Hyperfine Structure of the B³Pi₁ State and Predictions of Optical Cycling Behavior in the Xrightarrow B transition of TlF

The rotational and hyperfine spectrum of the $X^1\Sigma^+ \rightarrow B^3\Pi_1$ transition in TlF molecules was measured using laser-induced fluorescence from both a thermal and a cryogenic molecular beam. Rotational and hyperfine constants for the $B$ state are obtained. The large magnetic hyperfine interaction of the Tl nuclear spin leads to significant mixing of the lowest $B$ state rotational levels. Updated, more precise measurements of the $B\rightarrow X$ vibrational branching fractions are also presented. The combined rovibrational branching fractions allow for the prediction of the number of photons that can be scattered in a given TlF optical cycling scheme.