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Coherent laser spectroscopy of highly charged ions using quantum logic

P. Micke, Tobias Leopold, S. A. King, Erik Benkler, Lukas J. Spieß, L. Schmöger, M. Schwarz, J. R. Crespo López-Urrutia, Piet O. Schmidt

Published Jan 29, 2020• 35 citations
OpenAlex

Abstract

Abstract Precision spectroscopy of atomic systems1 is an invaluable tool for the study of fundamental interactions and symmetries2. Recently, highly charged ions have been proposed to enable sensitive tests of physics beyond the standard model2–5 and the realization of high-accuracy atomic clocks3, 5, owing to their high sensitivity to fundamental physics and insensitivity to external perturbations, which result from the high binding energies of their outer electrons. However, the implementation of these ideas has been hindered by the low spectroscopic accuracies (of the order of parts per million) achieved so far6–8. Here we cool trapped, highly charged argon ions to the lowest temperature reported so far, and study them using coherent laser spectroscopy, achieving an increase in precision of eight orders of magnitude. We use quantum logic spectroscopy9, 10 to probe the forbidden optical transition in 40Ar13+ at a wavelength of 441 nanometres and measure its excited-state lifetime and g-factor. Our work unlocks the potential of highly charged ions as ubiquitous atomic systems for use in quantum information processing, as frequency standards and in highly sensitive tests of fundamental physics, such as searches for dark-matter candidates11 or violations of fundamental symmetries2.

Related papers

Quantum Logic Spectroscopy of Highly Charged Ions

P. Micke

Fundamental interactions and symmetries define the structure and properties of all matter, in particular of its small and diverse visible constituents—the atoms. The study of their distinctive spectra through precision spectroscopy is therefore a vital tool to advance our understanding of nature. Highly charged ions (HCIs) constitute the largest fraction of all atoms since every atom has as many charge states as electrons it can bind. Although most of the matter on Earth is neutral, HCIs are ubiquitous in the universe and their systematic study is essential not only for atomic physics but eminently for astrophysics, nuclear physics, and fusion research, among others. Recently, HCIs have been identified as ideal candidates for sensitive tests of physics beyond the Standard Model of particle physics and for use in future high-accuracy optical atomic clocks. However, the realization of such proposals has been hindered by the hitherto constrained laboratory control and limited spectroscopic accuracy of about parts-per-million fractional uncertainty levels. This thesis reports the first coherent laser spectroscopy of HCIs, boosting the achievable spectroscopic precision by eight orders of magnitude compared to traditional spectroscopy methods. The 2P1/2–2P3/2 fine-structure ground-state transition in highly charged 40Ar13+ at an optical wavelength of 441 nm was chosen as a proof-of-principle case. A single ion of this species was isolated from a megakelvin-hot plasma cloud and co-trapped together with a laser-cooled singly charged 9Be+ ion in a two-ion crystal, confined in the harmonic potential of a cryogenic linear Paul trap. This coupled quantum-mechanical system was then cooled to its ground state of axial motion, corresponding to the lowest temperature of a HCI ever achieved. The spectroscopy was realized by implementing quantum logic techniques which allow preparation of the quantum state of the HCI and to map its electronic state after spectroscopy onto the 9Be+ logic ion in order to detect it there with high efficiency through electron shelving. In addition to the increase of spectroscopic precision, the excited-state lifetime and g-factor were measured—the latter one to unprecedented accuracy, resolving effects from special relativity, interelectronic interactions, and quantum electrodynamics. Moreover, it settled a discrepancy between theoretical predictions. The demonstrated techniques are not limited to the specific 40Ar13+ species but universally applicable to other HCIs. Thereby, this work unlocks the potential of HCIs for unrivaled tests of fundamental physics, the search for new physics—such as a 5th force, variations of fundamental constants and dark matter candidates—as well as the use of HCIs in novel optical atomic clocks.

