Population pumping of vibrational and rotational quantum states in the triatomic hydrogen ion observed by electron-beam-assisted high-resolution spectroscopy
We present a technique to observe the optical manipulation of individual quantum states of H3+ ions stored inside a heavy-ion storage ring, where the excitation is detected by electron-beam-assisted action spectroscopy. The transitions addressed here are chosen to enable multicolor spectroscopy of states far above the energetic barrier, where this molecule-with a triangular ground state-can sample linear geometries. This region of the spectrum has so far been inaccessible due to extremely weak direct transition strengths from the ground vibrational level. Our experiments pave the way for spectroscopy of the simplest polyatomic molecule in a previously unexplored energetic territory, which would benchmark theoretical data crucial for the understanding of this fundamental molecular system. Our results also demonstrate laser pumping to vibrationally and rotationally excited states of H3+ , gaining model-dependent access to their relative dissociative electron recombination rates.
Maxton, M., Berger, L., Bechtel, J., Enzmann, L., Grieser, M., Grussie, F., Himmelsbach, J., Isberner, L., Schmidt, V., Sharma, D., Wolf, A., Znotins, A., Urbain, X., Novotný, O., & Kreckel, H. (2026). Population pumping of vibrational and rotational quantum states in the triatomic hydrogen ion observed by electron-beam-assisted high-resolution spectroscopy. Physical Review Research, 8(4), 0-10. https://doi.org/10.1103/w9q1-yk99 (Original work published 2026)