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Spectral bands for the B(2) X(1) electronic transition in the doubly-polar open-shell KSr molecule are recorded at moderate resolution using the thermoluminescence technique. The spectra are simulated using three kinds of advanced electronic structure calculations, allowing for an assessment of their accuracy on one hand, and for the derivation of fundamental spectroscopic constants of the X(1) KSr ground state and the excited electronic state B(2), on the other hand. These results should facilitate further studies aiming at creating ultracold bosonic or fermionic KSr molecules.

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