Coherent Optical Creation of a Single Molecule Yu, Yichao González Férez, María Rosario We thank Bo Gao and Paul Julienne for discussion and Robert Moszynski for providing theoretical transition dipole moments of NaCs. This work is supported by the NSF (PHY-1806595), the AFOSR (FA9550-19-1-0089), ARO DURIP (W911NF1810194), and the Arnold and Mabel Beckman foundation. J. T. Z. is supported by a National Defense Science and Engineering Graduate Fellowship. W. B. C. is supported by a Max PlanckHarvard Research Center for Quantum Optics fellowship. K. W. is supported by an NSF GRFP fellowship. J. M. H. is supported by the UK Engineering and Physical Sciences Research Council (EPSRC) Grants No. EP/N007085/1, No. EP/P008275/1, and No. EP/P01058X/1. R. G.-F. acknowledges financial support of the Spanish Project FIS2017-89349-P (MINECO) and the Andalusian research group FQM-207. We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition. The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering. Starting fromtwo atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%. The molecules have a binding energy of 770.2 MHz at 8.83(2) G. This technique does not rely on Feshbach resonances or narrow excited-state lines and may allow a wide range of molecular species to be assembled atom by atom. 2021-10-28T10:32:08Z 2021-10-28T10:32:08Z 2021-09-17 journal article Yu, Y... [et al.] (2021). Coherent optical creation of a single molecule. Physical Review X, 11(3), 031061. [https://doi.org/10.1103/PhysRevX.11.031061] http://hdl.handle.net/10481/71156 10.1103/PhysRevX.11.031061 eng http://creativecommons.org/licenses/by/3.0/es/ open access Atribución 3.0 España American Physical Society