Spin-orbit-dependent lifetimes of long-range Rydberg molecules

• URL: http://arxiv.org/abs/2602.01871v1
• Date: Mon, 02 Feb 2026 09:44:04 GMT
• Title: Spin-orbit-dependent lifetimes of long-range Rydberg molecules
• Authors: Michael Peper, Jakob Skrotzki, Martin Trautmann, Ajith Sanjai C. V. Sivakumar, Johannes Deiglmayr,
• Abstract summary: Long-range Rydberg molecules form when a highly excited Rydberg electron scatters from ground-state atoms inside its orbit.<n>We present a combined theoretical and experimental study of caesium dimers correlated to 402P3/2 Rydberg states.
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• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Long-range Rydberg molecules (LRMs) form when a highly excited Rydberg electron scatters from ground-state atoms inside its orbit, creating oscillatory, long-range potentials. We present a combined theoretical and experimental study of caesium dimers correlated to 402P3/2 Rydberg states, with an emphasis on decay via autoionisation (associative ionisation). Our model includes a relativistic treatment of electron-atom scattering with spin-orbit coupling, the perturber's hyperfine structure, and coupling of vibrational levels to a continuum of short-range decay channels. Calculated potential-energy curves predict two families of wells: outer wells near the classical outer turning point supporting long-lived states, and inner wells at shorter range whose lifetimes are limited by tunneling and subsequent vibronic decay. Using photoassociation in an ultracold Cs gas and an analysis of pulsed-field-ionisation signals which are highly selective for the detection of molecules, we assign resonances by binding energy and measure lifetimes. The measured lifetimes of inner-well states increase systematically with increasing detuning and agree with calculated lifetimes; detection of Cs2+ product ions supports autoionisation as a dominant channel. We show that the lifetimes are strongly reduced by spin-orbit interactions in the transient Cs-collision complex, which lift the near-degeneracy in Omega observed for states in the outer well and control the inner-well binding. The identified states also provide promising pathways to create ultracold molecules in ion-pair states.

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