•Jan 1, 2020•1 citation

Methods of quantum logic in ion frequency standards, quantum computers, and modern spectroscopy

Ksenia Yu. Khabarova, Ilia V. Zalivako, N. Kolachevsky

Today, precise laser control of the quantum states of single ions cooled to low temperatures in traps ensures significant progress in the development of such physical areas as optical and microwave frequency standards, quantum computing, and accurate measurements of transition frequencies to confirm fundamental physical theories.Pioneering ideas about the possibility of using lasers in the development of frequency standards, expressed in the 1960s by the Nobel laureate N G Basov, have enjoyed rapid development: the relative accuracy of frequency standards has reached the 18th decimal place, and the experimentally demonstrated coherence time of narrow optical transitions amounts to tens of seconds.The paper presents a selective review, as well as the results of research at the Lebedev Physical Institute, in the area of using elements of quantum logic in the action of coherent laser pulses on single ions.Also discussed is the use of quantum logic methods in optical clocks based on the Al + ion and the multiply charged Al + ion, and also in quantum computers based on Ca + and Yb + ions.

Physics-Uspekhi•Oct 1, 2022•16 citations

Al+ Optical Clocks for Fundamental Physics and Geodesy

James Chin-wen Chou

Laser-cooled trapped atoms have long been recognized as potentially very accurate frequency standards for clocks. Ultimate accuracies of 10-18 to 10-19 appear possible, limited by the time-dilation of trapped ions that move at laser-cooled velocities. The Al+ ion is an attractive candidate for high accuracy, owing to its narrow electronic transition in the optical regime and low sensitivity to ambient field perturbations. Precision spectroscopy on Al+ is enabled by quantum information techniques. With Al+ “quantum-logic” clocks, the current accuracy of 8.6×10-18 has enabled a geo-potential-difference measurement that detected a height change of 37±17 cm due to the gravitational red-shift. We have also observed quantum coherence between two Al+ ions with a record Q-factor of 3.4×1016, and compared the Al+ resonance frequency to that of a single Hg+ ion to place limits on the temporal variation of the fine-structure constant.

•Jul 13, 2011•0 citations

Collective Quantum Logic Spectroscopy

Raphael Kaubruegger, Matthew Patkowski, Yicheng Zhang +3 more

Scaling trapped-ion quantum sensors from single ions to large ensembles is a key challenge for next-generation precision measurements. At the same time, many ion species of interest for optical clocks and tests of fundamental physics lack closed cycling transitions required for direct laser cooling and state detection. Collective quantum logic spectroscopy addresses both limitations by coupling an ensemble of sensor, or spectroscopy, ions to one or more logic ions that provide sympathetic cooling and state readout. Here, we establish the fundamental performance limits and operating regimes of this protocol, identifying how the interaction strength, interrogation time, and logic-ensemble size govern sensitivity, dynamic range, and robustness to experimental imperfections. We show that quantum-limited sensitivity can be retained even with a single logic ion, while increasing the number of logic ions substantially improves readout efficiency and robustness. Beyond precision metrology, the same collective interface enables many-body measurements relevant to quantum information processing, including parity measurements and stabilizer-like syndrome extraction. Our results establish collective quantum logic spectroscopy as a scalable framework for optical clocks, quantum-enhanced sensing, and trapped-ion quantum information processing.

quant-pharXiv:2608.20471•Aug 24, 2026•0 citations

Coulomb crystallization of highly charged ions

L. Schmöger, Oscar O. Versolato, M. Schwarz +13 more

Control over the motional degrees of freedom of atoms, ions, and molecules in a field-free environment enables unrivalled measurement accuracies but has yet to be applied to highly charged ions (HCIs), which are of particular interest to future atomic clock designs and searches for physics beyond the Standard Model. Here, we report on the Coulomb crystallization of HCIs (specifically (40)Ar(13+)) produced in an electron beam ion trap and retrapped in a cryogenic linear radiofrequency trap by means of sympathetic motional cooling through Coulomb interaction with a directly laser-cooled ensemble of Be(+) ions. We also demonstrate cooling of a single Ar(13+) ion by a single Be(+) ion-the prerequisite for quantum logic spectroscopy with a potential 10(-19) accuracy level. Achieving a seven-orders-of-magnitude decrease in HCI temperature starting at megakelvin down to the millikelvin range removes the major obstacle for HCI investigation with high-precision laser spectroscopy.

