Spin-orbit-dependent lifetimes of long-range Rydberg molecules
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arXiv
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2026
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| author | Peper, Michael Skrotzki, Jakob Trautmann, Martin Sivakumar, Ajith Sanjai C. V. Deiglmayr, Johannes |
| author_facet | Peper, Michael Skrotzki, Jakob Trautmann, Martin Sivakumar, Ajith Sanjai C. V. Deiglmayr, Johannes |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_01871 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Spin-orbit-dependent lifetimes of long-range Rydberg molecules Peper, Michael Skrotzki, Jakob Trautmann, Martin Sivakumar, Ajith Sanjai C. V. Deiglmayr, Johannes Atomic Physics Quantum Physics 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. |
| title | Spin-orbit-dependent lifetimes of long-range Rydberg molecules |
| topic | Atomic Physics Quantum Physics |
| url | https://arxiv.org/abs/2602.01871 |