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Molecules

Rydberg-State Double-Well Potentials of Van der Waals Molecules

Tomasz Urbańczyk, Andrzej Kędziorski, Marek Krośnicki, J. Koperski

Published Sep 30, 2024• 2 citations
Publisher

Abstract

Recent progress in studies of Rydberg double-well electronic energy states of MeNg (Me = 12-group atom, Ng = noble gas atom) van der Waals (vdW) molecules is presented and analysed. The presentation covers approaches in experimental studies as well as ab initio-calculations of potential energy curves (PECs). The analysis is shown in a broader context of Rydberg states of hetero- and homo-diatomic molecules with PECs possessing complex 'exotic' structure. Laser induced fluorescence (LIF) excitation spectra and dispersed emission spectra employed in the spectroscopical characterization of Rydberg states are presented on the background of the diverse spectroscopic methods for their investigations such as laser vaporization-optical resonance (LV-OR), pump-and-probe methods, and polarization labelling spectroscopy. Important and current state-of-the-art applications of Rydberg states with irregular potentials in photoassociation (PA), vibrational and rotational cooling, molecular clocks, frequency standards, and molecular wave-packet interferometry are highlighted.

DOI
10.3390/molecules29194657

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Recent progress in studies of Rydberg double-well electronic energy states of MeNg (Me = 12-group atom, Ng = noble gas atom) van der Waals (vdW) molecules is presented and analysed. The presentation covers approaches in experimental studies as well as ab initio-calculations of potential energy curves (PECs). The analysis is shown in a broader context of Rydberg states of hetero- and homo-diatomic molecules with PECs possessing complex 'exotic' structure. Laser induced fluorescence (LIF) excitation spectra and dispersed emission spectra employed in the spectroscopical characterization of Rydberg states are presented on the background of the diverse spectroscopic methods for their investigations such as laser vaporization-optical resonance (LV-OR), pump-and-probe methods, and polarization labelling spectroscopy. Important and current state-of-the-art applications of Rydberg states with irregular potentials in photoassociation (PA), vibrational and rotational cooling, molecular clocks, frequency standards, and molecular wave-packet interferometry are highlighted.
The energy level spectrum of a many-body system containing two shared, collective Rydberg excitations is measured using cold atoms in an optical dipole trap. Two pairs of independently tunable laser pulses are employed to spectroscopically probe the spectrum in a double-resonance excitation scheme. Depending on the magnitude of an applied electric field, the Rydberg-atom interactions can vary from resonant dipole-dipole to attractive or repulsive van der Waals, leading to characteristic signatures in the measured spectra. Our results agree with theoretical estimates of the magnitude and sign of the interactions.
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Vibrational properties of ultralong Rydberg Cs2_22​ molecules are investigated on corresponding potential curves obtained by perturbation theory. The Rydberg Cs2_22​ molecules are associated by a Rydberg Cs(nS/nPnS/nPnS/nP) atom (n=30−70)(n=30-70)(n=30−70) and a ground state Cs(6s6s6s) atom. The starting point for the perturbation treatment of corresponding Rydberg molecular potential curves is to generate accurate atomic Rydberg states from realistic {\it ab initio} effective core potential. The calculated results have similar characteristics with available experimental and theoretical investigations on Rydberg Rb2_22​ molecules. And this is the first time that Rydberg molecules are studied at the {\it ab initio} level.
We present a detailed analysis of our recent observation of synchronous Rabi oscillations between the electronic ground state and Rydberg states in a mesoscopic ensemble containing roughly 100 ultracold atoms (Reetz-Lamour et al submitted, Preprint 0711.4321). The mesoscopic cloud is selected out of a sample of laser-cooled Rb atoms by optical pumping. The atoms are coupled to a Rydberg state with principal quantum number around 30 by a two-photon scheme employing flat-top laser beams. The influence of residual spatial intensity fluctuations as well as sources of decoherence such as redistribution to other states, radiative lifetime and laser bandwidth are analysed. The results open up new possibilities for the investigation of coherent many-body phenomena in dipolar Rydberg gases. As an example we demonstrate the van der Waals blockade, a variant of the dipole blockade, for a mesoscopic atom sample.
We present a detailed analysis of our recent observation of synchronous Rabi oscillations between the electronic ground state and Rydberg states in a mesoscopic ensemble containing roughly 100 ultracold atoms (Reetz-Lamour et al submitted, Preprint 0711.4321). The mesoscopic cloud is selected out of a sample of laser-cooled Rb atoms by optical pumping. The atoms are coupled to a Rydberg state with principal quantum number around 30 by a two-photon scheme employing flat-top laser beams. The influence of residual spatial intensity fluctuations as well as sources of decoherence such as redistribution to other states, radiative lifetime and laser bandwidth are analysed. The results open up new possibilities for the investigation of coherent many-body phenomena in dipolar Rydberg gases. As an example we demonstrate the van der Waals blockade, a variant of the dipole blockade, for a mesoscopic atom sample.
In this dissertation I investigate cold Rydberg atoms and molecules in which the angular-momentum character of the quantum states involved strongly influences their properties and dynamics. In the first part I focus on long-range diatomic Rydberg molecules formed by a rubidium D-state Rydberg atom and a second rubidium atom in its ground state. Spectroscopic measurements of molecular binding energies are presented showing the effect of the Rydberg atom size and fine-structure coupling on the molecular potentials. A theoretical model is introduced that takes into account all relevant angular-momentum couplings between the molecular constituents, successfully reproducing experimental observations. Calculations of adiabatic potentials and binding energies, molecular-state lifetimes, electric and magnetic dipole moments are also presented. In the second part, I describe the production and magnetic trapping of cold circular Rydberg atoms. The circular Rydberg atoms are generated out of a cold gas of rubidium using the crossed-fields method and magnetically trapped. The trapping force is employed to induce center-of-mass oscillations of the trapped atom sample. Trap parameters and observed oscillation frequencies are used to measure the magnetic moments of the circular Rydberg atoms. Trap losses and the atomic internal-state evolution in the 300 Kelvin thermal background are also investigated.