Science•Mar 12, 2015•138 citations

Quantum-logic spectroscopy of forbidden vibrational transitions in single nitrogen molecular ions

Aleksandr Shlykov, Meissa L. Diouf, Richard Karl +3 more

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, N$_2^+$, 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

physics.atom-phCross-listedarXiv:2603.10553•Nature Communications•Mar 12, 2026•0 citations
Abstract Precision spectroscopy of atomic systems1 is an invaluable tool for the study of fundamental interactions and symmetries2. Recently, highly charged ions have been proposed to enable sensitive tests of physics beyond the standard model2–5 and the realization of high-accuracy atomic clocks3, 5, owing to their high sensitivity to fundamental physics and insensitivity to external perturbations, which result from the high binding energies of their outer electrons. However, the implementation of these ideas has been hindered by the low spectroscopic accuracies (of the order of parts per million) achieved so far6–8. Here we cool trapped, highly charged argon ions to the lowest temperature reported so far, and study them using coherent laser spectroscopy, achieving an increase in precision of eight orders of magnitude. We use quantum logic spectroscopy9, 10 to probe the forbidden optical transition in 40Ar13+ at a wavelength of 441 nanometres and measure its excited-state lifetime and g-factor. Our work unlocks the potential of highly charged ions as ubiquitous atomic systems for use in quantum information processing, as frequency standards and in highly sensitive tests of fundamental physics, such as searches for dark-matter candidates11 or violations of fundamental symmetries2.
Fundamental interactions and symmetries define the structure and properties of all matter, in particular of its small and diverse visible constituents—the atoms. The study of their distinctive spectra through precision spectroscopy is therefore a vital tool to advance our understanding of nature. Highly charged ions (HCIs) constitute the largest fraction of all atoms since every atom has as many charge states as electrons it can bind. Although most of the matter on Earth is neutral, HCIs are ubiquitous in the universe and their systematic study is essential not only for atomic physics but eminently for astrophysics, nuclear physics, and fusion research, among others. Recently, HCIs have been identified as ideal candidates for sensitive tests of physics beyond the Standard Model of particle physics and for use in future high-accuracy optical atomic clocks. However, the realization of such proposals has been hindered by the hitherto constrained laboratory control and limited spectroscopic accuracy of about parts-per-million fractional uncertainty levels. This thesis reports the first coherent laser spectroscopy of HCIs, boosting the achievable spectroscopic precision by eight orders of magnitude compared to traditional spectroscopy methods. The 2P1/2–2P3/2 fine-structure ground-state transition in highly charged 40Ar13+ at an optical wavelength of 441 nm was chosen as a proof-of-principle case. A single ion of this species was isolated from a megakelvin-hot plasma cloud and co-trapped together with a laser-cooled singly charged 9Be+ ion in a two-ion crystal, confined in the harmonic potential of a cryogenic linear Paul trap. This coupled quantum-mechanical system was then cooled to its ground state of axial motion, corresponding to the lowest temperature of a HCI ever achieved. The spectroscopy was realized by implementing quantum logic techniques which allow preparation of the quantum state of the HCI and to map its electronic state after spectroscopy onto the 9Be+ logic ion in order to detect it there with high efficiency through electron shelving. In addition to the increase of spectroscopic precision, the excited-state lifetime and g-factor were measured—the latter one to unprecedented accuracy, resolving effects from special relativity, interelectronic interactions, and quantum electrodynamics. Moreover, it settled a discrepancy between theoretical predictions. The demonstrated techniques are not limited to the specific 40Ar13+ species but universally applicable to other HCIs. Thereby, this work unlocks the potential of HCIs for unrivaled tests of fundamental physics, the search for new physics—such as a 5th force, variations of fundamental constants and dark matter candidates—as well as the use of HCIs in novel optical atomic clocks.
