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Physical Review A

Experimental studies of high-lying Rydberg states in atomic rubidium

Sylvain Liberman, Jacques Pinard

Published Aug 1, 1979• 69 citations
Publisher

Abstract

This paper summarizes a long series of experiments that have been done on Rydberg states of Rb. The basic experimental technique that has been used is atomic-beam laser spectroscopy which allows both low-resolution and high-resolution studies. Excitation of Rydberg states is provided by single-photon absorption from a suitably frequency-doubled rhodamine $6G$ tunable laser. Detection is done by field ionization and ion counting. These techniques have allowed us to study the critical ionizing field, which has been found to follow classical, hydrogenic behavior closely. Rydberg states of Rb have been observed from $n=28$ up to $n>100$. High-resolution spectroscopic studies have led to measurement of the fine structure for $\mathrm{np}$ levels located between $n=28$ and $n=60$, as well as the isotope shift of the ground state, $\ensuremath{\delta}\ensuremath{\nu}=(172\ifmmode\pm\else\textpm\fi{}15)$ MHz. Anomalies in the intensity ratio of the doublet $5s\ensuremath{-}np$ transitions have been observed and interpreted as relativistic effects. Perturbations by weak and strong dc electric field are reported. In the case of weak electric fields it is possible to evaluate the polarizability. In the case of strong dc electric fields, new phenomena have been observed and analyzed. We also find experimental evidence of selective photoionization in the presence of an appropriate dc electric field, which could have some applications in laser isotope separation. Finally, we give the preliminary results of an experiment on the effect of a strong nonresonant electromagnetic field on high-lying Rydberg states.

DOI
10.1103/physreva.20.507

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Experimental and theoretical study of Stark patterns in Rb Rydberg levels

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Optical spectroscopy of nP Rydberg states of Rb87 atoms with a 297-nm ultraviolet laser

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We report the measurement of the absolute transition frequencies of $^{87}\mathrm{Rb}$ atoms to the $n{P}_{1/2}$ ($n=34--52$) and $n{P}_{3/2}$ ($n=34--90$) Rydberg states by performing single-photon Rydberg excitation spectroscopy in a vapor cell. Rydberg transitions were detected by monitoring the transmission of a 780-nm probe beam. Based on the spectroscopic data, we determined the fine-splitting intervals and oscillator-strength ratios of the $nP$ doublets and also extracted the quantum defects and ionization frequency. These results extend the spectroscopic information of the $nP$ Rydberg series, providing basic knowledge for further applications to Rydberg atoms.

