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arXiv:1607.01325 · Journal of Physics B Atomic Molecular and Optical Physics

Controlling Rydberg atom excitations in dense background gases

Tara Cubel Liebisch, Michael Schlagmüller, Felix Engel, Huan Nguyen, Jonathan Balewski, G. Lochead, Fabian Böttcher, Karl M Westphal, Kathrin S Kleinbach, Thomas Schmid, Anita Gaj, Robert Löw, Sebastian Hofferberth, Tilman Pfau, Jesús Pérez‐Ríos, Chris H. Greene

Published Aug 23, 2016• 30 citations
arXivHTMLPDF

Abstract

Abstract We discuss the density shift and broadening of Rydberg spectra measured in cold, dense atom clouds in the context of Rydberg atom spectroscopy done at room temperature, dating back to the experiments of Amaldi and Segrè in 1934. We discuss the theory first developed in 1934 by Fermi to model the mean-field density shift and subsequent developments of the theoretical understanding since then. In particular, we present a model whereby the density shift is calculated using a microscopic model in which the configurations of the perturber atoms within the Rydberg orbit are considered. We present spectroscopic measurements of a Rydberg atom, taken in a Bose–Einstein condensate and thermal clouds with densities varying from 5 × 10 14 to 9 × 10 12 cm −3 . The density shift measured via the spectrum’s center of gravity is compared with the mean-field energy shift expected for the effective atom cloud density determined via a time of flight image. Lastly, we present calculations and data demonstrating the ability of localizing the Rydberg excitation via the density shift within a particular density shell for high principal quantum numbers.

