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Quantum state preparation and control of single molecular ions

Dietrich G. Leibfried

Published Aug 17, 2016• 33 citations
OpenAlex

Abstract

Abstract. Preparing molecules at rest and in a highly pure quantum state is a long standing dream in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information on the molecule. The outlined techniques might enable preparation, manipulation and measurement of a large multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics. 1.

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Quantum state preparation and control of single molecular ions

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Preparing molecules at rest and in a very pure quantum state is a long-standing aspiration in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower-energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information about the molecule. The outlined techniques might enable the preparation, manipulation and measurement of a multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics.

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

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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.

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Quantum Control of a Single H2+ Molecular Ion

David Holzapfel

In this thesis I describe how we achieve control over the quantum state of a single H2+ hydrogen molecular ion. Scientific progress is based on the comparison of theories with experimental measurements. For the simplest molecular quantum systems, such as the hydrogen molecular ions H2+ or HD+, the theoretical predictions of quantum electrodynamics are very accurate. In order to test the theory or to extract fundamental constants from the combination of theory and experiments, the experiments must also achieve high precision. In the recent past, hydrogen molecular ions were mainly measured in ensembles. For example, measurements exist both on molecular beams and with dissociative detection in ion traps. However, the spectroscopy of single ions is one of the most precise measurement methods in physics, which was demonstrated by the spectroscopy of a single ytterbium ion in an ion trap. To perform spectroscopy of a single ion in this way, it must have a suitable energy structure for laser cooling, state preparation and fluorescence detection. This is not the case for many ions, including H2+. Quantum logic spectroscopy (QLS) is a technique that makes it possible to perform measurements on an ion without such an energy structure. The ion to be measured (spectroscopy ion) is trapped in an ion trap with a second ion (helper ion), which has the properties described in the previous paragraph. The shared modes of motion between the two ions allow cooling, preparation and detection of the spectroscopy ion via the helper ion. This was demonstrated with an aluminum spectroscopy ion co-trapped with a magnesium helper ion. QLS can also be used for molecules. This has been shown with MgH+, CaH+ and N2+. We implement QLS to enable spectroscopy of a single H2+ ion. For this we trap H2+ together with a 9Be+ ion. We cool the joint motion of the ions to their ground state. We combine buffer gas cooling with a laser and microwave pulse based state preparation sequence to prepare the H2+ molecule in a pure quantum state. This allows us to perform high contrast QLS on a single H2+ ion. Furthermore, we can change and control the quantum state in the hyperfine structure using microwave pulses. We demonstrate the power of our technique by performing microwave spectroscopy on a magnetic field insensitive hyperfine transition. We use QLS to read out the result of the measurement. Within half an hour, we can achieve a statistical uncertainty of 2 Hz. This paves the way for future high-precision measurements on H2+. The techniques described here could potentially be applied to other light molecular ions.

•Jan 1, 2025•0 citations
Abstract. Preparing molecules at rest and in a highly pure quantum state is a long standing dream in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information on the molecule. The outlined techniques might enable preparation, manipulation and measurement of a large multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics. 1.
Preparing molecules at rest and in a very pure quantum state is a long-standing aspiration in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower-energy states is avoided. Instead, the molecule is always confined to rotational states within the electronic and vibrational ground-state manifold, while a co-trapped atomic ion provides efficient entropy removal and allows for extraction of information about the molecule. The outlined techniques might enable the preparation, manipulation and measurement of a multitude of molecular ion species with the same instrument, with applications including, but not limited to, precise determination of molecular properties and fundamental tests of physics.
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.
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.
Translationally cold, spatially localised molecular ions prepared by sympathetic cooling with laser-cooled atomic ions in ion traps have recently found a wide range of applications in both chemistry and physics. The very low temperatures of the ions (down to millikelvins), their tight localisation in the trap and the ability to control and manipulate single isolated molecules on the quantum level offer intriguing possibilities for new experiments in the realms of cold chemistry, precision molecular spectroscopy, mass spectrometry and quantum technology. The present article gives an overview of the basic experimental methods, current topics and recent developments in this field.
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.
In this thesis I describe how we achieve control over the quantum state of a single H2+ hydrogen molecular ion. Scientific progress is based on the comparison of theories with experimental measurements. For the simplest molecular quantum systems, such as the hydrogen molecular ions H2+ or HD+, the theoretical predictions of quantum electrodynamics are very accurate. In order to test the theory or to extract fundamental constants from the combination of theory and experiments, the experiments must also achieve high precision. In the recent past, hydrogen molecular ions were mainly measured in ensembles. For example, measurements exist both on molecular beams and with dissociative detection in ion traps. However, the spectroscopy of single ions is one of the most precise measurement methods in physics, which was demonstrated by the spectroscopy of a single ytterbium ion in an ion trap. To perform spectroscopy of a single ion in this way, it must have a suitable energy structure for laser cooling, state preparation and fluorescence detection. This is not the case for many ions, including H2+. Quantum logic spectroscopy (QLS) is a technique that makes it possible to perform measurements on an ion without such an energy structure. The ion to be measured (spectroscopy ion) is trapped in an ion trap with a second ion (helper ion), which has the properties described in the previous paragraph. The shared modes of motion between the two ions allow cooling, preparation and detection of the spectroscopy ion via the helper ion. This was demonstrated with an aluminum spectroscopy ion co-trapped with a magnesium helper ion. QLS can also be used for molecules. This has been shown with MgH+, CaH+ and N2+. We implement QLS to enable spectroscopy of a single H2+ ion. For this we trap H2+ together with a 9Be+ ion. We cool the joint motion of the ions to their ground state. We combine buffer gas cooling with a laser and microwave pulse based state preparation sequence to prepare the H2+ molecule in a pure quantum state. This allows us to perform high contrast QLS on a single H2+ ion. Furthermore, we can change and control the quantum state in the hyperfine structure using microwave pulses. We demonstrate the power of our technique by performing microwave spectroscopy on a magnetic field insensitive hyperfine transition. We use QLS to read out the result of the measurement. Within half an hour, we can achieve a statistical uncertainty of 2 Hz. This paves the way for future high-precision measurements on H2+. The techniques described here could potentially be applied to other light molecular ions.