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

Fuente: arXiv
Gespeichert in:
Bibliographische Detailangaben
Hauptverfasser: Peper, Michael, Skrotzki, Jakob, Trautmann, Martin, Sivakumar, Ajith Sanjai C. V., Deiglmayr, Johannes
Format: Preprint
Veröffentlicht: 2026
Schlagworte:
Online-Zugang:
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
_version_ 1866912868320935936
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