25-29 September 2023
Schloss Bückeburg
Europe/Berlin timezone

Reactive tunneling and vibrational quenching collisions in a cryogenic multipole trap

28 Sep 2023, 15:25
20m
Schloss Bückeburg

Schloss Bückeburg

Schlossplatz 1 31675 Bückeburg
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Speaker

Robert Wild (University of Innsbruck)

Description

Quantum tunneling reactions play an important role in chemistry when classical pathways are energetically forbidden [1]. Binary collisions of atomic with molecular hydrogen belong to the most fundamental molecular systems and are simple enough to be theoretically investigated using first-principle calculations. The rate of the tunneling reaction H$_2$ + D$^- \rightarrow$ H$^-$ + HD has been calculated [2] but has until now lacked verification. Here we present high-sensitivity measurements of the reaction rate carried out in a cryogenic 22-pole ion trap. A deviation of the reaction rate from linear scaling, which is observed at high H$_2$ densities, can be traced back to previously unobserved heating dynamics in radiofrequency ion traps. Our measured value agrees with quantum tunneling calculations, serving as a benchmark for molecular theory and advancing the understanding of fundamental collision processes [3].

Further work has focused on inelastic collisions of C$_2^-$, which has been proposed as a candidate for laser cooling due to the existence of multiple stable electronic states. We have demonstrated vibrational state control of C$_2^-$ via a novel scheme that uses optical pumping in conjunction with inelastic collisions of H$_2$ and measured the vibrational quenching rate [4]. Additionally, we precisely determined the proposed laser-cooling transitions of C$_2^-$. We resolve the spin-rotation splittings and use it to perform accurate thermometry in our newly-developed wire trap [5].

[1] McMahon, R. J. Chemical reactions involving quantum tunneling. Science 299, 833–834 (2003).
[2] Yuen, C. H., Ayouz, M., Endres, E. S., Lakhmanskaya, O., Wester, R., Kokoouline, V. Quantum-tunneling isotope-exchange reaction H$_2$ + D$^−\rightarrow$ HD + H$^−$. Phys. Rev. A 97, 022705 (2018).
[3] Wild, R., Nötzold, M., Simpson, M., Tran, T. D., Wester, R. Tunnelling measured in a very slow ion–molecule reaction. Nature (2023).
[4] Nötzold, M., Wild, R., Lochmann, C., Rahim, T., Melath, S. P., Mant, B., Franz, J., Gianturco, F., Wester, R. (in preparation)
[5] Nötzold, M., Wild, R., Lochmann, C., Wester, R. Spectroscopy and ion thermometry of C$_2^−$ using laser-cooling transitions, Phys. Rev. A 106, 023111 (2022).

Primary author

Robert Wild (University of Innsbruck)

Co-authors

Markus Nötzold (University of Innsbruck) Malcolm Simpson (University of Innsbruck) Christine Lochmann (University of Innsbruck) Tanja Rahim (University of Innsbruck) Sruthi Purushu Melath (University of Innsbruck) Thuy Dung Tran (Palacky University) Barry Mant (University College London) Jan Franz (Gdansk University of Technology) Francesco Gianturco (University of Innsbruck) Roland Wester (University of Innsbruck)

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