DOI
10.1088/0953-4075/49/18/182001

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•Aug 7, 2017•1 citation
Abstract We discuss the density shift and broadening of Rydberg spectra measured in cold, dense atom clouds in the context of Rydberg atom spectroscopy done at room temperature, dating back to the experiments of Amaldi and Segrè in 1934. We discuss the theory first developed in 1934 by Fermi to model the mean-field density shift and subsequent developments of the theoretical understanding since then. In particular, we present a model whereby the density shift is calculated using a microscopic model in which the configurations of the perturber atoms within the Rydberg orbit are considered. We present spectroscopic measurements of a Rydberg atom, taken in a Bose–Einstein condensate and thermal clouds with densities varying from 5 × 10 14 to 9 × 10 12 cm −3 . The density shift measured via the spectrum’s center of gravity is compared with the mean-field energy shift expected for the effective atom cloud density determined via a time of flight image. Lastly, we present calculations and data demonstrating the ability of localizing the Rydberg excitation via the density shift within a particular density shell for high principal quantum numbers.
We present a novel spectroscopic method for probing the \insitu~density of quantum gases. We exploit the density-dependent energy shift of highly excited {Rydberg} states, which is of the order 101010\MHz\,/\,1E14\,cm-3^{\text{-3}}-3 for \rubidium~for triplet s-wave scattering. The energy shift combined with a density gradient can be used to localize Rydberg atoms in density shells with a spatial resolution less than optical wavelengths, as demonstrated by scanning the excitation laser spatially across the density distribution. We use this Rydberg spectroscopy to measure the mean density addressed by the Rydberg excitation lasers, and to monitor the phase transition from a thermal gas to a Bose-Einstein condensate (BEC).
We present spectroscopy of a single Rydberg atom excited within a Bose-Einstein condensate. We not only observe the density shift as discovered by Amaldi and Segrè in 1934, but a line shape that changes with the principal quantum number n. The line broadening depends precisely on the interaction potential energy curves of the Rydberg electron with the neutral atom perturbers. In particular, we show the relevance of the triplet p-wave shape resonance in the e^{-}-Rb(5S) scattering, which significantly modifies the interaction potential. With a peak density of 5.5×10^{14} cm^{-3}, and therefore an interparticle spacing of 1300 a_{0} within a Bose-Einstein condensate, the potential energy curves can be probed at these Rydberg ion-neutral atom separations. We present a simple microscopic model for the spectroscopic line shape by treating the atoms overlapped with the Rydberg orbit as zero-velocity, uncorrelated, pointlike particles, with binding energies associated with their ion-neutral separation, and good agreement is found.
In recent years, Rydberg excitations in atomic quantum gases have become a successful platform to explore quantum impurity problems. A single impurity immersed in a Fermi gas leads to the formation of a polaron, a quasiparticle consisting of the impurity being dressed by the surrounding medium. With a radius of about the Fermi wavelength, the density profile of a polaron cannot be explored using in situ optical imaging techniques. In this Letter, we propose a new experimental measurement technique that enables the in situ imaging of the polaron cloud in ultracold quantum gases. The impurity atom induces the formation of a polaron cloud and is then excited to a Rydberg state. Because of the mesoscopic interaction range of Rydberg excitations, which can be tuned by the principal numbers of the Rydberg state, atoms extracted from the polaron cloud form dimers with the impurity. By performing first principle calculations of the absorption spectrum based on a functional determinant approach, we show how the occupation of the dimer state can be directly observed in spectroscopy experiments and can be mapped onto the density profile of the gas particles, hence providing a direct, real-time, and in situ measure of the polaron cloud.
A single Rydberg atom impurity excited in a BEC is a system that can be utilized to measure the quantum mechanical properties of electron - neutral scattering andthe electron probability density of a Rydberg atom. The Rydberg electron – neutral atom scattering process, is a fundamental scattering process, which can be described via Fermi’s pseudopotential as V{vec{r},vec{R} )=2pi textit{a}[k(R)]delta^{(3)}(vec{r}-vec{R}). The scattering length is dependent on the momentum of the Rydberg electron, and therefore is dependent on the separation of the Rydberg electron from the ion core. At the classical outermost turning point of the electron, it has the slowest momentum leading to s-wave dominated scattering potentials 10’s of MHz in depth for n<40 (Greene et al. PRL 85 2458 (2000), Bendkowsky et al. PRL 105 163201 (2010)). In alkali atoms there is a shape resonance for p-wave scattering, which becomes relevant at ion-neutral separations of ~75nm (I.I. Fabrikant J.Phys B 19, 1527 (1985)). This shape resonance potential is several GHz deep, spanning the energy level spacing between n and n-1 principal quantum numbers. At high BEC densities of 5x10^14cm-3 the nearest neighbor spacing is less than 70nm. A Rydberg atom excited within a BEC, is an excitation of the Rydberg atom and all N neutral atoms located within the Rydberg orbit, described as nS+N x 5S. The nS+N x 5S state is density shifted from the Rydberg resonance. Not only does the distribution of atoms within the Rydberg orbit lead to a density shift, but, at these high densities, atoms excited in the nS+N x 5S state near the shape resonance potential cause large perturbations to the density shift, leading to a line broadening. Therefore the spectroscopic line shape of a Rydberg atom in a BEC allows us to probe the theoretically calculated p-wave shape resonance potential. Furthermore, we can observe and measure the dynamics of neutrals excited in the nS+N x 5S state. In the ultracold regime of a BEC, the background neutral atoms within the Rydberg orbit have kinetic energies of a few kHz, and experience large forces due to the GHz-deep shape resonance potentials. An atom dragged into this deep potential leads to an exothermic state-changing collision. We measure the timescale of this state-changing collision and compare to semi-classical calculations of the neutral atoms evolving in the potential of the two-particle nS+ 5S system. We also measure the change in energy from the original nS state to the product state, (n-4)L (L<3). On time scales shorter than the state-changing collisions, which for n<100 is on the order of 10 microseconds, the neutral atoms will evolve and collect in the shallower electron-neutral potentials, which mimic the electron probability density of the Rydberg atom.With n<100, the Rydberg atom has a diameter greater than 2 micrometers. With an imaging system with <1 micrometer resolution, we expect to observe a macroscopic change in the density profile of the BEC indicating an nS versus nD Rydberg state. The BEC would serve as a contrast agent for observing textbook atomic wavefunctions (Karpiuk et al. New Journal of Physics 17, 053046 (2015)).
Rydberg-Rydberg collisions in a cold, dense Rydberg gas can lead to the conversion of internal energy into center-of-mass energy of the colliding atoms, resulting in Rydberg-atom velocities much larger than the initial velocities in the gas. We prepare cold Rydberg-atom gases by laser excitation of laser-cooled atom clouds and use time-of-flight measurements to demonstrate the production of fast Rydberg atoms. The velocity distributions of Rydberg atoms emerging from the Rydberg-atom gases are obtained. State-selective field ionization spectra indicate a correlation between the production of fast Rydberg atoms and the presence of Penning ionization signatures. The dependence of the yield of fast Rydberg atoms on Rydberg atom density is measured.
In this work I describe the excitation spectra of Rydberg atoms in ultracold gases of strontium and their decay mechanisms. In a few-body regime, we observe a highly structured spectrum re ecting excitation of ultralong-range molecules consisting of one or more ground-state atoms bound to the Rydberg core in potential wells formed by the Rydbergelectron wave function. In a many-body regime, with hundreds of ground-state atoms within the Rydberg orbital, the Rydberg atoms can be viewed as an impurity in a quantum gas, connecting to important concepts in condensed matter physics. The spectrum for impurity excitation displays signatures of polaronic states, in which the Rydberg atom signi cantly perturbs the density of the background gas. Additionally, decay channels of Rydberg excitations are examined by monitoring the time evolution of Rydberg populations. The measured lifetimes reveal new information on the decay processes of Rydberg molecules and place limits on the time scales over which studies involving Rydberg species in cold, dense atomic gases can be undertaken and limit the coherence times for such measurements.