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

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