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Nature Physics

Rotational laser cooling of vibrationally and translationally cold molecular ions

Peter Frøhlich Staanum, Klaus Højbjerre, Peter Sandegaard Skyt, Anders Kragh Hansen, Michael Drewsen

Published Mar 7, 2010• 203 citations
Publisher
DOI
10.1038/nphys1604

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Physical Review Letters•Sep 27, 2010•137 citations
Working with MgH+molecular ions in a linear Paul trap, we routinely cool their translational degrees of freedom by sympathetic cooling with Doppler laser cooled Mg+ions. Giving the time for the molecules to equilibrate internally to room temperature blackbody radiation, the vibrational degree of freedom is frozen out, leaving only the rotational degree of freedom to be cooled. We have implemented a new technique for laser-induced rotational ground-state cooling of vibrationally and translationally cold MgH+ions, using a scheme based on excitation of a single rovibrational transition. This technique is generalizable to any diatomic polar molecular ion, given an appropriate mid-infrared laser source such as a quantum cascade laser.
The first steps toward the implementation of a simple scheme for rotational cooling of MgH + ions based on rotational state optical pumping is considered. The various aspects of such an experiment are described in detail, and the rotational state-selective dissociation spectra of translationally and vibrationally cold MgH + ions are presented, with and without the optical pumping laser being present. While rotational cooling is as yet not evident, first results showed evidence of a change in the rotational distribution in the presence of the optical pumping laser.
We present a new method for the generation of rotationally and vibrationally state-selected, translationally cold molecular ions in ion traps. Our technique is based on the state-selective threshold photoionization of neutral molecules followed by sympathetic cooling of the resulting ions with laser-cooled calcium ions. Using N₂(+) ions as a test system, we achieve >90% selectivity in the preparation of the ground rovibrational level and state lifetimes on the order of 15 minutes limited by collisions with background-gas molecules. The technique can be employed to produce a wide range of apolar and polar molecular ions in the ground and excited rovibrational states. Our approach opens up new perspectives for cold quantum-controlled ion-molecule-collision studies, frequency-metrology experiments with state-selected molecular ions and molecular-ion qubits.