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arXiv:2501.02665 · Optics Letters

Sub-Doppler spectroscopy of Rydberg atoms via velocity selection memory in a hot vapor cell

Esther Butery, Biplab Dutta, Stephany Santos, S. Barreiro, Weliton Soares Martins, H. Failache, Athanasios Laliotis

Published Dec 17, 2024• 3 citations
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Abstract

We study resonance redistribution mechanisms inside a hot vapor cell. This is achieved by pumping cesium atoms on the 6S 1/2 →6P 1/2 resonance and subsequently probing the velocity distribution of the 6P 1/2 population by a linear absorption experiment on the 6P 1/2 →16S 1/2 or 6P 1/2 →15D 3/2 transitions at 514 nm and 512 nm, respectively. We demonstrate that despite the existence of thermalization processes, traces of the initial velocity selection, imposed by the pump, survive in both hyperfine levels of the intermediate (6P 1/2 ) state. This observation allows us to perform sub-Doppler resolution vapor cell spectroscopy on Rydberg states using a simple pump–probe setup. At high cesium densities, redistribution mechanisms dominate, and the velocity selection vanishes. However, spectral analysis provides the collisional shifts and broadenings of the probed Rydberg states.

DOI
10.1364/ol.542755

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[Study of resonance exchange collisions in cesium vapour by optical-optical double resonance spectroscopy].

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An experimental study of cesium resonance exchange collision, Cs(6P(3/2), v) + Cs(6S(1/2), v')-->Cs(6S(1/2), v) + Cs (6P(3/2), v'), was carried out. Populations of excited atoms that all have the same z component of velocity were produced by pumping a vapor with a narrow-band laser. A counterpropagating single-mode diode laser was used to probe the excited atom velocity distribution in the 6P(3/2)-->8S(1/2) transition. Fluorescence was monitored in the 8S(1/2)-->6P(3/2) transition. The magnitude of the thermalizinng effect of resonance exchange collisions was estimated by measuring the ratio of the intensity in the narrow features to that associated with the Doppler pedestals. The rate coefficient of 9.62 x 10(-7) cm3 x s(-1) for the resonance exchange collisions was yielded. This work demonstrates that, in a pure metal vapor, the thermalization of velocity-selected excited-atom distribution by the mechanism of resonance exchange can be three orders of magnitude greater than that from velocity-changing collisions.

