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Optics Letters

Three-photon excitation of hydrogen Rydberg states

Wallace L. Glab, Munir Hasan Nayfeh

Published Jan 1, 1983• 11 citations
Publisher

Abstract

A three-photon process using radiation at 2430 and 3660 A and with a 1s-2s two-photon resonance is used to excite atomic hydrogen from the ground state to Rydberg states of high principal quantum number. Collision-induced ionization is used to monitor the excitation.
DOI
10.1364/ol.8.000030

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Two-photon-resonant, three-photon ionization of atomic hydrogen and deuterium is performed at 243 nm, and the ions are detected by time-of-flight mass spectrometry. The power dependence of the 1S-2S two-photon excitation and one-photon ionization of 2S hydrogen and deuterium are determined. The ionization step saturates at 4 x 10(6) W/cm(2). The two-photon step-power dependence varies with laser linewidth, with saturation occurring between 1 x 10(7) and 3 x 10(7) W/cm(2). The extraction electric field in the mass spectrometer does not affect the 2S excitation. Strong signals are recorded at atomic concentrations of 10(5) atoms/cm(3). Nonresonant ionization of background gases producing H(+) and D(+) is minimized.
Tunable coherent ultraviolet radiation has been used to excite selectively the n=3n=3n=3 level in hydrogen and deuterium atoms via two-photon absorption from the ground state. The resulting Balmer-$\ensuremath{\alpha}$ fluorescence at 656 nm was observed as well as resonant three-photon ionization. This work demonstrates several advantages over other techniques for selective detection of neutral H and D atoms, including three-dimensional spatial resolution and a remote monitoring capability afforded by the use of laser-induced-fluorescence detection.
Tunable coherent ultraviolet radiation has been used to excite selectively the n=3n=3n=3 level in hydrogen and deuterium atoms via two-photon absorption from the ground state. The resulting Balmer-$\ensuremath{\alpha}$ fluorescence at 656 nm was observed as well as resonant three-photon ionization. This work demonstrates several advantages over other techniques for selective detection of neutral H and D atoms, including three-dimensional spatial resolution and a remote monitoring capability afforded by the use of laser-induced-fluorescence detection.
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.
We have measured the resonance-enhanced four-photon ionization of atomic hydrogen. The degenerate four-photon process occurs via a three-photon resonance between the 1s and the 2p levels, with subsequent one-photon ionization near threshold. We have studied the highly asymmetric resonance-enhanced profile, i.e., the photoion yield as a function of laser detuning from three-photon resonance between the 1s and 2p levels. In particular, we have determined the width, shift, peak, and asymmetry of the profile as a function of laser intensity. The experimental results are compared to theoretical models. These models involve both the properties of the atom in an intense near-resonant radiative field, and a detailed model for the multimode laser field, particularly the field fluctuations due to mode beating. The asymmetric resonance-enhanced photoionization profile is well reproduced by both a random-phase and a chaotic-light model.