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arXiv:2608.23516

Extreme-ultraviolet spectroscopy using quantum logic: a feasibility study for singly-ionized helium

A. Martínez de Velasco, V. P. J. Barbé, E. L. Gründeman, A. Díaz Calderon, M. Collombon, J. J. Krauth, C. F. Roth, M. Favier, R. Taieb, T. E. Mehlstäubler, P. O. Schmidt, L. S. Dreissen, K. S. E. Eikema

physics.atom-phquant-phSubmitted Aug 24, 2026• Announced Aug 25, 2026
v1 · Aug 24, 2026v2 · Sep 24, 2026
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Abstract

Extreme-ultraviolet (XUV) spectroscopy represents an important new direction in precision physics, with potential applications ranging from the metrology of fundamental constants to tests of physics beyond the Standard Model. However, the application of quantum control methods for precision spectroscopy remains an open challenge in the XUV range. Here we present a novel quantum logic (QL) spectroscopy method for precision spectroscopy of weak XUV transitions, and numerically validate its feasibility for the $1S-2S$ transition at 40.81\,eV in singly-ionized helium (He$^{+}$). We propose a scheme based on a single He$^{+}$ ion co-trapped with a Be$^{+}$ ion in a Paul trap, and He$^{+}$ excitation with pairs of frequency-comb (FC) laser pulses upconverted to the XUV via High-Harmonic Generation (HHG). We investigate a nondestructive QL scheme to detect $1S-2S$ excitation, and compare its performance with a destructive readout based on state-selective ionization. Phase coherence of the XUV light is modelled and an optical cavity is used to filter the FC pulses prior to HHG. We model the motional excitation dynamics of trapped ions outside the Lamb-Dicke regime, and numerically validate a scheme we proposed in \cite{Grundeman} to cancel the first-order Doppler broadening and the recoil shift by synchronizing the ion's secular period with the time delay between the two excitation pulses. We show that precision spectroscopy of the $1S-2S$ transition in He$^{+}$ at the 10 kHz level is feasible, for improved tests of quantum electrodynamics (QED), a measurement of the Rydberg constant $R_{\infty}$ independent of hydrogen measurements, or an improved determination of the alpha particle and helion charge radii. The proposed method may also be applied to XUV spectroscopy of other ions outside the Lamb-Dicke regime.

Comments
26 pages, 19 figures

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Abstract Ultrashort, coherent light pulses in the extreme ultraviolet (XUV) wavelength region are excellent tools for a wide range of experiments. These XUV pulses are in particular used to characterize electron dynamics. Additionally, the high photon energy enables quantum control of short-lived transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Coherent XUV pulses would be even more useful if the tools to control and manipulate them existed. Presently, however, no modulators exist for these frequencies, which significantly reduces the number of possible ultrafast optics experiments and applications in the XUV regime. This Ph.D. tutorial addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light we have developed a method for opto-optical modulation (OOM), which modulates the phase of XUV light emitted from a gas of atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation and emit light after the excitation pulse passed. By shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse, the phase of the emitted light, and therefore its wavefront, is controlled. With OOM the direction of XUV light emitted from noble gases has been controlled, and the temporal dynamics of the emission studied. By varying the delay between the excitation and the control pulse, the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, a proof-of-principle experiment with two control pulses was performed, resulting in a shaped XUV pulse with controlled duration. The technique of OOM presented in this article is still at a very early stage and in order to obtain complete control of the amplitude and phase of the XUV pulses further development is necessary. Such development would present new opportunities for ultrafast XUV quantum control.
Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.
Abstract Precision spectroscopy has been the driving force for progress of our physical understanding and still is a promising tool for the investigation of new physics. Molecules offer transitions which allow tests that are not possible in atomic systems. However, usually precision spectroscopy of molecules is challenging due to the lack of cycling transitions for state preparation and state detection. For molecular ions, this obstacle can be overcome by quantum logic spectroscopy, where dissipation for state preparation and detection is provided by a co-trapped atomic ion exploiting the shared eigenstates of motion. Here, we propose a full quantum logic spectroscopy scheme for molecular oxygen ions and theoretically investigate the feasibility of quantum logic-assisted state detection and preparation. Furthermore, we provide coupling rates for a direct single-photon quadrupole excitation of a vibrational overtone transition that can serve as a sensitive reference for tests of a possible variation of the proton-to-electron mass ratio.