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Journal of the Optical Society of America B

Infrared radio-frequency double-resonance spectroscopy of molecular vibrational-overtone bands using a Fabry–Perot cavity-absorption cell

Chikako Ishibashi, 竜二 実藤, Hiroyuki Sasada

Published Jul 1, 2001• 5 citations
Publisher

Abstract

Infrared (ir) radio-frequency (rf) double-resonance spectroscopy was carried out on the vibrational-overtone band of methyl iodide molecules (CH3I). An optical Fabry-Perot cavity was employed as an absorption cell to record saturated ir spectral lines even by a small-power extended-cavity diode laser with a high sensitivity and a wide tunability in the presence of a rf field. These features allowed investigation of molecules strongly coupled with monochromatic and bichromatic rf fields, or dressed molecules, at various rf power levels and detuning frequencies for a variety of ir and rf transitions. At appropriate energy-level schemes, quantum-interference effects were observed. All resultant spectra showed good agreement with dressed-state theoretical calculations, indicating that the present spectrometer is valid for precise investigation of dressed molecules.

DOI
10.1364/josab.18.001019

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Infrared (ir) radio-frequency (rf) double-resonance spectroscopy was carried out on the vibrational-overtone band of methyl iodide molecules (CH3I). An optical Fabry-Perot cavity was employed as an absorption cell to record saturated ir spectral lines even by a small-power extended-cavity diode laser with a high sensitivity and a wide tunability in the presence of a rf field. These features allowed investigation of molecules strongly coupled with monochromatic and bichromatic rf fields, or dressed molecules, at various rf power levels and detuning frequencies for a variety of ir and rf transitions. At appropriate energy-level schemes, quantum-interference effects were observed. All resultant spectra showed good agreement with dressed-state theoretical calculations, indicating that the present spectrometer is valid for precise investigation of dressed molecules.
We investigate and employ optical Rydberg resonances in an atomic vapor cell for measurements of high-intensity VHF-band radio frequency (rf) electric fields. An atomic vapor cell with integrated electrodes is used to generate high-intensity 50--500 MHz rf electric fields reaching $\ensuremath{\sim}5$ kV/m in a submillimeter gap. The fields are measured using Rydberg electromagnetically induced transparency as an optical readout of field-sensitive 30DJ30{D}_{J}30DJ​ and 35DJ35{D}_{J}35DJ​ Rydberg states of atoms within the gap. The rf electric field is determined by matching observed spectroscopic markers, including ac level shifts, even-harmonic rf sidebands, and rf-induced avoided crossings in the Rydberg manifold to calculated spectra derived from a nonperturbative Floquet theory. In our measurements, rf field frequencies and electric-field amplitudes are determined to an accuracy of 1.01.0%1.0 and 1.51.5%1.5, respectively. In the atom-field interaction, we observe a transition from a quantum regime, characterized by discrete even-harmonic Floquet states separated by an even multiple of the rf field frequency, into a semiclassical regime at very strong fields, in which the spectrum exhibits unresolved resonances whose strengths are smoothly modulated at a frequency of approximately five times the rf frequency. The underlying physics is explored.
We study sub-Doppler saturation resonances at cesium molecular transitions in the absorption band B1Πu ← X1∑g+ near 780 nm by using a commercial diode laser. The saturation power is measured as low as 5.7 mW with the laser beam diameter of 0.1 cm. Optical saturation is associated with the optical pumping of molecular ground-state levels. The long relaxation time of ground-state levels could attract interest to electromagnetically induced transparency and quantum state memory in the molecular gas. We propose to use the molecular transitions as references for doubled-frequency sources in the communication band around 1550 nm.
The molecular response in laser intracavity experiments where molecules interact simultaneously with a radio frequency field and an infrared one is analyzed theoretically. In the quantized field approach the molecule–radio frequency interaction is treated exactly. For the laser intensity the density matrix equations are solved either in a third-order perturbation treatment or through a matrix continued fraction analysis. The resonance line shapes in different two-level and three-level configurations are analyzed numerically.
We examine spectral signatures of Rydberg atoms driven with near-resonant dual-tone radio-frequency (RF) fields in the regime of strong driving. We experimentally demonstrate and theoretically model a variety of nonlinear and multiphoton phenomena in the atomic Rydberg response that manifest in the EIT spectra. Our results echo previous studies of two-level atoms driven with bichromatic optical fields. In comparison to the optical studies, the RF-driven Rydberg system utilizes a more complex excitation pathway, and electromagnetic fields from two different spectral regimes: a two-photon optical excitation continuously creates highly excited Rydberg atoms, while RF fields drive resonant coupling between the Rydberg levels and generate strong mixing. Yet, our spectra reflect nearly identical effects of the dual-tone RF fields on the atomic Rydberg observables, showing detuning-dependent splittings and Rabi frequency dependent peak numbers and relative strengths, and avoided crossings at subharmonic resonances. We thus validate previous two-state models in this more complex physical system. In the context of Rydberg electrometry, we use these investigations to explore a technique where we tune a known RF field to observe spectra which give frequency and power of an unknown RF field using the complex dual-tone spectra.
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We study Rydberg atoms modulated by strong radio-frequency (rf) fields with a frequency of 70 MHz. The Rydberg atoms are prepared in a room-temperature cesium cell, and their level structure is probed using electromagnetically induced transparency (EIT). As the rf field increases from the weak- into the strong-field regime, the range of observed rf-induced phenomena progresses from ac level shifts through increasingly pronounced and numerous rf modulation sidebands to complex state mixing and level crossings with $\mathrm{high}\ensuremath{-}l$ hydrogenlike states. Weak anharmonic admixtures in the rf field generate clearly visible modifications in the Rydberg EIT spectra. A Floquet analysis is employed to model the Rydberg spectra, and good agreement with the experimental observations is found. Our results show that all-optical spectroscopy of Rydberg atoms in vapor cells can serve as an antenna-free, atom-based, and calibration-free technique to measure rf electric fields and to analyze their higher-harmonic contents.