Abstract
We have applied optical-optical-optical triple resonance spectroscopy to resolve a system of high Rydberg states in BH that serves quantitatively to characterize a fundamental example of electron-orbital–cation core rotational coupling. The third-color ionization-detected absorption spectrum originating from the photoselected Rydberg state with vibrational and total angular momentum quantum numbers, and consists entirely of vibrationally autoionizing resonances for which final that converge in series to the rotational limits, , 1, and 2. For series with converging to and 2, Rydberg orbital and rotational angular momenta couple to systematically perturb level energies and distribute lifetime in a well-isolated two-channel rotronic interaction that spans hundreds of wave numbers.
- Received 28 October 2003
DOI:https://doi.org/10.1103/PhysRevLett.92.173005
©2004 American Physical Society