Collinear laser spectroscopy experiments were performed to determine the magnetic dipole and electric quadrupole hyperfine coupling constants for multiple atomic transitions of aluminum. The magnetic dipole coupling constants of the $3p{}^2{P}_{1/2}$, $3p{}^2{P}_{3/2}$, and $4s{}^2{S}_{1/2}$ atomic states were remeasured. Relativistic coupled-cluster calculations including single, double, and triple excitations reproduce the experimental results well and are consistent with previous literature values. In contrast, the electric quadrupole coupling constant of the $3p{}^2{P}_{3/2}$ state exhibits large scatter among existing data, with the theoretical results in agreement with our new measurements. The magnetic dipole and electric quadrupole coupling constants of the $5s{}^2{S}_{1/2}$ state, as well as of the strongly mixed $ndy{}^2{D}_{3/2}$ and $ndy{}^2{D}_{5/2}$ states, were determined here for the first time. The theoretical calculations presented in this work reproduce these experimental results well. Our results provide valuable guidance for future experiments seeking to extract nuclear-structure information from hyperfine-structure measurements of exotic aluminum isotopes. They also demonstrate that atomic-structure calculations can accurately account for mixing effects, enabling the use of these mixed atomic states to extract reliable nuclear properties from hyperfine-structure measurements.

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• Atomic & molecular structure
• Electronic excitation & ionization
• Electronic structure of atoms & molecules
• Fine & hyperfine structure
• Laser spectroscopy