Ultracold molecules, because of their rich internal structures and interactions, have been proposed as a promising platform for quantum science and precision measurement. Direct laser-cooling promises to be a rapid and efficient way to bring molecules to ultracold temperatures. For trapped molecules, laser-cooling to the quantum motional ground state remains an outstanding challenge. A technique capable of reaching the motional ground state is Raman sideband cooling, first demonstrated in trapped ions and atoms. In this work, we demonstrate for the first time Raman sideband cooling of molecules. Specifically, we demonstrate 3D Raman cooling for single CaF molecules trapped in an optical tweezer array, achieving average radial (axial) motional occupation as low as $\bar{n}_r=0.27(7)$ ($\bar{n}_z=7.0(10)$). Notably, we measure a 1D ground state fraction as high as 0.79(4), and a motional entropy per particle of $s = 4.9(3)$, the lowest reported for laser-cooled molecules to date. These lower temperatures could enable longer coherence times and higher fidelity molecular qubit gates desirable for quantum information processing and quantum simulation. With further improvements, Raman cooling could also be a new route towards molecular quantum degeneracy applicable to many laser-coolable molecular species including polyatomic ones. 

The dataset comprises quantities extracted experimentally from binarized molecular fluorescence images. The binarization procedure and the relevant numerical simulation procedures are described in the methods and supplementary material. Full binarized datasets are available upon request. These binarized datasets do not contain additional information than the provided data files.

All data is provided as csv files. No proprietary software is required.