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arXiv:physics/0507181 · Journal of Physics B Atomic Molecular and Optical Physics

Probabilistic state preparation of a single molecular ion by projection measurement

I S Vogelius, L B Madsen, M Drewsen

Published Sep 25, 2006• 27 citations
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Abstract

We show how to prepare a single molecular ion in a specific internal quantum state in a situation where the molecule is trapped and sympathetically cooled by an atomic ion and where its internal degrees of freedom are initially in thermal equilibrium with the surroundings. The scheme is based on conditional creation of correlation between the internal state of the molecule and the translational state of the collective motion of the two ions, followed by a projection measurement of this collective mode by atomic ion shelving techniques. State preparation in a large number of internal states is possible.

DOI
10.1088/0953-4075/39/19/s31

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•Jun 1, 2011•0 citations
We show how to prepare a single molecular ion in a specific internal quantum state in a situation where the molecule is trapped and sympathetically cooled by an atomic ion and where its internal degrees of freedom are initially in thermal equilibrium with the surroundings. The scheme is based on conditional creation of correlation between the internal state of the molecule and the translational state of the collective motion of the two ions, followed by a projection measurement of this collective mode by atomic ion shelving techniques. State preparation in a large number of internal states is possible.
Polyatomic molecular ions contain many desirable attributes of a useful quantum system, including rich internal degrees of freedom and highly controllable coupling to the environment. To date, the vast majority of state-specific experimental work on molecular ions has concentrated on diatomic species. The ability to prepare and read out polyatomic molecules in single quantum states would enable diverse experimental avenues not available with diatomics, including new applications in precision measurement, sensitive chemical and chiral analysis at the single-molecule level, and precise studies of Hz-level molecular tunneling dynamics. While cooling the motional state of a polyatomic ion via sympathetic cooling with a laser-cooled atomic ion is straightforward, coupling this motional state to the internal state of the molecule has proven challenging. Here we propose a method for readout and projective measurement of the internal state of a trapped polyatomic ion. The method exploits the rich manifold of technically accessible rotational states in the molecule to realize robust state preparation and readout with far less stringent engineering than quantum logic methods recently demonstrated on diatomic molecules. The method can be applied to any reasonably small $(\ensuremath{\lesssim}10$ atoms) polyatomic ion with an anisotropic polarizability.
We give a detailed characterization of a recently developed method to prepare translationally cold, internally state-selected molecular ions in ion traps [X. Tong, A. H. Winney, and S. Willitsch, Phys. Rev. Lett. 105, 143001 (2010)]. The technique relies on the generation of molecular ions in a well-defined rotational-vibrational quantum state using threshold photoionization followed by sympathetic cooling of the translational motion with laser-cooled Ca+{}^{+}+ ions. We discuss the experimental requirements for the successful generation and sympathetic cooling of state-selected ions, explore the influence of collisional and radiative processes on the population redistribution dynamics, and give an assessment of the scopeof the method.
We propose a scheme for the preparation, manipulation and detection of quantum states of single molecular ions. In this scheme, molecular and atomic ions are confined in radio-frequency Paul trap and share common modes of motion. A frequency comb laser field is used to drive stimulated Raman transitions that couple internal states of the molecular ion with the motion of ions. State transfer from the molecular ion to the atomic ion via the common mode of motion results in efficient state detection for the molecule. The coupling of molecular states to the motion and the subsequent sideband cooling of the ions provide a way to prepare the molecular ion in a well-defined state.
Sympathetic cooling of molecular ions through the Coulomb interaction with laser-cooled atomic ions is an efficient tool to prepare translationally cold molecules without, ideally, affecting the internal state of the molecular ions. However, the electric field due to the Coulomb interaction may induce rotational transitions that change the purity of initially quantum state prepared molecules. Here, we use estimates of rotational state changes in single collisions of diatomic ions with atomic ions [J. M. Berglund, M. Drewsen, and C. P. Koch, ] to determine the overall rotational excitation accumulated over the sympathetic cooling. Considering two different experimental scenarios, that of a molecular ion cotrapped with a single atomic ion and a molecular ion immersed in a Coulomb crystal of atomic ions, we also estimate the cooling time.
