Chunhai Lyu

Ultraintense pulses from X-ray free-electron lasers can drive, within femtoseconds, multiple processes in the inner shells of atoms and molecules in all phases of matter. The ensuing complex ionization pathways of outer-shell electrons from the neutral to the final highly charged states make a comparison with theory enormously difficult. We resolve these pathways by preparing highly charged ions in an electron beam ion trap before exposing them to the pulsed radiation. This reveals how relativistic fine-structure effects shift electronic energies, largely compensate the core-screening potential, and enable the consecutive, resonant absorption of two quasi-monochromatic X-ray photons that would generally be unfeasible. This doubly-resonant channel enhances the efficiency of two-photon ionization by more than two orders of magnitude, dominating in this regime the nonlinear interaction of light and matter with possible application for future precision X-ray metrology.

The atomic mass of uranium-238 has been determined to be $238.050\,787\,618(15)\,\text{u}$, improving the literature uncertainty by two orders of magnitude. It is obtained from a measurement of the mass ratio of $^{238}$U$^{47+}$ and $^{132}$Xe$^{26+}$ ions with an uncertainty of $3.5\times 10^{-12}$. The measurement was carried out with the Penning-trap mass spectrometer \textsc{Pentatrap} and was accompanied by a calculation of the binding energies $E_{\text{U}}$ and $E_{\text{Xe}}$ of the 47 and 26 missing electrons of the two highly charged ions, respectively. These binding energies were determined using an \textit{ab initio} multiconfiguration Dirac-Hartree-Fock (MCDHF) method to be $E_{\text{U}} = 39\,927(10)\,\text{eV}$ and $E_{\text{Xe}} = 8\,971.2(21)\,\text{eV}$. The new mass value will serve as a reference for high-precision mass measurements in the heavy mass region of the nuclear chart up to transuranium nuclides.

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 XUV 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$^{41+}$ which 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 $4\times10^{-12}$. This experimental result agrees within 1 $σ$ with two partially different \textit{ab initio} multi-configuration 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 $1.1\times10^{23}$ and allows for the construction of a HCI clock with a fractional frequency instability of $<10^{-19}/\sqrtτ$.