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Coulomb crystallization of xenon highly charged ions in a laser-cooled Ca+ matrix

L. Prokhorov, A.C. Smith, M. Xu, Kostas Georgiou, Vera Guarrera, Lakshmi Priya Kozhiparambil Sajith, Elwin Dijck, Christian Warnecke, M. Wehrheim, A. Wilzewski, L. Blackburn, M. Keller, Vincent Boyer, T. Pfeifer, U. Schwanke, Ç. İşsever, S. D. Worm, P. Schmidt, J. R. Crespo López-Urrutia, Giovanni Barontini

Published Apr 15, 2026• 0 citations
OpenAlex

Abstract

We report the sympathetic cooling and Coulomb crystallization of xenon highly charged ions (HCIs) with laser-cooled Ca+ ions. The HCIs are produced in a compact electron beam ion trap, then charge selected, decelerated, and finally injected into a cryogenic linear Paul trap. There, they are captured into 40 Ca+ Coulomb crystals, and cocrystallized within them, causing dark voids in their fluorescence images. Fine control over the number of trapped ions and HCIs allows us to realize mixed-species crystals with arbitrary ordering patterns. By investigating Xeq+ − Ca+ strings, we confirm the HCI charge states, measure their lifetime, and characterize the mixed-species motional modes. Our system effectively combines the established quantum control toolbox for Ca+ with the rich set of atomic properties of Xe highly charged ions, providing a resourceful platform for optical frequency metrology, searches for signatures of new physics, and quantum information science.

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Coulomb crystallization of xenon highly charged ions in a laser-cooled Ca+ matrix

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physics.atom-phCross-listedarXiv:2512.12266•Physical Review A•Dec 16, 2025•1 citation

Coulomb crystallization of highly charged ions

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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.

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Electron beam ion traps used for spectroscopy of highly charged ions (HCI) produce a deep trapping potential leading to high temperatures of the stored ions, and thus limiting the achievable spectral resolution. A novel device at the Max-Planck-Institut für Kernphysik, the Cryogenic linear Paul Trap Experiment (CryPTEx), attached to an electron beam ion trap, provides a new experimental platform to overcome these limitations. The trap assembly operates at a temperature of 4 K and offers optical access for quantum manipulation and imaging of the trapped ions. Since forbidden optical transitions in HCI do not support direct laser cooling, sympathetic cooling with Coulomb crystals of singly charged ions such as Be+ or Mg+ will be applied in order to reach the natural linewidth of optical forbidden transitions in HCI of interest. With the added advantage of long ion trapping times resulting from residual gas pressures of H2 at 4 K below 10−15 mbar, CryPTEx has been commissioned in collaboration with the Ion Trap Group in Århus using rovibrationally cooled MgH+ ions. Strong suppression of the black body radiation at the trap center, ion storage times of about 28 hours, and largely enhanced population of the rovibrational ground state were achieved.

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Simultaneous control over both excitational and motional degrees of freedom of quantum objects facilitates measurement accuracies at a level that enables the measurement of subtle relativistic effects, tests of the Standard Model and even the search for expected effects of physics beyond it. Theoretical calculations predict enhanced sensitivities of forbidden optical transitions in highly charged ions (HCIs) to possible variations of fundamental constants, such as the fine structure constant. Within this thesis, a versatile preparation technique of cold and strongly localized HCIs has been developed and demonstrated, adding a multitude of laser accessible systems to the quantum toolbox, that have enhanced sensitivity to fundamental physics. HCIs are extracted from an electron beam ion trap (EBIT), where they are produced in the MK temperature range. Subsequently they are cooled down to the mK regime, needed for high precision laser spectroscopy, in a cryogenic linear Paul trap. Deceleration, precooling and multi-pass stopping approaches enable HCI implantation within a prestored, continuously laser-cooled Be+-Coulomb crystal. Here the HCIs are co-crystallized in mixed-species ensembles (specifically Ar13+ highly charged and Be+ coolant ions) - ranging from large 3-dimensional crystals over ion strings down to a single Ar13+ ion cooled by a single Be+ ion. The precooling, retrapping and sympathetic stopping process, as well as various Coulomb crystal configurations are characterized and compared to simulations and theoretical models. The developed experimental concept and its modular implementation enable, for the first time, the localization of HCIs in a microscopic region of a Paul trap, today's standard method for singly-charged ion frequency metrology. This is a necessary prerequisite for the development of novel ultra-precise optical clocks based on quantum logic spectroscopy on forbidden transitions in HCIs and subsequent low-energy searches for physics beyond the Standard Model.

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Coulomb crystals, containing up to a few hundred ions of which more than 50% were cooled sympathetically by the Coulomb interaction with laser cooled Mg+ ions, have been produced in a linear Paul trap. By controlling the balance of the radiation pressure from the two cooling lasers, the Coulomb crystals could be segregated according to ion species. Previous studies of ion crystals and molecular dynamics simulations suggest that the temperature may be around 10 mK or lower. The obtained results indicate that a wide range of atomic and molecular ions, which due to their internal structures are not amenable to direct laser cooling, can be effectively cooled and localized (crystallized) in linear Paul traps. For high resolution spectroscopy of such ions this may turn out to be very useful.