Sympathetic cooling of molecular ions through the Coulomb interaction with laser-cooled atomic ions is an efficient tool to prepare translationally cold molecules without, ideally, affecting the internal state of the molecular ions. However, the electric field due to the Coulomb interaction may induce rotational transitions that change the purity of initially quantum state prepared molecules. Here, we use estimates of rotational state changes in single collisions of diatomic ions with atomic ions [J. M. Berglund, M. Drewsen, and C. P. Koch, Phys. Rev. A 113, 042816 (2026)] to determine the overall rotational excitation accumulated over the sympathetic cooling. Considering two different experimental scenarios, that of a molecular ion cotrapped with a single atomic ion and a molecular ion immersed in a Coulomb crystal of atomic ions, we also estimate the cooling time.
Stationary molecules in well-defined internal states are of broad interest in both physics and chemistry. Through high-resolution spectroscopy, fundamental physics can be tested and lead to, e.g., improved values of the electron-to-proton mass ratio [1], new boundaries on the electron electric dipole moment [2] and observation of the potential evolution of the fine structure constant over time [3]. Translationally and internally cold molecules have as well been considered promising candidates for qubits in new quantum computing senarios [4], and molecular ions could in the future likely become an excellent alternative to atomic qubits in the realization of a practical ion trap based quantum computer due to favourable internal state decoherence rates. In chemistry, state prepared molecular targets are an ideal starting point for uni-molecular reactions, including coherent control of photofragmentation through the application of various laser sources [5,6]. In cold bi-molecular reactions, where the effect of even tiny potential barriers becomes significant, experiments with state prepared molecules can yield important information on the details of the potential curves of the molecular complexes [7,8,9]. Furthermore, in order to learn more about the chemistry in interstellar clouds, astrochemists can benefit greatly from direct measurements on cold reactions in laboratories [9]. Working with MgH+ molecular ions in a linear Paul trap, we routinely cool their translational degree of freedom by sympathetic cooling with Doppler laser cooled Mg+ ions. Giving the time for the molecules to equilibrate internally to the room temperature blackbody radiation, the vibrational degree of freedom will freeze out, leaving only the rotational degree of freedom to be cooled. We report here on the implementation of a new technique for laser-induced rotational ground-state cooling of vibrationally and translationally cold MgH+ ions [10]. The scheme is based on excitation of a single rovibrational transition [11], and it should be generalizable to any diatomic polar molecular ion, given appropriate mid-infrared laser sources such as a quantum cascade laser are available. In recent experiments, a nearly 15-fold increase in the rotational ground-state population was obtained, with the resulting ground-state population of 36,7±1,2 %, equivalent to that of a thermal distribution at about 20 K. The obtained cooling results imply that, through this technique, cold molecular-ion experiments can now be carried out at cryogenic temperatures in room-temperature set-ups. References [1] Koelemeij, J. C. J., Roth, B., Wicht, A., Ernsting, I. and Schiller, S., Phys. Rev. Lett. 98, 173002 (2007). [2] Hudson, J. J., Sauer, B. E., Tarbutt, M. R. and Hinds, E. A., Phys. Rev. Lett. 89, 023003 (2002). [3] Hudson, E. R., Lewandowski, H. J., Sawyer, B. C. and Ye, J, Phys. Rev. Lett. 96, 143004 (2006). [4] DeMille, D, Phys. Rev. Lett. 88, 067901 (2002). [5] Rice, S. A. and Zaho, M. Optical control of molecular dynamics (Wiley, New York, 2000). [6] Shapiro, M. and Brumer, P. W. Principles of the Quantum Control of Molecular Processes (Wiley, New York, 2003). [7] Willitsch, S., Bell, M. T., Gingell, A. D. and Softley, T. P., Phys. Chem. Chem. Phys. 10, 7200 ( 2008). [8] Krems, R. V., Phys. Chem. Chem. Phys. 10, 4079 (2008). [9] Smith, I. W. M., Low temperatures and cold molecules (Imperial College Press, London, 2008). [10] Staanum, P. F., Højbjerre, K., Skyt, P.S., Hansen, A. K. and Drewsen, M., Nat. Phys. 6, 271 (2010). [11] Vogelius, I. S., Madsen, L. B. and Drewsen, M., Phys. Rev. Lett. 89, 173003 (2002).