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Physical Review Letters

Selective Production of Rydberg-Stark States of Positronium

Thomas E. Wall, A. Alonso, B. S. Cooper, Adam Deller, S. D. Hogan, D. B. Cassidy

Published Apr 28, 2015• 48 citations
Publisher

Abstract

Rydberg positronium (Ps) atoms have been prepared in selected Stark states via two-step (1s→2p→nd/ns) optical excitation. Two methods have been used to achieve Stark-state selection: a field ionization filter that transmits the outermost states with positive Stark shifts, and state-selected photoexcitation in a strong electric field. The former is demonstrated for n=17 and 18 while the latter is performed for n=11 in a homogeneous electric field of 1.9 kV/cm. The observed spectral intensities and their dependence on the polarization of the laser radiation are in agreement with calculations that include the perturbations of the intermediate n=2 manifold. Our results pave the way for the generation of Rydberg Ps atoms with large electric dipole moments that are required for the realization of schemes to control their motion using inhomogeneous electric fields, an essential feature of some proposed Ps free-fall measurements requiring focused beams of long-lived atoms.

DOI
10.1103/physrevlett.114.173001

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Rydberg positronium (Ps) atoms have been prepared in selected Stark states via two-step (1s→2p→nd/ns) optical excitation. Two methods have been used to achieve Stark-state selection: a field ionization filter that transmits the outermost states with positive Stark shifts, and state-selected photoexcitation in a strong electric field. The former is demonstrated for n=17 and 18 while the latter is performed for n=11 in a homogeneous electric field of 1.9 kV/cm. The observed spectral intensities and their dependence on the polarization of the laser radiation are in agreement with calculations that include the perturbations of the intermediate n=2 manifold. Our results pave the way for the generation of Rydberg Ps atoms with large electric dipole moments that are required for the realization of schemes to control their motion using inhomogeneous electric fields, an essential feature of some proposed Ps free-fall measurements requiring focused beams of long-lived atoms.
We report experiments in which positronium (Ps) atoms were guided using inhomogeneous electric fields. Ps atoms in Rydberg-Stark states with principal quantum number n=10 and electric dipole moments up to 610 D were prepared via two-color two-photon optical excitation in the presence of a 670 V cm^{-1} electric field. The Ps atoms were created at the entrance of a 0.4 m long electrostatic quadrupole guide, and were detected at the end of the guide via annihilation gamma radiation. When the lasers were tuned to excite low-field-seeking Stark states, a fivefold increase in the number of atoms reaching the end of the guide was observed, whereas no signal was detected when high-field-seeking states were produced. The data are consistent with the calculated geometrical guide acceptance.
A Surko-type positron trap has been used to produce intense positron pulses, and thus a dilute positronium (Ps) gas in vacuum with an initial density of 10^7 cm-3. This gas was excited with lasers for a variety of experiments. n = 2 atoms were prepared using a single-photon excitation scheme (1S to 2P) in controlled electric and magnetic fields for studies of Stark and Zeeman effects, measurements of Ps cooling via Doppler spectroscopy, and for the produciton of ensembles of atoms in pure 2S states. The first measurements of Ps excitation to specific Rydberg-Stark states were performed via a two-color two-photon excitation scheme ( 1S to 2P to nS/nD). Ps atoms in low-field–seeking Rydberg Stark states were prepared at the entrance of an electrostatic quadrupole guide which was used to control the trajectories and velocity distributions of the Ps atoms. These advances, together with the results from numerical simulations, suggest that these methods could be used in to perform Stark deceleration and trapping of Rydberg Ps, high-precision Ps spectroscopy, and to create positron-atom bound states.
We demonstrate experimentally the production of Rydberg positronium (Ps) atoms in a two-step process, comprising incoherent laser excitation, first to the 2(3)P state and then to states with principal quantum numbers ranging from 10 to 25. We find that excitation of 2(3)P atoms to Rydberg levels occurs very efficiently (~90%) and that the ~25% overall efficiency of the production of Rydberg atoms is determined almost entirely by the spectral overlap of the primary excitation laser and the Doppler broadened width of the 1 (3)S-2(3)P transition. The observed efficiency of Rydberg Ps production can be explained if stimulated emission back to the 2P states is suppressed, for example, by intermixing of the Rydberg state Stark sublevels. The efficient production of long-lived Rydberg Ps in a high magnetic field may make it possible to perform direct measurements of the gravitational free fall of Ps.
Rydberg states of atomic helium with principal quantum numbers ranging from n=20n=20n=20 to n=100n=100n=100 have been prepared by non-resonance-enhanced single-color two-photon excitation from the metastable 23S12\phantom{\rule{0.16em}{0ex}}{{}^{3}S}_{1}23S1​ state. Photoexcitation was carried out using linearly and circularly polarized pulsed laser radiation. In the case of excitation with circularly polarized radiation, Rydberg states with azimuthal quantum number $|{m}_{\ensuremath{\ell}}|=2$ were prepared in zero electric field and in homogeneous electric fields oriented parallel to the propagation axis of the laser radiation. In sufficiently strong electric fields, individual Rydberg--Stark states were resolved spectroscopically, highlighting the suitability of non-resonance-enhanced multiphoton excitation schemes for the preparation of long-lived high-$|{m}_{\ensuremath{\ell}}|$ hydrogenic Rydberg states for deceleration and trapping experiments. Applications of similar schemes for Doppler-free excitation of positronium atoms to Rydberg states are also discussed.
Abstract We produce Rydberg Ps by a two-step laser excitation from and from to states of principal quantum level that are Stark split by a motionally induced electric field. Our measurements are largely free of first-order Doppler shifts such that we are able to investigate the impact of laser polarization on the population of the closely spaced Stark levels. We find a variation in the distribution that is primarily dependent on the IR laser polarization with respect to the direction of the motionally induced electric field. With the IR light polarized parallel to the electric field F , the ratio of excitation probability to the levels of maximal Stark splitting compared to that of excitation to the states of minimal Stark splitting is found to be 3.37 ± 0.51, whereas with the IR light polarized perpendicular to F , the excitation ratio is 0.87 ± 0.64. Our results agree with those of Wall et al (2015 Phys. Rev. Lett. 114 173001 ) obtained with n = 11 and will be useful in the preparation of high- n states of Ps for a variety of experiments, including measuring the interaction of Ps with gravity, in precision time-of-flight (TOF) energy spectroscopy, and precision optical spectroscopy of Ps.