AIP conference proceedings•Jan 1, 1999•0 citations
We report the sympathetic cooling and Coulomb crystallization of xenon highly charged ions (HCIs) with laser-cooled Ca+ ions. The HCIs are produced in a compact electron beam ion trap, then charge selected, decelerated, and finally injected into a cryogenic linear Paul trap. There, they are captured into 40 Ca+ Coulomb crystals, and cocrystallized within them, causing dark voids in their fluorescence images. Fine control over the number of trapped ions and HCIs allows us to realize mixed-species crystals with arbitrary ordering patterns. By investigating Xeq+ − Ca+ strings, we confirm the HCI charge states, measure their lifetime, and characterize the mixed-species motional modes. Our system effectively combines the established quantum control toolbox for Ca+ with the rich set of atomic properties of Xe highly charged ions, providing a resourceful platform for optical frequency metrology, searches for signatures of new physics, and quantum information science.
We report on the sympathetic cooling and Coulomb crystallization of xenon highly charged ions (HCIs) with laser-cooled Ca+^++ ions. The HCIs are produced in a compact electron beam ion trap, then charge selected, decelerated, and finally injected into a cryogenic linear Paul trap. There, they are captured into 40^{40}40Ca+^++ Coulomb crystals, and co-crystallized within them, causing dark voids in their fluorescence images. Fine control over the number of trapped ions and HCIs allows us to realize mixed-species crystals with arbitrary ordering patterns. By investigating Xeq+^{q+}q+--Ca+^++ strings, we confirm the HCI charge states, measure their lifetime and characterize the mixed-species motional modes. Our system effectively combines the established quantum control toolbox for Ca+^++ with the rich set of atomic properties of Xe highly charged ions, providing a resourceful platform for optical frequency metrology, searches for signatures of new physics, and quantum information science.
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.
Electron beam ion traps used for spectroscopy of highly charged ions (HCI) produce a deep trapping potential leading to high temperatures of the stored ions, and thus limiting the achievable spectral resolution. A novel device at the Max-Planck-Institut für Kernphysik, the Cryogenic linear Paul Trap Experiment (CryPTEx), attached to an electron beam ion trap, provides a new experimental platform to overcome these limitations. The trap assembly operates at a temperature of 4 K and offers optical access for quantum manipulation and imaging of the trapped ions. Since forbidden optical transitions in HCI do not support direct laser cooling, sympathetic cooling with Coulomb crystals of singly charged ions such as Be+ or Mg+ will be applied in order to reach the natural linewidth of optical forbidden transitions in HCI of interest. With the added advantage of long ion trapping times resulting from residual gas pressures of H2 at 4 K below 10−15 mbar, CryPTEx has been commissioned in collaboration with the Ion Trap Group in Århus using rovibrationally cooled MgH+ ions. Strong suppression of the black body radiation at the trap center, ion storage times of about 28 hours, and largely enhanced population of the rovibrational ground state were achieved.
Simultaneous control over both excitational and motional degrees of freedom of quantum objects facilitates measurement accuracies at a level that enables the measurement of subtle relativistic effects, tests of the Standard Model and even the search for expected effects of physics beyond it. Theoretical calculations predict enhanced sensitivities of forbidden optical transitions in highly charged ions (HCIs) to possible variations of fundamental constants, such as the fine structure constant. Within this thesis, a versatile preparation technique of cold and strongly localized HCIs has been developed and demonstrated, adding a multitude of laser accessible systems to the quantum toolbox, that have enhanced sensitivity to fundamental physics. HCIs are extracted from an electron beam ion trap (EBIT), where they are produced in the MK temperature range. Subsequently they are cooled down to the mK regime, needed for high precision laser spectroscopy, in a cryogenic linear Paul trap. Deceleration, precooling and multi-pass stopping approaches enable HCI implantation within a prestored, continuously laser-cooled Be+-Coulomb crystal. Here the HCIs are co-crystallized in mixed-species ensembles (specifically Ar13+ highly charged and Be+ coolant ions) - ranging from large 3-dimensional crystals over ion strings down to a single Ar13+ ion cooled by a single Be+ ion. The precooling, retrapping and sympathetic stopping process, as well as various Coulomb crystal configurations are characterized and compared to simulations and theoretical models. The developed experimental concept and its modular implementation enable, for the first time, the localization of HCIs in a microscopic region of a Paul trap, today's standard method for singly-charged ion frequency metrology. This is a necessary prerequisite for the development of novel ultra-precise optical clocks based on quantum logic spectroscopy on forbidden transitions in HCIs and subsequent low-energy searches for physics beyond the Standard Model.
Optical clocks have garnered widespread attention due to their unparalleled precision in time-frequency standards, geodetic measurements, and fundamental physics research. Among emerging developments, highly charged ion (HCI)-based optical clocks have attracted significant scientific interest owing to their exceptional resilience against electromagnetic perturbations and enhanced sensitivity to variations in the fine-structure constant (ααα). While the recent successful demonstration of an Ar13+^{13+}13+ optical clock has validated the feasibility of HCI-based systems, Ni12+^{12+}12+ -- featuring an ultranarrow clock transition linewidth -- stands out as a superior candidate for achieving HCI optical clocks with 10−1910^{-19}10−19 level uncertainty and stability. In this work, we report the Coulomb crystallization of nickel highly charged ions (Ni-HCIs). Through a precision deceleration and sympathetic cooling protocol in a room-temperature Paul trap, high-energy Ni-HCI bunches were sympathetically cooled from megakelvin to the 100-millikelvin range using laser-cooled Be+^{+}+ ions. This work represents a pivotal step toward the realization of an optical clock based on the Ni12+^{12+}12+ ion.
Coulomb crystals, containing up to a few hundred ions of which more than 50% were cooled sympathetically by the Coulomb interaction with laser cooled Mg+ ions, have been produced in a linear Paul trap. By controlling the balance of the radiation pressure from the two cooling lasers, the Coulomb crystals could be segregated according to ion species. Previous studies of ion crystals and molecular dynamics simulations suggest that the temperature may be around 10 mK or lower. The obtained results indicate that a wide range of atomic and molecular ions, which due to their internal structures are not amenable to direct laser cooling, can be effectively cooled and localized (crystallized) in linear Paul traps. For high resolution spectroscopy of such ions this may turn out to be very useful.