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Ultrafast Infrared Spectroscopy with Single Molecular Ions

Schindler, Philipp

We propose a method to investigate the vibrational dynamics of single polyatomic molecular ions confined in a Paul trap [1]. Quantum logic techniques are employed to detect the recoil of single photon absorption events in the molecule via a co-trapped atomic ion. In particular, the recoil is mapped onto the electronic state of the atom which can be read out with high fidelity. This recoil detection serves as the basis for a pump-probe scheme to investigate ultrafast molecular dynamics, such as intra-molecular vibrational redistribution. The total recoil from the interaction with a sequence of ultrafast laser pulses with the molecular vibration is measured. This work discusses the experimental requirements and expected performance for multiple molecular ions. Furthermore, we will discuss the possibility to perform quantum non-demolition measurements of the molecule’s vibrational state, and a procedure to perform coherent state transfer between the molecule and the atomic ion.

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