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Journal of the Optical Society of America B

Two-color photoexcitation of Rydberg states via an electric quadrupole transition

Leping Li, Quanli Gu, Joseph L. Knee, John D. Wright, Jack DiSciacca, T. J. Morgan

Published Feb 13, 2008• 1 citation
Publisher

Abstract

We report the observation of an electric quadrupole transition between the 4s′[1/2]o0 and 3d[3/2]o2 states in the spectrum of argon and use it in the first step of a scheme to excite Rydberg states. The initial identification of the transition is based on one-color, two-photon photoionization. A different experiment utilizing two-color, two-photon photoexcitation to Rydberg states confirms the identification. Despite the unavoidable background of one-color, two-photon photoionization, the latter experimental technique makes possible two-photon spectroscopy of Rydberg states using a resonant intermediate state populated by an electric quadrupole transition.

DOI
10.1364/josab.25.000334

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We report the observation of an electric quadrupole transition between the 4s′[1/2]o0 and 3d[3/2]o2 states in the spectrum of argon and use it in the first step of a scheme to excite Rydberg states. The initial identification of the transition is based on one-color, two-photon photoionization. A different experiment utilizing two-color, two-photon photoexcitation to Rydberg states confirms the identification. Despite the unavoidable background of one-color, two-photon photoionization, the latter experimental technique makes possible two-photon spectroscopy of Rydberg states using a resonant intermediate state populated by an electric quadrupole transition.
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.
An advanced undergraduate experiment to study the 5P3/2→6P3/2 electric quadrupole transition in rubidium atoms is presented. The experiment uses two external cavity diode lasers, one operating at the D2 rubidium resonance line and the other built with commercial parts to emit at 911 nm. The lasers produce the 5s→5p→6p excitation sequence in which the second step is the forbidden transition. Production of atoms in the 6P3/2 state is observed by detection of the 420 nm fluorescence that results from electric dipole decay into the ground state. Lines whose widths are significantly narrower than the Doppler width are used to study the hyperfine structure of the 6P3/2 state in rubidium. The spectra illustrate characteristics unique to electric dipole forbidden transitions, like the electric quadrupole selection rules; they are also used to show general aspects of two-color laser spectroscopy such as velocity selection and hyperfine pumping.
We report the observation of dipole-forbidden, but quadrupole-allowed, one-photon transitions to high-Rydberg states in Rb. Using pulsed uv excitation of ultracold atoms in a magneto-optical trap, we excite $5s\ensuremath{\rightarrow}nd$ transitions over a range of principal quantum numbers n=27−−59n=27--59n=27−−59. Compared to dipole-allowed (E1) transitions from $5s\ensuremath{\rightarrow}np$, these E2 transitions are weaker by a factor of approximately 2000. We also report measurements of the anomalous np3/2:np1/2n{p}_{3/2}:n{p}_{1/2}np3/2​:np1/2​ fine-structure transition strength ratio for n=28−−75n=28--75n=28−−75. Both results are in agreement with theoretical predictions.
Two-step resonant photoionization of free Ni atoms is studied by one-color and two-color processes, using pulsed lasers with photon energies around half the ground-state ionization energy. Two-color two-step resonance ionization from the ground state a3{\mathrm{}}^{3}3F4{\mathit{F}}_{4}F4​ and the first metastable state a3{\mathrm{}}^{3}3D3{\mathit{D}}_{3}D3​ via the triplet states z3{\mathrm{}}^{3}3G3,4,50{\mathit{G}}_{3,4,5}^{0}G3,4,50​ was used to probe the autoionizing states just above the ionization limit. Several strong lines in the one-color ionization spectrum are explained as direct two-photon transitions to autoionizing states. Photoionization cross sections were deduced from saturation measurements. The large cross sections observed for specific one-color two-step transitions are due to the near double resonant excitation into autoionizing states. \textcopyright{} 1996 The American Physical Society.
We explore a single-photon approach to Rydberg state excitation and Rydberg blockade. Using detailed theoretical models, we show the feasibility of direct excitation, predict the effect of background electric fields, and calculate the required interatomic distance to observe Rydberg blockade. We then measure and control the electric field environment to enable coherent control of Rydberg states. With this coherent control, we demonstrate Rydberg blockade of two atoms separated by 6.6(3) {\mu}m. When compared with the more common two-photon excitation method, this single-photon approach is advantageous because it eliminates channels for decoherence through photon scattering and AC Stark shifts from the intermediate state while moderately increasing Doppler sensitivity.
Abstract We present the first evidence of excitation of the 5 p 3 / 2 → 6 p 1 / 2 electric dipole-forbidden transition in atomic rubidium. The experiments were done in a rubidium vapor cell using Doppler-free optical–optical double resonance spectroscopy with counter-propagating beams, with a similar scheme to the excitation of the other fine transition 6 p 3/2 in the 6 p J manifold reported in Ponciano-Ojeda et al (2015 Phys. Rev. A 92 042511). The 5 p 3 / 2 → 6 p 1 / 2 dipole-forbidden excitation occurs at a wavelength λ ≈ 917.5 nm. The spectra showed the two main hyperfine states of the 6 p 1/2 manifold, and also resolved up to three satellites that appear due to effects of selection of velocities in thermal rubidium atoms. The polarization dependence of the relative intensities of the hyperfine lines of the decay fluorescence is also investigated. The data show that the individual line intensities and also the total cross-section have a strong dependence on the polarization direction. Experimental data for different polarization configurations of the light beams used in this two-photon spectroscopy are compared with the results of calculations that consider a strong atom-field coupling in the preparation step, followed by a weak electric quadrupole excitation and the blue fluorescence decay emission. Good agreement between experiment and this three-step model is found in the case of linear–linear polarizations, which confirms the results found for the 5 p 3 / 2 → 6 p 3 / 2 forbidden transition. The results presented here complete the information about the 5 p 3/2 → 6 p J electric dipole-forbidden transition in rubidium.