Trilobites and other molecular animals: How Rydberg-electrons catch ground state atoms

Donald W. Booth, Jonathan Tallant, Patrick Zabawa +2 more

Max Althön, Markus Exner, R. BLATTNER +1 more

In trilobite Rydberg molecules, an atom in the ground state is bound by electron-atom scattering to a Rydberg electron that is in a superposition of high angular momentum states. This results in a homonuclear molecule with a permanent electric dipole moment in the kilo-debye range. Trilobite molecules have previously been observed only with admixtures of low-l states. Here we report on the observation of two vibrational series of pure trilobite Rubidium-Rydberg molecules that are nearly equidistant. They are produced by three-photon photoassociation and lie energetically more than 15 GHz below the atomic 22F state of rubidium. We show that these states can be used to measure the electron-atom scattering length at low energies in order to benchmark current theoretical calculations. In addition to measuring their kilo-Debye dipole moments, we also show that the molecular lifetime is increased compared to the 22F state due to the high-l character. The observation of an equidistant series of vibrational states opens the way to observe coherent molecular wave packet dynamics.

K. S. Kleinbach, Florian Meinert, F. Engel +4 more

We report on a novel method for the photoassociation of strongly polar trilobite Rydberg molecules. This exotic ultralong-range dimer, consisting of a ground-state atom bound to the Rydberg electron via electron-neutral scattering, inherits its polar character from the admixture of high-angular-momentum electronic orbitals. The absence of low-L character hinders standard photoassociation techniques. Here, we show that for suitable principal quantum numbers the resonant coupling of the orbital motion with the nuclear spin of the perturber, mediated by electron-neutral scattering, hybridizes the trilobite molecular potential with the more conventional S-type molecular state. This provides a general path to associate trilobite molecules with large electric dipole moments, as demonstrated via high-resolution spectroscopy. We find a dipole moment of 135(45) D for the trilobite state. Our results are compared to theoretical predictions based on a Fermi model.

Perttu Luukko, Jan Michael Rost

Frederic Hummel, Kevin Keiler, Peter Schmelcher

We investigate the quantum dynamics of ultra-long-range trilobite molecules exposed to homogeneous electric fields. A trilobite molecule consists of a Rydberg atom and a ground-state atom, which is trapped at large internuclear distances in an oscillatory potential due to scattering of the Rydberg electron off the ground-state atom. Within the Born-Oppenheimer approximation, we derive an analytic expression for the two-dimensional adiabatic electronic potential energy surface in weak electric fields valid up to 500 V/m. This is used to unravel the molecular quantum dynamics employing the multiconfigurational time-dependent Hartree method. Quenches of the electric field are performed to trigger the wave-packet dynamics including the case of field inversion. Depending on the initial wave packet, we observe radial intrawell and interwell oscillations as well as angular oscillations and rotations of the respective one-body probability densities. Opportunities to control the molecular configuration are identified, a specific example being the possibility to superimpose different molecular bond lengths by a series of periodic quenches of the electric field.

L. Suess, R. Parthasarathy, S. B. Hill +2 more