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Physical Review A

Technique for measuring the linewidth of autoionizing Rydberg states

Grzegorz Waligorski, Lei Zhou, William E. Cooke

Published Feb 1, 1997• 6 citations
Publisher

Abstract

We present a variation of the isolated-core excitation (ICE) method that measures the linewidths of autoionizing resonances regardless of the limitations imposed by an instrumental linewidth. By exciting an autoionizing state via different ICE satellite transitions, we determine the linewidth of the state from Fano q values of asymmetric spectral profiles. Since the Fano q is insensitive to instrumental broadening, we can measure autoionizing resonance linewidths below the bandwidth of our laser.

DOI
10.1103/physreva.55.1544

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We present a variation of the isolated-core excitation (ICE) method that measures the linewidths of autoionizing resonances regardless of the limitations imposed by an instrumental linewidth. By exciting an autoionizing state via different ICE satellite transitions, we determine the linewidth of the state from Fano q values of asymmetric spectral profiles. Since the Fano q is insensitive to instrumental broadening, we can measure autoionizing resonance linewidths below the bandwidth of our laser.
In the study of Yb atomic Rydberg states, new members of 6sns 1 S 0 series for n=23, 24, 66-116 and 6snd 1 D 2 series for n=81-114 were observed. The data are in excellent agreement with the MQDT analysing results. The autoionizing Rydberg series 6p 1 2 /n's ( 1/2 , 1/2 ) 1 0 were investigated by three-step laser excitation. The ICE model was used to explain the experimental spectrum, and it has been proved to be suitable for describing the excitation of the autoionizing Rydberg states with a weakly-excited core.
Photon absorption spectroscopy is a powerful tool for uncovering the structure of atoms, molecules, and solids. Symmetric Lorentzian and asymmetric Fano line shapes are fundamental spectroscopic signatures related to the structural and dynamical properties. Recently, Ott et al. [Science 340, 716 (2013)] successfully transferred Fano profile into Lorentzian line shape using an intense infrared laser, after excitation of autoionizing states in helium by attosecond XUV pulse. This is a very important step forward in quantum phase control. However, here we show experimentally that an autoionizing state can have both Fano and Lorentzian behavior naturally, depending on the process involved. This study utilized the inverse process of photon absorption ionization, i.e., electron ion recombination with photon emission, making sure the resonant autoionizing state is not modified or decorated by the laser fields. Our result implies that excitation of the state through different paths---for example, one photon versus multiphoton excitation, or even one step versus multistep excitation---can lead to different Fano profiles for the same resonant state. We also report an experimental determination of the energy shifts in the recombination photon-intensity peaks due to the interference between the resonant and nonresonant processes.
We study, using a combination of experiment and theory, the excitation and decay of very-high-$n\phantom{\rule{4pt}{0ex}}(n\ensuremath{\sim}280\text{--}430)$ strontium autoionizing Rydberg states formed by near-resonant driving of the $5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2}\ensuremath{\rightarrow}5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}$ core-ion transition. The branching ratio between decay through radiative transitions and through autoionization is explored. Autoionization rates are measured as a function of both the nnn and $\ensuremath{\ell}$ quantum numbers of the Rydberg electron. The nonstationary decay dynamics is studied by creating and manipulating Rydberg wave packets and by varying the laser pulse that drives the core excitation.
When two levels can be strongly coupled by a pulsed laser, it is possible to measure the decay rate from the upper state by applying sufficient laser power to depletion broaden the transition. The depletion broadening is proportional to the square root of the decay rate times the total energy density of the laser pulse. With sufficient laser power, this technique can be used even if the decay rate is smaller than inhomogeneous broadenings or the laser linewidth. The technique is used here to measure autoionizing rates of some 6P((1/2))ns states.
New experimental quantum simulation platforms have recently been implemented with divalent atoms trapped in optical tweezer arrays, with promising performance.The second valence electron also brings about new prospects through the so-called isolated core excitation (ICE).However, autoionization presents a strong limitation to this use.In this study, we propose and demonstrate a new approach to applying a sizable light shift to a Rydberg state with close-to-resonant ICE while avoiding autoionization.In particular, we investigate the ICE of ytterbium atoms in 1 S 0 Rydberg states.Spectroscopic studies of the induced autoionization and the light shift imparted to the Rydberg states are well accounted for with multichannel quantum defect theory.Such control over the inner electron without disturbing the Rydberg electron brings about a new tool for the targeted coherent manipulation of Rydberg states in quantum simulation or quantum computing experiments performed with alkaline-earth atoms.