main characteristics of these echoes, when the infinite linewidth of the inhomogeneous broadening and the $\ensuremath{\delta}$-function-type excitation for one of the pulses are assumed.
The increasing interest in the study of the interaction of several resonant fields with multilevel quantum systems is due to a wide range of possible applications of various effects observed in the multi-frequency excitation of quantum objects. Among them, we can note color echo holography, information compression in three-level environments, copying of quantum information, and multi-level quantum gates that perform logical operations. In addition, the recording and reproduction of echo holograms in multi-level systems leads to the possibility, along with logical operations, to perform a change in the real-time scale and the sequence of events in the echo-hologram response, the data on which were embedded into the temporal structure of the object laser pulse. The formation of optical transient processes in multilevel systems occurs when the short laser pulses separated in time and resonant of different frequency transitions at the substance have an effect on the system, so that their interaction with each other becomes possible only through the medium and only if the medium has a sufficiently long phase memory. In this situation, each laser pulse transmits information about its wave characteristics to the medium, and this information is retained here until the arrival of the next laser pulses. The formation of optical transient processes in a multilevel system in a solid depends essentially on the degree of correlation of the inhomogeneous broadening on different frequency transitions and different time intervals, in connection with the possible destruction of the reversible phase memory of the system due to a partial mutual fixation energies of transitions. The influence of external spatially inhomogeneous electric fields on the resonant medium can lead to an additional artificially created inhomogeneous broadening. In this case, it is possible to control the phase memory of the system by changing the parameters of external spatially inhomogeneous electric fields, and the most pronounced effect on phase memory is the case of laser excitation of narrow frequency regions of inhomogeneously broadened lines of the resonance transitions. Moreover, the artificially created inhomogeneous broadening by external spatially inhomogeneous electric fields due to the Stark effect can be comparable with the spread of frequencies due to a partial mutual fixation of the transition energies, which leads to a partial restoration of the coherence of the multilevel system. This effect can lead to an increase in the intensity of the response of the stimulated photon echo (SPE) in the three-level system, which is the opposite effect of photon echo locking.
A simple application of the Stark-pulse technique, developed by Brewer and Shoemaker, demonstrates optical free induction decay-the optical analog of free induction decay in NMR. A molecular sample which is coherently prepared by a cw laser beam exhibits such a decay when it is suddenly switched out of resonance by a Stark field. Observations are presented for a nondegenerate Doppler-broadened infrared transition of NH2{\mathrm{H}}_{2}H2​D, where the sample is optically thin, and the decay behavior can be compared quantitatively with a solution of the Bloch equations. When the molecular sample is prepared under steady-state conditions, the solutions are analytic; for pulse excitation, a numerical solution is required. The treatment invokes a hard-collision relaxation model. Such characteristics as the abrupt termination of the decay and the related edge echo, which result from Doppler dephasing, can be examined for Stark pulses of finite extent.