Abstract
Six core-penetrating Rydberg series have been assigned in the CaCl molecule by a combination of double-resonance spectroscopic techniques. Two2Σ+series, with approximate quantum defects (δ) of 0.51 and 0.25, have been observed with effective principal quantum numbers (n*) in the range of 5–8 using theD2Σ+state as the resonant intermediate state for REMPI and/or ion-dip detection. A third2Σ+series with δ ≈ 0.84 and a2Δ series with δ ≈ 0.95 have been observed withn* = 16–18 using theA2Π3/2state as the resonant intermediate state for preparation ofv+= 1 vibrationally autoionizing states. Two additional series in the same region with δ ≈ 0.90 and 0.07 are tentatively identified as the expected core-penetrating2Π series. Vibrational assignments have been confirmed in many cases on the basis of isotope shifts between the35Cl and37Cl isotopomers. The ion-dip and REMPI spectra display linewidths systematically broadened by predissociation. In addition to the assigned core-penetrating series, both the REMPI and the ion-dip spectra display some sharper features that have not yet been assigned. These sharper features most likely arise from perturbations of optically “bright” core-penetrating states by nominally “dark” higher-lcore-nonpenetrating states.
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