Observation of a Low-Lying Metastable Electronic State in Highly Charged Lead by Penning-Trap Mass Spectrometry.

Highly charged ions (HCIs) offer many opportunities for next-generation clock research due to the vast landscape of available electronic transitions in different charge states. The development of extreme ultraviolet frequency combs has enabled the search for clock transitions based on shorter wavelengths in HCIs. However, without initial knowledge of the energy of the clock states, these narrow transitions are difficult to be probed by lasers. In this Letter, we provide experimental observation and theoretical calculation of a long-lived electronic state in Nb-like Pb^{41+} that could be used as a clock state. With the mass spectrometer PENTATRAP, the excitation energy of this metastable state is directly determined as a mass difference at an energy of 31.2(8) eV, corresponding to one of the most precise relative mass determinations to date with a fractional uncertainty of 4×10^{-12}. This experimental result agrees within 1σ with two partially different ab initio multiconfiguration Dirac-Hartree-Fock calculations of 31.68(13) eV and 31.76(35) eV, respectively. With a calculated lifetime of 26.5(5.3) days, the transition from this metastable state to the ground state bears a quality factor of 1.1×10^{23} and allows for the construction of a HCI clock with a fractional frequency instability of <10^{-19}/sqrt[τ].

High-precision mass measurement of doubly magic 208 Pb.

The absolute atomic mass of 208 Pb has been determined with a fractional uncertainty of 7 × 10 - 11 by measuring the cyclotron-frequency ratio R of 208 Pb 41 + to 132 Xe 26 + with the high-precision Penning-trap mass spectrometer Pentatrap and computing the binding energies E Pb and E Xe of the missing 41 and 26 atomic electrons, respectively, with the ab initio fully relativistic multi-configuration Dirac-Hartree-Fock (MCDHF) method. R has been measured with a relative precision of 9 × 10 - 12 . E Pb and E Xe have been computed with an uncertainty of 9.1 eV and 2.1 eV, respectively, yielding 207.976 650 571 ( 14 )  u ( u = 9.314 941 024 2 ( 28 ) × 10 8  eV/c 2 ) for the 208 Pb neutral atomic mass. This result agrees within 1.2 σ with that from the Atomic-Mass Evaluation (AME) 2020, while improving the precision by almost two orders of magnitude. The new mass value directly improves the mass precision of 14 nuclides in the region of Z = 81-84 and is the most precise mass value with A > 200 . Thus, the measurement establishes a new region of reference mass values which can be used e.g. for precision mass determination of transuranium nuclides, including the superheavies.

Interrogating the Temporal Coherence of EUV Frequency Combs with Highly Charged Ions.

A scheme to infer the temporal coherence of EUV frequency combs generated from intracavity high-order harmonic generation is put forward. The excitation dynamics of highly charged Mg-like ions, which interact with EUV pulse trains featuring different carrier-envelope-phase fluctuations, are simulated. While demonstrating the microscopic origin of the macroscopic equivalence between excitations induced by pulse trains and continuous-wave lasers, we show that the coherence time of the pulse train can be determined from the spectrum of the excitations. The scheme will provide a verification of the comb temporal coherence at timescales several orders of magnitude longer than current state of the art, and at the same time will enable high-precision spectroscopy of EUV transitions with a relative accuracy up to δω/ω∼10^{-17}.

Narrow-band hard-x-ray lasing with highly charged ions.

A scheme is put forward to generate fully coherent x-ray lasers based on population inversion in highly charged ions, created by fast inner-shell photoionization using broadband x-ray free-electron-laser (XFEL) pulses in a laser-produced plasma. Numerical simulations based on the Maxwell-Bloch theory show that one can obtain high-intensity, femtosecond x-ray pulses of relative bandwidths Δω/ω = 10-5-10-7, by orders of magnitude narrower than in x-ray free-electron-laser pulses for discrete wavelengths down to the sub-ångström regime. Such x-ray lasers can be applicable in the study of x-ray quantum optics and metrology, investigating nonlinear interactions between x-rays and matter, or in high-precision spectroscopy studies in laboratory astrophysics.