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High-Precision Spectroscopy of the 2 3S1 → 2 1S0 Transition in Quantum Degenerate 4He and 3He

Kees Steinebach

Published Aug 5, 2026• 0 citations
Publisher

Abstract

Although the Standard Model is highly successful, it is not complete. One approach to searching for effects beyond our current understanding of physics is to measure finite-size effects in simple atomic systems through high-precision spectroscopy. In this thesis, we present new measurements of the 2 3S1 -> 2 1S0 transition in 3He and 4He with the highest precision achieved to date. We perform these measurements in ultracold trapped gases in the quantum-degenerate regime. These spectroscopic measurements are used to determine the difference in charge radius between the helion and the alpha particle, the nuclei of 3He and 4He, respectively. By comparing the extracted charge-radius difference with values obtained from other experiments, we test isotope-shift calculations and bound-state quantum electrodynamics.

DOI
10.5463/thesis.1697

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Although the Standard Model is highly successful, it is not complete. One approach to searching for effects beyond our current understanding of physics is to measure finite-size effects in simple atomic systems through high-precision spectroscopy. In this thesis, we present new measurements of the 2 3S1 -> 2 1S0 transition in 3He and 4He with the highest precision achieved to date. We perform these measurements in ultracold trapped gases in the quantum-degenerate regime. These spectroscopic measurements are used to determine the difference in charge radius between the helion and the alpha particle, the nuclei of 3He and 4He, respectively. By comparing the extracted charge-radius difference with values obtained from other experiments, we test isotope-shift calculations and bound-state quantum electrodynamics.
The helium atom, being a calculable system with narrow transitions that can be measured precisely, is an excellent candidate for testing state-of-the-art Quantum Electrodynamics calculations. This thesis presents a series of precise spectroscopic measurements on a narrow transition in ultracold trapped quantum gases of helium, using both the 3-He and 4-He isotopes, which exhibit distinctly different quantum-statistical behaviour in this ultracold regime. From the shift of this transition between the two isotopes, the difference in their nuclear charge radii is extracted, which is used as a benchmark quantity for comparison with other measurements and tests of Quantum Electrodynamics theory.
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−2S1S-2S1S−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−2S1S-2S1S−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−2S1S-2S1S−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∞R_{\infty}R∞​ 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.
Precision spectroscopy of simple atomic systems has refined our understanding of the fundamental laws of quantum physics. In particular, helium spectroscopy has played a crucial role in describing two-electron interactions, determining the fine-structure constant and extracting the size of the helium nucleus. Here we present a measurement of the doubly forbidden 1557-nanometer transition connecting the two metastable states of helium (the lowest energy triplet state 2 (3)S(1) and first excited singlet state 2 (1)S(0)), for which quantum electrodynamic and nuclear size effects are very strong. This transition is weaker by 14 orders of magnitude than the most predominantly measured transition in helium. Ultracold, submicrokelvin, fermionic (3)He and bosonic (4)He atoms are used to obtain a precision of 8 × 10(-12), providing a stringent test of two-electron quantum electrodynamic theory and of nuclear few-body theory.
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.
Exotic helium atoms act as unique atomic traps for heavy, negatively charged particles, protecting them from nuclear annihilation and nuclear capture on timescales long enough to enable high-precision laser spectroscopy. Such measurements serve as stringent tests of three-body quantum electrodynamics and offer a direct route to determining fundamental particle masses. Motivated by upcoming spectroscopic efforts targeting pionic (π− 4He+π^{-\,4}\mathrm{He}^+π−4He+) and kaonic (K− 4He+K^{-\,4}\mathrm{He}^+K−4He+) helium, we present a rigorous theoretical evaluation of the collisional and density effects governing these systems. Using an ab initio potential energy surface and coupled-channel quantum scattering calculations, we study the collisional stability of the candidate metastable states against inelastic quenching in a cryogenic helium buffer gas. Furthermore, we provide theoretical reference values for the pressure broadening and pressure shift coefficients of the targeted transitions. These results establish an essential benchmark for future experiments, paving the way for refined determinations of the pion and kaon masses.
A large-scale full-configuration-interaction calculation based on the Dirac-Coulomb-Breit (DCB) Hamiltonian is performed for the 21S02{\phantom{\rule{0.16em}{0ex}}}^{1}{S}_{0}21S0​ and 23S12{\phantom{\rule{0.16em}{0ex}}}^{3}{S}_{1}23S1​ states of helium. The operators of the normal and specific mass shifts are directly included in the DCB framework to take the finite nuclear mass correction into account. High-accuracy energies and matrix elements involved nnn (the main quantum number) up to 13 are obtained from one diagonalization of Hamiltonian. The dynamic dipole polarizabilities are calculated by using the sum rule of intermediate states, and a series of magic wavelengths with QED and hyperfine effects included for the $2{\phantom{\rule{0.16em}{0ex}}}^{3}{S}_{1}\ensuremath{\rightarrow}2{\phantom{\rule{0.16em}{0ex}}}^{1}{S}_{0}$ transition of helium are identified. In addition, the high-order ac Stark shift determined by the dynamic hyperpolarizabilities at the magic wavelengths are also evaluated. Since the most promising magic wavelength for application in experiment is 319.8 nm, the high-accuracy magic wavelength of 319.815 3(6) nm of 4He^{4}\mathrm{He}4He is in good agreement with the recent measurement value of 319.815 92(15) nm [R. J. Rengelink et al., arXiv:1804.06693], and the present magic wavelength of 319.830 2(7) nm for 3He^{3}\mathrm{He}3He would provide theoretical support for experimentally designing an optical dipole trap to precisely determine the nuclear charge radius of helium in the future.