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Physical Review A

Interference and stabilization in the quasibound Stark spectrum

Christian Chardonnet, Dominique Delande, J. C. Gay

Published Feb 1, 1989• 15 citations
Publisher

Abstract

Experimental studies of the quasibound Stark spectrum of cesium are reported with emphasis on the Stark redistribution of nonhydrogenic states onto the linear Stark manifold. We show that most characteristics of the spectra are understood with analytical models describing the interaction of one or several discrete states with one or several quasicontinua of discrete states. In particular, we give experimental evidence for the discrete versions of Fano profiles and stabilization of states due to interference effects. These are also important features of the continuum region which several experiments have recently demonstrated.

DOI
10.1103/physreva.39.1066

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Experimental studies of the quasibound Stark spectrum of cesium are reported with emphasis on the Stark redistribution of nonhydrogenic states onto the linear Stark manifold. We show that most characteristics of the spectra are understood with analytical models describing the interaction of one or several discrete states with one or several quasicontinua of discrete states. In particular, we give experimental evidence for the discrete versions of Fano profiles and stabilization of states due to interference effects. These are also important features of the continuum region which several experiments have recently demonstrated.
We have studied experimentally and theoretically two-step photoionization through the 3P state of sodium in an electric field of up to 3.90 kV/cm. The apparatus uses an atomic beam crossed by two pulsed laser beams, one at 589 nm for the first step, and the other swept through the zero field threshold Eo near 409 nm for the ionization. We observe broad undulations in the photocurrent above Eo that narrow with decreasing energy and eventually sharpen into well-defined but asymmetric transitions to Stark-shifted Rydberg states. We calculate the oscillator strength density for the appropriate transitions using modified hydrogenic wave functions and find excellent agreement for the position and relative strength of all the spectral features. We model the asymmetries as Fano-type interferences between quasi-discrete and continuum ionization channels. Using appropriate core potentials, and taking into account core-induced coupling of both discrete-to-continuum and continuum-to-continuum states, we obtain estimates of Fano's q and Ɖ that agree reasonably well with our measurements.
Fano resonance is a well-celebrated weak-coupling phenomenon whereby a small interaction between a discrete and a continuum of excited states leads to an interference between the respective two transition amplitudes, resulting in an asymmetric line shape in the excitation spectra. We present the strong-coupling phase of the Fano's model where the interaction is localized in a region $\ensuremath{\xi}$ that is smaller than the collective coupling between the discrete state and the continuum. We explore the behavior of the excitation probability $\ensuremath{\sigma}$ as a function of $\ensuremath{\xi}$, the ratio of the bare transition amplitudes, and the energy of the discrete state. In the strong-coupling phase, the spectral function of the discrete state splits up and produces up to three complete destructive interferences or zeros of $\ensuremath{\sigma}$ along with ultrasharp features. We also find that the discrete state does not have to lie within the continuum to produce the well-known weak-coupling profiles of $\ensuremath{\sigma}$ as long as the collective coupling is strong enough. In addition, we consider a broadened state instead of a continuum and present a method that exactly treats such cases by explicitly including the source of the broadening---a weak coupling to the continuum of environment states---in the model.
A theory of nonhydrogenic Stark spectra based on the hydrogen atom is specialized to quasidiscrete levels. Algebraic expressions for level positions ${\ensuremath{\epsilon}}_{r}$, widths ${\ensuremath{\Gamma}}_{r}$, and oscillator strengths frF{f}_{r}^{F}frF​ are derived in terms of matrices HF{\mathit{H}}^{F}HF and hF{\mathit{h}}^{F}hF, which represent the hydrogenic density of states in a Stark field FFF. Core effects appear through zero-field quantum defects ${\ensuremath{\mu}}_{l}$ and dipole matrix elements dl0{d}_{l}^{0}dl0​. Normalized oscillator strengths f‾rF{\overline{f}}_{r}^{F}f​rF​ are defined which are independent of all dl0{d}_{l}^{0}dl0​ for $s\ensuremath{\rightarrow}p$ transitions. Isolated and interacting Stark manifolds with m=0and1m=0 \mathrm{and} 1m=0and1 are examined for systems with two nonnegligible ${\ensuremath{\mu}}_{l}$. Extensive comparisons are made with experimental Li spectra and matrix-diagonalization calculations of Zimmerman, Littman, Kash, and Kleppner [Phys. Rev. A 20, 2251 (1979); ZLKK]. For small fields F<13n5F<\frac{1}{3{n}^{5}}F<3n51​ level positions are given analytically with respect to H levels of fixed nnn; m=0m=0m=0 intensity distributions do not appear hydrogenic in Li since ${\ensuremath{\mu}}_{0}\ensuremath{\sim}\frac{1}{2}$. At F>13n5F>\frac{1}{3{n}^{5}}F>3n51​, degenerate parabolic eigenstates from different manifolds are coupled by the spherical core and avoid crossing. The upper levels disappear at m=1m=1m=1 anticrossings in Li, as observed in ZLKK. For m=0m=0m=0 the lower levels usually vanish instead. A full Stark map of calculated intensities f‾rF{\overline{f}}_{r}^{F}f​rF​ is presented for Li (m=0m=0m=0) and agrees with experiment. Pseudocrossings occur at near triple degeneracies of hydrogen Stark states. Extensions to include ls\mathrm{ls}ls coupling are indicated. Experimental ionization rates in He are analyzed in a companion paper by van de Water, Mariani, and Koch [Phys. Rev. A 30, 2399 (1984)].
Stark spectra of barium Rydberg states above the classical field-ionization limit have been recorded at high density of states employing high-resolution laser spectroscopy. The spectra, taken at a binding energy of about \ensuremath{\varepsilon}\ensuremath{\approxeq}-55 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with respect to zero-field threshold and at electric-field strengths F\ensuremath{\approxeq}100 V/cm exhibit dramatic variations in line profiles with increasing external field strength. The WKB quantum-defect theory of the Stark effect of nonhydrogenic atoms was used to analyze the recorded spectra, and excellent agreement between measured and calculated line profiles was achieved. Core-induced coupling of closed and open hydrogenic Stark channels was found to contribute dominantly to the linewidth of the recorded Stark resonances. In addition, a reformulation of this theory by McNicholl, Ivri, and Bergeman (unpublished) in terms of a configuration-interaction model was employed to analyze a particular avoided crossing of several Stark components. In this way recorded line profiles were parametrized within a limited model to obtain resonance energies, linewidths, and Fano q parameters.