Engineered Molecular Clock Transitions for Symmetry Violation Searches

Abstract: Heavy polar molecules are sensitive probes of physics Beyond the Standard Model. However, uncontrolled external electromagnetic fields pose challenges to achieving precise and accurate measurements. Minimizing susceptibility to these fields is therefore critical and has played an important role in all precision experiments of this type. Here we devise and demonstrate clock transitions engineered to realize robust symmetry violation searches in the polyatomic molecule YbOH. Sensitivities to external fields can be suppressed by orders-of-magnitude while preserving high sensitivity to the electron electric dipole moment (eEDM). We perform Ramsey measurements on these clock transitions and observe suppression of electric and magnetic sensitivities by at least a factor of 700 and 200, respectively, and demonstrate the robustness of their spin coherence against large electromagnetic field fluctuations. We further identify and employ selected quantum states to make sensitive measurements of external magnetic and electric fields, another critical feature for highly accurate measurements. This approach of molecular engineering is broadly applicable to diverse molecular species and states, including those with complex nuclei and those that are compatible with state-of-the-art cooling and trapping techniques, thereby offering the potential to significantly improve experimental sensitivity to a wide range of New Physics while expanding the chemical design space for molecular quantum science.