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arXiv:1412.3043 · Physical Review A

Single-color two-photon spectroscopy of Rydberg states in electric fields

Thomas E. Wall, D. B. Cassidy, S. D. Hogan

Published Nov 25, 2014• 10 citations
arXivHTMLPDF

Abstract

Rydberg states of atomic helium with principal quantum numbers ranging from $n=20$ to $n=100$ have been prepared by non-resonance-enhanced single-color two-photon excitation from the metastable $2\phantom{\rule{0.16em}{0ex}}{{}^{3}S}_{1}$ 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.

DOI
10.1103/physreva.90.053430

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Circular Rydberg states with n=70n=70n=70 have been prepared in helium using a modified version of the crossed-fields method. This approach to the preparation of high-nnn circular Rydberg states overcomes limitations of the standard crossed-fields method which arise at this, and higher, values of nnn. The experiments were performed with atoms traveling in pulsed supersonic beams that were initially laser photoexcited from the metastable 1s2s3S11s2s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s2s3S1​ level to the 1s73s3S11s73s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s73s3S1​ level by resonance-enhanced two-color two-photon excitation in a magnetic field of 16.154 G. These excited atoms were then polarized using a perpendicular electric field of 0.844 V/cm, and transferred by a pulse of microwave radiation to the state that, when adiabatically depolarized, evolves into the n=70n=70n=70 circular state in zero electric field. The excited atoms were detected by state-selective electric field ionization. Each step of the circular state preparation process was validated by comparison with the calculated atomic energy-level structure in the perpendicular electric and magnetic fields used. Of the atoms initially excited to the 1s73s3S11s73s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s73s3S1​ level, $\ensuremath{\sim}80%$ were transferred to the n=70n=70n=70 circular state. At these high values of $n, \mathrm{\ensuremath{\Delta}}n=1$ circular-to-circular Rydberg state transitions occur at frequencies below 20 GHz. Consequently, atoms in these states, and the circular state preparation process presented here, are well suited to hybrid cavity QED experiments with Rydberg atoms and superconducting microwave circuits.
Helium atoms travelling in pulsed supersonic beams have been photoexcited from the metastable 1s2s 3 S 1 level to Rydberg states with principal quantum numbers exceeding 400 by resonance-enhanced two-colour two-photon excitation using narrow-bandwidth CW laser radiation. To achieve this, the photoexcitation region was shielded and stray electric fields cancelled using a cubic arrangement of 80 mm × 80 mm copper plates. The excited Rydberg atoms were detected by pulsed electric field ionisation downstream from this photoexcitation region. Comparison of the experimental spectra with the results of calculations indicate that the stray electric fields at the position of Rydberg state photoexcitation were reduced to as low as 160 μ V cm –1 . Using helium in these experiments minimises temporal changes in the stray fields resulting from surface adsorption. Measurements performed 70 h apart indicate that the rate of change of these fields was on the order of 2 μ V cm –1 per h, making beams of metastable helium atoms ideally suited as probes for high precision electrometry in spectroscopy experiments involving less readily available species such as positronium or antihydrogen.
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.
Helium atoms have been prepared in the circular $|n=55,\ensuremath{\ell}=54,{m}_{\ensuremath{\ell}}=+54\ensuremath{\rangle}$ Rydberg state using the crossed electric and magnetic fields method. The atoms, initially traveling in pulsed supersonic beams, were photoexcited from the metastable 1s2s3S11s2s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s2s3S1​ level to the outermost, ${m}_{\ensuremath{\ell}}=0$ Rydberg-Stark state with n=55n=55n=55 in the presence of a strong electric field and weak perpendicular magnetic field. Following excitation, the electric field was adiabatically switched off causing the atoms to evolve into the circular state with ${m}_{\ensuremath{\ell}}=+54$ defined with respect to the magnetic-field quantization axis. The circular states were detected by ramped electric-field ionization along the magnetic-field axis. The dependence of the circular state production efficiency on the strength of the excitation electric field, and the electric-field switch-off time was studied, and microwave spectroscopy of the circular-to-circular $|55,54,+54\ensuremath{\rangle}\ensuremath{\rightarrow}|56,55,+55\ensuremath{\rangle}$ transition at $\ensuremath{\sim}38.5$ GHz was performed.
Fluorescence-dip spectroscopy based on an optical double resonance is used to probe the Stark splitting in highly excited Rydberg states of atomic hydrogen. After Doppler-free two-photon excitation to n=3n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}3n=3, fluorescence at Balmer $\ensuremath{\alpha}$ is observed. When the radiation of a second laser is tuned over the resonance between n=3n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}3n=3 and a Rydberg state, the Stark splitting manifests itself as a series of dips in the Balmer- $\ensuremath{\alpha}$ fluorescence intensity. Rydberg states up to n=55n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}55n=55 can be identified. The minimum detectable electric field is 5V/cm5\mathrm{V}/\mathrm{cm}5V/cm. This is about an order of magnitude more sensitive than other laser-induced fluorescence techniques.
The Stark splitting of the second excited level of atomic hydrogen (with principal quantum number n=3n=3n=3) has been measured by pulsed laser spectroscopy in order to determine small electric fields by optical means. Doppler-free excitation with two counterpropagating laser beams at 205nm205\phantom{\rule{0.3em}{0ex}}\mathrm{nm}205nm allows us to measure the n=3n=3n=3 Stark spectra either by an optogalvanic signal after ionization by a third laser photon or by detection of the Balmer-$\ensuremath{\alpha}$ fluorescence photons emitted by the excited atoms. Three different cases of laser polarization have been investigated in order to evaluate the possibilities and limitations of this one-step laser excitation method for electric field determination, especially at field strengths below 200V∕cm200\phantom{\rule{0.3em}{0ex}}\mathrm{V}∕\mathrm{cm}200V∕cm. The method provides the best field sensitivity achieved with lower excited levels that can be reached directly by two-photon absorption from the ground state (in contrast to the more sensitive Rydberg levels). For this purpose, an advanced tunable pulsed uv laser with narrow bandwidth almost at the Fourier limit has been used. The high spectral resolution allowed us to deduce electric field strengths as small as 50V∕cm50\phantom{\rule{0.3em}{0ex}}\mathrm{V}∕\mathrm{cm}50V∕cm from the frequency shift between two selected isolated Stark components. As a main advantage, this simple analysis of the measured spectra does not rely on knowledge of the line intensities which may be strongly affected by the measuring conditions.