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We propose and experimentally investigate a scheme for narrow-line cooling of KRb molecules in the rovibrational ground state. We show that the spin-forbidden transition of KRb is ideal for realizing narrow-line laser cooling of molecules because it has highly diagonal Franck-Condon factors and narrow linewidth. In order to confirm the prediction, we performed the optical and microwave spectroscopy of ultracold KRb molecules, and determined the linewidth ( 4.9(4) kHz) and Franck-Condon factors for the transition (0.9474(1)). This result opens the door towards all-optical production of polar molecules at sub-microkelvin temperatures.

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