Magnetic hyperfine structure constants of ¹³⁷BaF in the ²Π_1/2 and ²Π_3/2 excited states

High-precision molecular experiments testing the Standard Model of particle physics require an accurate understanding of the molecular structure at the hyperfine level, both for the control of the molecules and for the interpretation of the results. In this work, we calculate the hyperfine structure constants for the excited states (Formula Presented) of ¹³⁷BaF due to the ¹³⁷Ba nucleus. We use the four-component relativistic Fock-space coupled-cluster method, extrapolating our results to the complete basis set limit. We investigate the effect of the basis sets and electron correlation, and estimate the uncertainty in our final results. Our results are used in the interpretation of the experimental spectroscopy of the hyperfine and rovibrational spectra of BaF, and the planning of laser-cooling schemes for future parity-violating anapole moment measurements.