Photoassociation of Trilobite Rydberg Molecules via Resonant Spin-Orbit Coupling

Area of Science:

• Quantum Chemistry
• Atomic Physics
• Molecular Spectroscopy

Background:

• Trilobite Rydberg molecules are exotic ultralong-range dimers formed by a ground-state atom and a Rydberg electron.
• Their polar character, derived from high-angular-momentum electronic orbitals, complicates standard photoassociation.
• The lack of low-L character in these states hinders conventional association methods.

Purpose of the Study:

• To develop a novel photoassociation technique for strongly polar trilobite Rydberg molecules.
• To overcome the limitations of standard methods in creating these exotic molecular states.
• To demonstrate a general pathway for associating trilobite molecules with large electric dipole moments.

Main Methods:

• Utilizing resonant coupling between orbital motion and nuclear spin of the perturber.
• Mediating this coupling via electron-neutral scattering.
• Employing high-resolution spectroscopy to characterize the associated molecules.

Main Results:

• A novel photoassociation method for trilobite Rydberg molecules was successfully demonstrated.
• The resonant coupling hybridizes trilobite molecular potentials with S-type molecular states.
• A significant electric dipole moment of 135(45) D was measured for the trilobite state.

Conclusions:

• The developed method provides a general pathway for creating trilobite molecules with large electric dipole moments.
• This work overcomes previous challenges in photoassociating these exotic molecular systems.
• Results are consistent with theoretical predictions from a Fermi model.