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arXiv:1910.11600 · Science

Quantum-nondemolition state detection and spectroscopy of single trapped molecules

Mudit Sinhal, Ziv Meir, Kaveh Najafian, Gregor Hegi, Stefan Willitsch

Published Mar 12, 2020• 74 citations
arXivHTMLPDF

Abstract

Trapped atoms and ions, which are among the best-controlled quantum systems, find widespread applications in quantum science. For molecules, a similar degree of control is currently lacking owing to their complex energy-level structure. Quantum-logic protocols in which atomic ions serve as probes for molecular ions are a promising route for achieving this level of control, especially for homonuclear species that decouple from blackbody radiation. Here, a quantum-nondemolition protocol on single trapped [Formula: see text] molecules is demonstrated. The spin-rovibronic state of the molecule is detected with >99% fidelity, and a spectroscopic transition is measured without destroying the quantum state. This method lays the foundations for new approaches to molecular spectroscopy, state-to-state chemistry, and the implementation of molecular qubits.

DOI
10.1126/science.aaz9837

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Spectroscopy Achieving efficient quantum control of ultracold molecular systems may open opportunities in molecular precision spectroscopy, quantum information, and related fields. Sinhal et al. report a quantumnondemolition protocol for the detection of the spin-rovibronic state of a single trapped cold molecular ion co-trapped with an atomic ion. They show that monitoring the motion of Ca+ after coherent motional excitation of the Ca+-N2+ string makes it possible to detect the N2+ state without destroying either the molecule or the state itself. The procedure can be repeated multiple times while preserving the high readout fidelity. Science , this issue p. [1213][1] [1]: /lookup/doi/10.1126/science.aaz9837
We present theoretical and experimental progress towards a new approach for the precision spectroscopy, coherent manipulation and state-to-state chemistry of single isolated molecular ions in the gas phase. Our method uses a molecular beam for creating packets of rotationally cold neutrals from which a single molecule is state-selectively ionized and trapped inside a radiofrequency ion trap. In addition to the molecular ion, a single co-trapped atomic ion is used to cool the molecular external degrees of freedom to the ground state of the trap and to detect the molecular state using state-selective coherent motional excitation from a modulated optical-dipole force acting on the molecule. We present a detailed discussion and theoretical characterization of the present approach. We simulate the molecular signal experimentally using a single atomic ion, indicating that different rovibronic molecular states can be resolved and individually detected with our method. The present approach for the coherent control and non-destructive detection of the quantum state of a single molecular ion opens up new perspectives for precision spectroscopies relevant for, e.g., tests of fundamental physical theories and the development of new types of clocks based on molecular vibrational transitions. It will also enable the observation and control of chemical reactions of single particles on the quantum level. While focusing on N2+ as a prototypical example in the present work, our method is applicable to a wide range of diatomic and polyatomic molecules.
Electric-dipole forbidden spectroscopic transitions in atoms form the basis of many advanced implementations of quantum computers, atomic clocks and quantum sensors. Coherently addressing such transitions in molecules which are among the most ubiquitous and versatile quantum objects has remained a long-standing challenge owing to their complex energy-level structure. Here, we report the search, observation and coherent manipulation of electric-quadrupole rotational-vibrational transitions in single trapped molecules using a quantum-logic-spectroscopy protocol. We identified individual hyperfine-Zeeman-rotational components of the fundamental vibrational transition of the nitrogen molecular ion, N2+_2^+2+​, and performed coherent population transfer between energy levels. Our work opens up new perspectives for precision molecular spectroscopy, for high-fidelity qubits encoded in the rotational-vibrational motion of molecules, for precise infrared molecular clocks and for searches for new physics
We review our recent experimental results on the non-destructive quantum-state detection and spectroscopy of single trapped molecules. At the heart of our scheme, a single atomic ion is used to probe the state of a single molecular ion without destroying the molecule or even perturbing its quantum state. This method opens up perspectives for new research directions in precision spectroscopy, for the development of new frequency standards, for tests of fundamental physical concepts and for the precise study of chemical reactions and molecular collisions with full control over the molecular quantum state.
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.
Quantum-logic techniques for state preparation, manipulation, and non-destructive interrogation are increasingly being adopted for experiments on single molecular ions confined in traps. The ability to control molecular ions on the quantum level via a co-trapped atomic ion offers intriguing possibilities for new experiments in the realms of precision spectroscopy, quantum information processing, cold chemistry, and quantum technologies with molecules. The present article gives an overview of the basic experimental methods, recent developments and prospects in this field.