High-Precision Multiphoton Ionization of Accelerated Laser-Ablated Species

We demonstrate that the pulsed-time structure and high-peak ion intensity provided by the laser-ablation process can be directly combined with the high resolution, high efficiency, and low background offered by collinear resonance ionization spectroscopy. This simple, versatile, and powerful method offers new and unique opportunities for high-precision studies of atomic and molecular structures, impacting fundamental and applied physics research. We show that even for ion beams possessing a relatively large energy spread, high-resolution hyperfine-structure measurements can be achieved by correcting the observed line shapes with the time-of-flight information of the resonantly ionized ions. This approach offers exceptional advantages for performing precision measurements on beams with large energy spreads and allows measurements of atomic parameters of previously inaccessible electronic states. The potential of this experimental method in multidisciplinary research is illustrated by performing, for the first time, hyperfine-structure measurements of selected states in the naturally occurring isotopes of indium, ^113,115In. Ab initio atomic-physics calculations have been performed to highlight the importance of our findings in the development of state-of-the-art atomic many-body methods, nuclear structure, and fundamental-physics studies.