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DETECTION OF "TRILOBITE" AND "BUTTERFLY" RYDBERG MOLECULES IN CESIUM WITH KILODEBYE DIPOLE MOMENTS

Donald W. Booth

Published Apr 6, 2015• 0 citations
OpenAlex

Abstract

The detection and characterization of two classes of ultralong-range Rydberg molecules known as "trilobite" and "butterfly" molecules is presented. These molecules are a subset of a class of Rydberg molecules which asymptotically consist of a Rydberg atom and a ground state atom. The trilobite and butterfly molecules have giant, body-fixed permanent dipole moments on the order of 1000 Debye. The two classes of molecules are distinguished by the relative dominance of the s-wave and p-wave electron scattering. Spectra for (nS_1/2 + 6S_1/2) ^3 Sigma molecules, where n = 37, 39 and 40 and measurements of the Stark broadenings of selected trilobite states in Cs due to the application of a constant external electric field are presented. Additionally, measurements of spectra and Stark splittings for p-wave dominated (nS_1/2 + 6S_1/2) ^3 Pi molecules, where n = 31 and 32 are presented. Computational work on Rydberg pair interactions is also discussed.

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The detection and characterization of two classes of ultralong-range Rydberg molecules known as "trilobite" and "butterfly" molecules is presented. These molecules are a subset of a class of Rydberg molecules which asymptotically consist of a Rydberg atom and a ground state atom. The trilobite and butterfly molecules have giant, body-fixed permanent dipole moments on the order of 1000 Debye. The two classes of molecules are distinguished by the relative dominance of the s-wave and p-wave electron scattering. Spectra for (nS_1/2 + 6S_1/2) ^3 Sigma molecules, where n = 37, 39 and 40 and measurements of the Stark broadenings of selected trilobite states in Cs due to the application of a constant external electric field are presented. Additionally, measurements of spectra and Stark splittings for p-wave dominated (nS_1/2 + 6S_1/2) ^3 Pi molecules, where n = 31 and 32 are presented. Computational work on Rydberg pair interactions is also discussed.
Permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions, and realization of strongly correlated many-body quantum systems. However, large molecular permanent electric dipole moments are challenging to realize experimentally. We report the observation of ultralong-range Rydberg molecules with bond lengths of ~100 nanometers and kilo-Debye permanent electric dipole moments that form when an ultracold ground-state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit. The electronic character of this hybrid class of "trilobite" molecules is dominated by degenerate Rydberg manifolds, making them difficult to produce by conventional photoassociation. We used detailed coupled-channel calculations to reproduce their properties quantitatively. Our findings may lead to progress in ultracold chemistry and strongly correlated many-body physics.
The ultralong-range Cs2 Rydberg molecules consisting of a Rydberg, nD5/2 ( principal quantum number n =35-38), and a ground state atom, 6S1/2 (F=4) are prepared by a two-photon photoassociation spectroscopy in an ultracold Cs gas. This kind of molecule is bound with the low energy scattering and has a permanent dipole moment. We observe two Rydberg-ground state molecular spectra, one is deep-bound molecule, TΣ state, bound by triplet s-wave scattering length and the other one is shallow-bound molecule, S,TΣ state, bound by mixed singlet-triplet s-wave scattering length. The binding energy of Rydberg-ground molecules are attained by analyzing the two photon photoassociation spectrum, corresponding permanent dipole moment is measured by applying an external electric field, which is compared to the calculation.
Ultra-cold long-range Rydberg-ground molecule consisting of a Rydberg atom and one or more ground-state atoms is formed by low-energy scattering between the Rydberg electron and ground-state atoms located inside the Rydberg electron’s wave function. The low-energy scattering interaction, initially investigated by Fermi and Omont, has been predicted to lead to molecular binding in a novel type of Rydberg molecules, including the trilobite and butterfly molecules. Their unconventional binding mechanism, which is unlike covalent, or ionic, or van der Waals bonds, results in loosely bound molecules with bond lengths on the order of thousands of Bohr radius. This kind of molecule with large size and huge permanent electric dipole moment is a good candidate for realizing the certain strongly correlated many-body gases and for quantum information processing, as well as for dipolar quantum gases and spin systems with long-range interactions. Consequently, these molecules have received considerable attention in recent years. In this paper, we review the recent theoretical and experimental investigations of ultra-cold long-range Rydberg-ground molecules, including the scattering interaction between the Rydberg electron and ground-state atom and the resulting adiabatic potential curves, experimental observations of photo-associated Rydberg-ground molecules spectra, as well as the measurements of permanent electric dipole moment. Ultra-cold long-range Rydberg-ground molecules are prepared by photoassociation in a high-density cold atom sample. Therefore, the Rydberg electron can bind several ground-state atoms to form a polyatomic Rydberg-ground molecule. The permanent molecular electric-dipole moments are revealed by spectral line broadening in the electric fields. The latest research pointed out that the permanent electric dipole moments of the Cs nDJ -type Rydberg-ground molecules are negative, which is different from the previous reports (the electric dipole moments are positive). The negative sign reflects a deficiency of Rydberg-electron density near the ground-state perturber, which is caused by electronic configuration mixing.
The authors investigate long-range Cs2{}_{2}2​ molecules consisting of a ground-state and a Rydberg atom, and measure and calculate permanent molecular electric-dipole moments showing that the sign of the dipole moment is negative, reflecting a deficiency of Rydberg-electron density near the ground-state constituent
Cold and ultracold Rydberg atoms are in considerable vogue for their ability to creating strong interactions, stemming from their exaggerated and readily tunable properties. Ultralong-range Rydberg molecules have been predicted to form from the interaction of ultracold Rydberg atoms with ground-state atoms and polar molecules. In this work, we discuss and demonstrate how such molecules, which are homonuclear, form substantially large permanent electric dipole moments. A corollary benefit of such strong hybridisation is the realisation of high angular momentum degenerate Rydberg molecules (so-called trilobite molecules) with standard photoassociation techniques.
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.