Methods of excitation and analysis of double-Rydberg states of the neutral barium atom are discussed. Spectra of 9dn′d double-Rydberg series of barium are studied and interpreted in a two-channel quantum-defect model. An example of stabilization for the 9d5/227d state is shown. We propose a new investigative method for Rydberg levels of the Ba+ ion that is based on a microwave-ionization process coupled with a double time-of-flight mass spectrometer. This novel setup permits us to obtain initial experimental evidence of highly excited double-Rydberg states, 26dn′p and 27sn′p (n′ ≳ 45), of the barium atom.
The fine structure of high-angular-momentum
n=9 and 10 Rydberg states of barium has been measured precisely, using the resonant excitation Stark ionization spectroscopy method. Optical transitions corresponding to $(n,{n}^{\ensuremath{'}})=(10,30)$, (9,17), and (9,20) were induced with a Doppler-tuned
CO2 laser, determining the fine-structure energies corresponding to all
n=9 and 10 levels with $L\ensuremath{\geqslant}6$. The pattern of these fine-structure energies conforms closely with an effective potential model, by comparison with which the dipole and quadrupole polarizabilities of
Ba+ can be determined. Combining our data with earlier measurements made it possible to deduce, in addition, the portion of ${\ensuremath{\alpha}}_{2}$ due to the lowest excited
D state of
Ba+. Our best estimates of these three properties are ${\ensuremath{\alpha}}_{1}=124.30(16){a}_{0}^{3}$, ${\ensuremath{\alpha}}_{2}=2462(361){a}_{0}^{5}$, and ${\ensuremath{\alpha}}_{2}^{0}=1828(88){a}_{0}^{5}$.