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We present theoretical and experimental progress towards a new approach forthe precision spectroscopy, coherent manipulation and state-to-state chemistryof single isolated molecular ions in the gas phase. Our method consists of amolecular beam for creating packets of rotationally cold neutrals from which asingle molecule is state-selectively ionized and trapped inside aradiofrequency ion trap. In addition to the molecular ion, a single co-trappedatomic ion is used to cool the molecular external degrees of freedom to theground state of the trap and to detect the molecular state usingstate-selective coherent motional excitation from a modulated optical-dipoleforce acting on the molecule. We present a detailed discussion and theoreticalcharacterization of the present approach. We simulate the molecular signalexperimentally using a single atomic ion indicating that different rovibronicmolecular states can be resolved and individually detected with our method. Thepresent approach for the coherent control and non-destructive detection of thequantum state of a single molecular ion opens up new perspectives for precisionspectroscopies relevant for, e.g., tests of fundamental physical theories andthe development of new types of clocks based on molecular vibrationaltransitions. It will also enable the observation and control of chemicalreactions of single particles on the quantum level. While focusing on N$_2^+$as a prototypical example in the present work, our method is applicable to awide range of diatomic and polyatomic molecules.

faraday discussions

State-selective coherent motional excitation as a new approach for the  manipulation, spectroscopy and state-to-state chemistry of single molecular  ions