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Bulletin of the American Physical Society

Direct excitation of butterfly states in Rydberg molecules

Carsten Lippe, Thomas Niederprüm, Olivier Thomas, Tanita Eichert, Herwig Ott

Published May 27, 2016• 0 citations
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Bulletin of the American Physical Society•Jun 7, 2012•0 citations
We report on the observation of highly excited ( ν ∼ 100 ) vibrational states of a trilobite ultralong-range Rydberg molecule in Rb 87 . These states manifest spectroscopically in a regularly spaced series of peaks red-detuned from the 25 f 7 / 2 dissociation threshold. The existence and observed stability of these states require the almost complete suppression of the adiabatic decay pathway induced by the P -wave shape resonance of Rb. This stabilization is predicted to occur only for certain Rydberg levels where the avoided crossing between trilobite and P -wave-dominated butterfly potential energy curves nearly vanishes, allowing the vibrational states to diabatically traverse the crossing with almost unit probability. This is the first direct measurement of beyond-Born-Oppenheimer physics in long-range Rydberg molecules, and paves the way for future experiments to access and manipulate wave packets formed from high-lying vibrational states.
Ultralong-range Rydberg molecules provide an exciting testbed for molecular physics at exaggerated scales. In the so-called trilobite and butterfly Rydberg molecules, the Born-Oppenheimer approximation can fail due to strong nonadiabatic couplings arising from the combination of radial oscillations and rapid energy variations in the adiabatic potential energy curves. We utilize an accurate coupled-channel treatment of the vibronic system to observe the breakdown of Born-Oppenheimer physics, such as nonadiabatic trapping and decay of molecular states found near pronounced avoided crossings in the adiabatic potential curves. Even for vibrational states localized far away from avoided crossings, a single-channel model is quantitatively sufficient only after including the diagonal nonadiabatic corrections to the Born-Oppenheimer potentials. Our results indicate the importance of including nonadiabatic physics in the description of ultralong-range Rydberg molecules and in the interpretation of measured vibronic spectra.
Recent experiments in our group on the excitation of Rydberg molecules in ultracold quantum gases have been reviewed. Quantum gases are a well‐suited environment to excite Rydberg molecules, due to the high atomic density and the perfect control of the internal spin degrees of freedom and the center of mass motion of the atoms. In parallel, the coupling to Rydberg molecules can be used to probe and manipulate the interaction in ultracold quantum gases. In this Feature Article, a comprehensive introduction to the field of Rydberg molecules, including ultralong‐range molecules and butterfly molecules is given. The Rydberg molecules have been characterized spectroscopically and their internal spin structure is discussed. Then, it is shown how these Rydberg molecules work as a tool to monitor the double occupancy in optical lattice experiments and to change the inter‐particle interaction with the help of a so‐called optical Feshbach resonance.