STIRAP preparation of a coherent superposition of ThO $H^3\Delta_1$ states for an improved electron EDM measurement

Abstract

Experimental searches for the electron electric dipole moment (EDM) probe new physics beyond the Standard Model. The current best EDM limit was set by the ACME Collaboration [Science \textbf{343}, 269 (2014)], constraining time reversal symmetry ($T$) violating physics at the TeV energy scale. ACME used optical pumping to prepare a coherent superposition of ThO $H^3\Delta_1$ states that have aligned electron spins. Spin precession due to the molecule's internal electric field was measured to extract the EDM. We report here on an improved method for preparing this spin-aligned state of the electron by using STIRAP. We demonstrate a transfer efficiency of $75\pm5\%$, representing a significant gain in signal for a next generation EDM experiment. We discuss the particularities of implementing STIRAP in systems such as ours, where molecular ensembles with large phase-space distributions are transfered via weak molecular transitions with limited laser power and limited optical access.