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arXiv:1307.4461 · New Journal of Physics

Microwave quantum logic spectroscopy and control of molecular ions

Molu Shi, Peter F. Herskind, Michael Drewsen, Isaac L. Chuang

Published Nov 11, 2013• 20 citations
arXivHTMLPDF

Abstract

A general method for rotational microwave spectroscopy and control of polar molecular ions via direct microwave addressing is considered. Our method makes use of spatially varying ac Stark shifts, induced by far off-resonant, focused laser beams to achieve an effective coupling between the rotational state of a molecular ion and the electronic state of an atomic ion. In this setting, the atomic ion is used for read-out of the molecular ion state, in a manner analogous to quantum logic spectroscopy based on Raman transitions. In addition to high-precision spectroscopy, this setting allows for rotational ground state cooling, and can be considered as a candidate for the quantum information processing with polar molecular ions. All elements of our proposal can be realized with currently available technology.

DOI
10.1088/1367-2630/15/11/113019

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A general method for rotational microwave spectroscopy and control of polar molecular ions via direct microwave addressing is considered. Our method makes use of spatially varying ac Stark shifts, induced by far off-resonant, focused laser beams to achieve an effective coupling between the rotational state of a molecular ion and the electronic state of an atomic ion. In this setting, the atomic ion is used for read-out of the molecular ion state, in a manner analogous to quantum logic spectroscopy based on Raman transitions. In addition to high-precision spectroscopy, this setting allows for rotational ground state cooling, and can be considered as a candidate for the quantum information processing with polar molecular ions. All elements of our proposal can be realized with currently available technology.
Quantum logic enables state preparation, readout and spectroscopy of otherwise difficult-to-study ions. Using the coupled harmonic motion shared between co-trapped ions, information can be transferred from the "spectroscopy" ion to the easily manipulated "logic" ion. With this technique we perform high-resolution terahertz-scale rotational spectroscopy of a single CaH+ molecular ion in pure states by leveraging a Ca+ ion as our logic ion. Entangled states between a CaH+ and a Ca+ have also been demonstrated, making molecular ions possible components of hybrid systems for quantum information processing. Because all our laser operations on the molecule are driving stimulated Raman transitions with high detuning, the technique promises to be generalizable to a wide variety of molecular ion species. Additionally, we study the systematic effects of the trap RF electric field on molecular levels and use it to obtain a measurement of the dipole moment of the charged molecule.
Expanding the toolbox available for the control of individual atoms or ions to single molecules has many promising applications. Using quantum-logic spectroscopy, our group has demonstrated preparation, coherent manipulation, and nondestructive detection of rotational states of CaH+ molecular ions, as well as entangled states relevant for quantum information processing. We are currently building a new cryogenic experimental setup which features a molecular beam with interchangeable gas sources to overcome limitations in the existing experimental setup. With this setup, we plan to improve control over small molecules such as CaH+ and explore quantum state control of larger molecules.
Recently developed techniques for quantum computation using trapped ions allow precise coherent control of the internal and external states of single atoms. Here we report how these techniques can be employed to perform precision spectroscopy of atomic and molecular ions that lack accessible transitions for laser cooling and detection. Furthermore, we discuss how quantum logic can be used to laser‐cool molecules to near their rotational and vibrational ground state by avoiding detrimental spontaneous emission of photons from the molecule.
High-precision spectroscopy of atomic and molecular ions is an established platform for investigating fundamental aspects of physics. An important step in this direction was the development of quantum logic techniques that enable the spectroscopy of ions whose electronic structure does not allow direct laser cooling. Particularly challenging in this context is the investigation of atomic and molecular systems with many long-lived metastable states. The preparation of a pure quantum state for spectroscopy purposes often requires the prior detection of these long-lived states. For molecular ions, schemes for the detection of their rotational degree of freedom have already been developed in the past. However, quantum logic control of transition metals, in which the many metastable states result from several valence electrons, remained elusive. In this cumulative thesis, the first experimental implementation of a quantum logic assisted scheme for internal state detection of atomic systems as complex as a titanium ion is presented. Furthermore, a scheme based on simultaneous co-magnetometry for measuring the Landé g factor was developed and demonstrated for different fine structure states in 48Ti+. The presented method allows the suppression of systematic uncertainties arising from varying magnetic fields at the position of the ion and can be transferred to a variety of other species. Crucial for quantum logic based applications is the reliable preparation of a two-ion crystal consisting of one spectroscopy ion and one logic ion. A third aspect of this work is the deterministic preparation of such a two-ion crystal. The method based on fluorescence imaging is associated with a significantly reduced calibration effort compared to other schemes and can be easily transferred to other combinations of spectroscopy and logic ions. The quantum logic control capabilities demonstrated in this work are applicable to a wide range of other atoms with complex electronic structures as well as to molecular ions. The investigation of transition metals can provide important reference data for the calibration of absorption spectra from astrophysical objects. Molecular ions have applications in the search for a possible variation of fundamental constants or the measurement of energy shifts caused by an electron electric dipole moment, both representing promising approaches to test the standard model of particle physics.
Laser spectroscopy is a versatile tool to investigate the internal structure of atoms, molecules and nuclei.High precision spectroscopy requires laser cooling to reduce Doppler broadening and Doppler shifts.Sympathetic cooling extends these advantages to species which do not have an appropriate transition for laser cooling and allows precision spectroscopy of previously inaccessible species using the quantum logic technique.The original implementation of quantum logic spectroscopy relies on the long lifetime of the excited spectroscopy state to realize a transfer sequence.Precision spectroscopy of transitions with a short-lived excited state is typically performed using laser induced uorescence or laser absorption spectroscopy.Neither of these methods has reached the fundamental quantum projection noise limit and are rather limited by photon shot noise.For these situations, we develop the technique of photon recoil spectroscopy as an extension of quantum logic spectroscopy to broad transitions.The common motion of a sideband-cooled two-ion crystal is excited by photon recoil during photon absorption on the spectroscopically investigated ion.This motional excitation is transferred to an internal state excitation on the co-trapped ion of a dierent species and detected with high eciency.We demonstrate the technique on the 2 S 1/2 ↔ 2 P 1/2 transition of the 40 Ca + ion and resolve the line center to 1/300 of its observed linewidth.The simplicity and versatility of the technique promises applications to other previously inaccessible species.A variation of the technique is proposed for rotational state preparation of molecular ions.A moving optical lattice is employed to exert a state-dependent force on the molecule.This would allow the detection of the rotational state of the molecular ion and therefore enable precision spectroscopy of specic rovibrational transitions in the molecule.
We propose a fast and nondestructive spectroscopic method for single molecular ions that implements quantum logic schemes between an atomic ion and the molecular ion of interest. Our proposal relies on a hybrid coherent manipulation of the two-ion system, using optical or magnetic forces depending on the types of molecular levels to be addressed (e.g., Zeeman, rotational, vibrational or electronic degrees of freedom). The method is especially suited for the nondestructive precision spectroscopy of single molecular ions and sets a starting point for new hybrid quantum computation schemes that combine molecular and atomic ions, covering the measurement and entangling steps.