Today, precise laser control of the quantum states of single ions cooled to low temperatures in traps ensures significant progress in the development of such physical areas as optical and microwave frequency standards, quantum computing, and accurate measurements of transition frequencies to confirm fundamental physical theories.Pioneering ideas about the possibility of using lasers in the development of frequency standards, expressed in the 1960s by the Nobel laureate N G Basov, have enjoyed rapid development: the relative accuracy of frequency standards has reached the 18th decimal place, and the experimentally demonstrated coherence time of narrow optical transitions amounts to tens of seconds.The paper presents a selective review, as well as the results of research at the Lebedev Physical Institute, in the area of using elements of quantum logic in the action of coherent laser pulses on single ions.Also discussed is the use of quantum logic methods in optical clocks based on the Al + ion and the multiply charged Al + ion, and also in quantum computers based on Ca + and Yb + ions.
Laser-cooled trapped atoms have long been recognized as potentially very accurate frequency standards for clocks. Ultimate accuracies of 10-18 to 10-19 appear possible, limited by the time-dilation of trapped ions that move at laser-cooled velocities. The Al+ ion is an attractive candidate for high accuracy, owing to its narrow electronic transition in the optical regime and low sensitivity to ambient field perturbations. Precision spectroscopy on Al+ is enabled by quantum information techniques. With Al+ “quantum-logic” clocks, the current accuracy of 8.6×10-18 has enabled a geo-potential-difference measurement that detected a height change of 37±17 cm due to the gravitational red-shift. We have also observed quantum coherence between two Al+ ions with a record Q-factor of 3.4×1016, and compared the Al+ resonance frequency to that of a single Hg+ ion to place limits on the temporal variation of the fine-structure constant.
Scaling trapped-ion quantum sensors from single ions to large ensembles is a key challenge for next-generation precision measurements. At the same time, many ion species of interest for optical clocks and tests of fundamental physics lack closed cycling transitions required for direct laser cooling and state detection. Collective quantum logic spectroscopy addresses both limitations by coupling an ensemble of sensor, or spectroscopy, ions to one or more logic ions that provide sympathetic cooling and state readout. Here, we establish the fundamental performance limits and operating regimes of this protocol, identifying how the interaction strength, interrogation time, and logic-ensemble size govern sensitivity, dynamic range, and robustness to experimental imperfections. We show that quantum-limited sensitivity can be retained even with a single logic ion, while increasing the number of logic ions substantially improves readout efficiency and robustness. Beyond precision metrology, the same collective interface enables many-body measurements relevant to quantum information processing, including parity measurements and stabilizer-like syndrome extraction. Our results establish collective quantum logic spectroscopy as a scalable framework for optical clocks, quantum-enhanced sensing, and trapped-ion quantum information processing.
Control over the motional degrees of freedom of atoms, ions, and molecules in a field-free environment enables unrivalled measurement accuracies but has yet to be applied to highly charged ions (HCIs), which are of particular interest to future atomic clock designs and searches for physics beyond the Standard Model. Here, we report on the Coulomb crystallization of HCIs (specifically (40)Ar(13+)) produced in an electron beam ion trap and retrapped in a cryogenic linear radiofrequency trap by means of sympathetic motional cooling through Coulomb interaction with a directly laser-cooled ensemble of Be(+) ions. We also demonstrate cooling of a single Ar(13+) ion by a single Be(+) ion-the prerequisite for quantum logic spectroscopy with a potential 10(-19) accuracy level. Achieving a seven-orders-of-magnitude decrease in HCI temperature starting at megakelvin down to the millikelvin range removes the major obstacle for HCI investigation with high-precision laser spectroscopy.
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