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We show that quantum interference-based coherent control is a highly efficient tool for tuning ultracold molecular collision dynamics, and is free from the limitations of commonly used methods that rely on external electromagnetic fields. By varying {the relative populations and} phases of an initial coherent superpositions of degenerate molecular states, we demonstrate complete coherent control over integral scattering cross sections in the ultracold $s$-wave regime of both the initial and final collision channels. The proposed control methodology is applied to ultracold O$_2$~+~O$_2$ collisions, showing extensive control over $s$-wave spin-exchange cross sections and product branching ratios over many orders of magnitude.
Quantum control of reactive systems has enabled microscopic probes of underlying interaction potentials, the opening of novel reaction pathways, and the alteration of reaction rates using quantum statistics. However, extending such control to the qua
Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic chemical reaction at ultracold temperatures allows its qu
Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could a
We consider losses in collisions of ultracold molecules described by a simple statistical short-range model that explicitly accounts for the limited lifetime of classically chaotic collision complexes. This confirms that thermally sampling many isola
We demonstrate the ability to coherently control ultracold atomic Rb collisions using frequency-chirped light on the nanosecond time scale. For certain center frequencies of the chirp, the rate of inelastic trap-loss collisions induced by negatively