Physical Review A•Apr 5, 2019•17 citations
This paper summarizes a long series of experiments that have been done on Rydberg states of Rb. The basic experimental technique that has been used is atomic-beam laser spectroscopy which allows both low-resolution and high-resolution studies. Excitation of Rydberg states is provided by single-photon absorption from a suitably frequency-doubled rhodamine 6G6G6G tunable laser. Detection is done by field ionization and ion counting. These techniques have allowed us to study the critical ionizing field, which has been found to follow classical, hydrogenic behavior closely. Rydberg states of Rb have been observed from n=28n=28n=28 up to n>100n>100n>100. High-resolution spectroscopic studies have led to measurement of the fine structure for np\mathrm{np}np levels located between n=28n=28n=28 and n=60n=60n=60, as well as the isotope shift of the ground state, \ensuremathδ\ensuremathν=(172\ifmmode±\else\textpm\fi15)\ensuremath{\delta}\ensuremath{\nu}=(172\ifmmode\pm\else\textpm\fi{}15)\ensuremathδ\ensuremathν=(172\ifmmode±\else\textpm\fi15) MHz. Anomalies in the intensity ratio of the doublet 5s\ensuremath−np5s\ensuremath{-}np5s\ensuremath−np transitions have been observed and interpreted as relativistic effects. Perturbations by weak and strong dc electric field are reported. In the case of weak electric fields it is possible to evaluate the polarizability. In the case of strong dc electric fields, new phenomena have been observed and analyzed. We also find experimental evidence of selective photoionization in the presence of an appropriate dc electric field, which could have some applications in laser isotope separation. Finally, we give the preliminary results of an experiment on the effect of a strong nonresonant electromagnetic field on high-lying Rydberg states.
Stark patterns of high-lying excited states of rubidium (Rydberg states $n\ensuremath{\sim}48$) in electric fields from 0 to 20 V/cm have been studied both experimentally and theoretically. Recordings have been obtained with high-resolution laser techniques. Theoretical interpretation takes into account a great number of close-lying levels in the diagonalization process. In order to reproduce the positions as well as the intensities of the one-photon transitions from the ground state, it is necessary to use for sss, ppp, and ddd levels the wave functions calculated from a central potential specific to the Rb spectrum.
In this dissertation, I explore several aspects of Rydberg physics with laser spectroscopy. The experiments center around the use of a very deep, cavity-generated, one-dimensional optical lattice in a cold atom sample. The optical lattice produces elongated clouds of dense, cold atoms via dipole trapping and is able to generate extreme light shifts in the atoms due to its high intensity. I describe experiments which may be divided into two main classes. In the first, I use the dipole trap to prepare a dense sample of atoms for photoassociation of Rb atom pairs into diatomic Rydberg molecules. The Rydberg molecules are formed by low-energy scattering of the Rydberg electron of one atom from the other atom, which is a ground-state atom. This novel binding mechanism also has relevance for chemical physics. I present binding energy measurements for eight different cases of Rydberg molecules. The binding energies reveal information about electron-atom collisions, such as their scattering lengths, and about the spin couplings present within the molecular system. In the second class of experiments, I introduce two proposed measurements in which the optical lattice is ramped to very high intensity during the laser excitation, creating AC Stark shifts in the transition frequencies. In one measurement, low-lying atomic states are probed. Measurements of the light shifts are expected to yield data on the dynamic polarizability and the photoionization cross section of the 5D3/2D_{3/2}D3/2​-state in rubidium in a 1064-nm light field. I show corresponding preliminary experimental data. The polarizability and photo-ionization cross-section measurements will provide tests of atomic structure theory, which is important both at a fundamental level and for applications such as atomic clocks. In another proposed measurement, Rydberg atoms in the lattice experience ponderomotive shifts and strong mixing of their angular-momentum states, allowing direct optical excitation of the lattice-mixed high-angular-momentum states. I describe the theoretical basis and experimental preparation for spectroscopically characterizing the lattice-mixed states. The ability to optically excite selected high-angular-momentum states without the use of static or RF fields may be useful for quantum information processing and simulation.
A frequency stabilized ring dye laser, with a linewidth of (TURN)250 kHz, has been utilized to selectively excite Rb(N('2)S, N('2)D) states in the range N = 20 - 100 by a two photon process. The highly excited atoms were detected by the technique of electric field ionization. Excited states with (VBAR)M(,L)(VBAR) < 3 have been observed to ionize along predominantly adiabatic paths and states with (VBAR)M(,L)(VBAR) (GREATERTHEQ) 3 have been observed to ionize along predominantly diabatic paths for the range of N investigated. The electric field dependence of the ionization threshold has been determined to be in good agreement with that calculated from a simple model based on the energies and ionization rates of hydrogen.\nCollisions between highly excited rubidium atoms and neutral xenon atoms, which result in a change in the N and L of the excited state of the rubidium atom, have been investigated. The N of the final state has been shown to be limited to those states which lie closest in energy to the initial state, in good agreement with theory. The distribution of L of the final states has been shown to be completely statistical or biased towards production of high L. The distribution of final L is definitely not biased toward production of states with low values of L.
Doppler-free two-photon absorption spectroscopy was applied to study highly-excited D states of Rb atoms. Using a cw dye laser as an excitation source, transitions from the ground 5S state to nd 2D states (n=11-32) were observed, the ionization energy of the highest state being only 117cm-1. These D doublets are not inverted. The fine structure splittings of these states do not vary as (neff) -3, nor as n-3. The isotope shift of the 85Rb, 87Rb ground states is found to be 160±12MHz. No pressure broadening was observed for these transitions within the instrumental resolution of 15 MHz.
In highly excited Rydberg atoms, the excited electron is in a large, loosely bound orbit. Hence, in contrast with the ground states, the Rydberg states are very sensitive to external electric field and can be ionized in rather weak fields. The low ionization threshold of Rydberg states results in effective state-specific detection by the selective field ionization technique. \t In this thesis, high-resolution spectroscopy of Rydberg states of Rubidium using millimeter wave transitions and selective field ionization has been used as a probe of external electric and magnetic fields. Laser cooling and trapping techniques in a magneto-optical trap (MOT) are employed to have a high density and narrow velocity distribution for the atomic sample. In this work the magnetic field inhomogeneity inherent in a MOT is minimized and the stray electric field present at the trap region is compensated in order to have resolved spectra. The Stark line broadening of the spectra obtained in this work may be used to determine the electric field distribution in an expanding ultra-cold neutral plasma.
We report the measurement of the absolute transition frequencies of 87Rb^{87}\mathrm{Rb}87Rb atoms to the nP1/2n{P}_{1/2}nP1/2​ (n=34−−52n=34--52n=34−−52) and nP3/2n{P}_{3/2}nP3/2​ (n=34−−90n=34--90n=34−−90) Rydberg states by performing single-photon Rydberg excitation spectroscopy in a vapor cell. Rydberg transitions were detected by monitoring the transmission of a 780-nm probe beam. Based on the spectroscopic data, we determined the fine-splitting intervals and oscillator-strength ratios of the nPnPnP doublets and also extracted the quantum defects and ionization frequency. These results extend the spectroscopic information of the nPnPnP Rydberg series, providing basic knowledge for further applications to Rydberg atoms.