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International Symposium on Molecular Spectroscopy (ISMS)

DOUBLE RESONANCE SPECTROSCOPY OF BaF AUTOIONIZING RYDBERG STATES

Timothy Barnum, Robert W. Field, Yan Zhou, David Grimes

Published Jun 23, 2015• 1 citation

Abstract

We have studied the $nu$=1 Rydberg states of BaF in the energy region E=38800-39100 wn (n*=15-25) via optical-optical double resonance spectroscopy. Rydberg states excited above the first ionization potential spontaneously autoionize and $^{138}$Ba$^{19}$F$^{+}$ ions are detected by TOF-MS. In addition, BaF possesses a particularly low ionization potential, which allows for the study of autoionization dynamics in the absence of predissociative decay. This work extends the assignments of core-penetrating Rydberg states of BaF (Jakubek and Field, 2000) for applications to state-selective ion production schemes. Polarization and Stark spectroscopy techniques will be discussed in the context of accurate and efficient assignment of spectra.

DOI: 10.15278/isms.2015.tj06

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We have studied the

nu

=1 Rydberg states of BaF in the energy region E=38800-39100 wn (n*=15-25) via optical-optical double resonance spectroscopy. Rydberg states excited above the first ionization potential spontaneously autoionize and

^{138}

Ba

^{19}

F

^{+}

ions are detected by TOF-MS. In addition, BaF possesses a particularly low ionization potential, which allows for the study of autoionization dynamics in the absence of predissociative decay. This work extends the assignments of core-penetrating Rydberg states of BaF (Jakubek and Field, 2000) for applications to state-selective ion production schemes. Polarization and Stark spectroscopy techniques will be discussed in the context of accurate and efficient assignment of spectra.

The ionization of

6sns^{1}S_{0}

Rydberg states of

^{138}\mathrm{Ba}

has been investigated by high-resolution electron spectroscopy. The Rydberg states were excited by two cw dye lasers via the

6s6p^{1}P_{1}

level. The electron spectra show rich structure between 0.025 and 3 eV, largely attributable to collisional (Penning) ionization, photoionization, and autoionizing transitions. The first process might be interpreted as superelastic scattering of the Rydberg electron by optically pumped

\mathrm{Ba}(6s6p^{1}P_{1})

or

\mathrm{Ba}(6s5d^{1}D_{2})

atoms.

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

{\mathrm{CO}}_{2}

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

{\mathrm{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

{\mathrm{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 ${\ensuremath{\alpha}}_{2}^{0}=1828(88){a}_{0}^{5}$.