•Nov 1, 2006•0 citations
We study resonance redistribution mechanisms inside a hot vapor cell. This is achieved by pumping cesium atoms on the 6S 1/2 →6P 1/2 resonance and subsequently probing the velocity distribution of the 6P 1/2 population by a linear absorption experiment on the 6P 1/2 →16S 1/2 or 6P 1/2 →15D 3/2 transitions at 514 nm and 512 nm, respectively. We demonstrate that despite the existence of thermalization processes, traces of the initial velocity selection, imposed by the pump, survive in both hyperfine levels of the intermediate (6P 1/2 ) state. This observation allows us to perform sub-Doppler resolution vapor cell spectroscopy on Rydberg states using a simple pump–probe setup. At high cesium densities, redistribution mechanisms dominate, and the velocity selection vanishes. However, spectral analysis provides the collisional shifts and broadenings of the probed Rydberg states.
We study the excitation redistribution from cesium 7P1/27\mathrm{P}_{1/2}7P1/2​ or 7P3/27\mathrm{P}_{3/2}7P3/2​ to neighboring energy levels by Black Body Radiation (BBR) and inter atomic collisions using pump-probe spectroscopy inside a vapor cell. At low vapor densities we measure redistribution of the initial, velocity-selected, atomic excitation by BBR. This preserves the selected atomic velocities allowing us to perform high resolution spectroscopy of the 6D→7F\mathrm{6D\rightarrow 7F}6D→7F transitions. This transfer mechanism could also be used to perform sub-Doppler spectroscopy of the cesium highly-excited nG\mathrm{nG}nG levels. At high densities we observe interatomic collisions redistributing the excitation within the cesium 7P\mathrm{7P}7P fine and hyperfine structure. We show that 7P\mathrm{7P}7P redistribution involves state-changing collisions that preserve the initial selection of atomic velocities. These redistribution mechanisms can be of importance for experiments probing high lying excited states in dense alkali vapor.
Abstract We study the excitation redistribution from cesium 7P 1/2 or 7P 3/2 to neighboring energy levels by black body radiation (BBR) and inter atomic collisions using pump-probe spectroscopy inside a vapor cell. At low vapor densities we measure redistribution of the initial, velocity-selected, atomic excitation by BBR. This redistribution preserves the selected atomic velocities allowing us to perform high resolution spectroscopy of the 6D → 7F transitions. This transfer mechanism could also be used to perform sub-Doppler spectroscopy of the cesium highly-excited nG levels. At high densities we observe interatomic collisions redistributing the excitation within the cesium 7P fine and hyperfine structure. We show that 7P redistribution involves state-changing collisions that preserve the initial selection of atomic velocities. These redistribution mechanisms can be of importance for experiments probing high lying excited states in dense alkali vapor.
A velocity-selective spectroscopy technique for studying the spectra of Rydberg gases is presented. This method provides high-resolution spectrum measurements. We present experimental results for a ladder system 6S 1/2 → 6P 3/2 → n S(D) electromagnetically-induced transparency involving highly-excited Rydberg states. Based on a radio-frequency modulation technique, we measure the hyperfine structure splitting of intermediate states and the fine structure splitting of Rydberg states in a room temperature 133 Cs vapor cell. The experimental data and theoretical predictions show excellent agreement.
The spectra of Rydberg atoms are of great significance for studying the energy levels of Rydberg atoms and the interaction between neutral atoms, especially, the high-precision spectra of Rydberg atoms can be used to measure the energy level shifts of Rydberg atoms resulting from the dipole-dipole interactions in room-temperature vapor cells. In this paper we report the preparation of cesium Rydberg states based on the cascaded two-photon excitation of 509 nm laser and 852 nm laser in opposite, and the measurements of the fine structure of cesium Rydberg states. In this experiment, the 509 nm laser is generated by the cavity-enhanced second-harmonic generation from 1018 nm laser with a periodically-poled KTP crystal and has a maximum power of about 1 W, and the 852 nm probe laser is provided by an external-cavity diode laser with a maximum output power of 5 mW and a typical linewidth of 1 MHz. By scanning the frequency of 509 nm coupling laser, it is presented that the Doppler-free spectra based on electromagnetically-induced transparency (EIT) of 509 nm coupling laser and 852 nm probe laser. The velocity-selective EIT spectra are used to study the spectral splitting of 6S1/26P3/257S(D) ladder-type system of cesium Rydberg atoms in a room-temperature vapor cell. The powers of 852 nm probe laser and 509 nm coupling laser are 0.3 upW and 200 mW, respectively. Their waist radii are both approximately 50 m. The intervals of hyperfine splitting of the intermediate state 6P3/2(F'=3, 4, 5) and fine splitting of 57D3/2 and 57D5/2 Rydberg states are measured by a frequency calibrating. Concretely, the velocity-selective spectrum with a radio frequency (RF) modulation of 30 MHz is used as a reference to calibrate the Rydberg fine-structure states in the hot vapor cell, where the RF frequency precision is smaller than a hertz on long time scales and the EIT linewidth is smaller than 13 MHz. The experimental value of the fine structure splitting of 57D3/2 and 57D5/2 Rydberg states is (354.72.5) MHz, that is in consistence with the value of 346.8 MHz calculated by Rydberg-Ritz equation and quantum defects of 57D3/2 and 57D5/2 Rydberg states. The experimental values of hyperfine splitting of intermediate state 6P3/2(F'=3, 4, 5) are also coincident with the theoretical calculated values. The dominant discrepancy existing between the experimental and calculated results may arise from the nonlinear correspondence of the PZT while the 509 nm wavelength cavity is scanned, and the measurement accuracy influenced by the spectral linewidth. The velocity-selective spectroscopy technique can also be used to measure the energy level shifts caused by the interactions of Rydberg atoms.
We demonstrate a velocity selection scheme that mitigates suppression of electromagnetically induced transparency (EIT) by Doppler shifts for coupling wavelengths larger than the probe wavelength. An optical pumping beam counterpropagating with the EIT probe beam transfers atoms between hyperfine states in a velocity-selective fashion. Measurement of the transmitted probe beam synchronous with chopping of the optical pumping beam enables a Doppler-free EIT signal to be detected. Transition frequencies between 5P1/25{P}_{1/2}5P1/2​ and nS1/2n{S}_{1/2}nS1/2​ states for n=26n=26n=26, 27, and 28 in 39K^{39}\mathrm{K}39K are obtained via EIT spectroscopy in a heated vapor cell with a probe beam stabilized to the $4{S}_{1/2}\ensuremath{\rightarrow}5{P}_{1/2}$ transition. Using previous high-resolution measurements of the $4{S}_{1/2}\ensuremath{\rightarrow}n{S}_{1/2}$ transitions, we make a determination of the absolute frequency of the $4{S}_{1/2}\ensuremath{\rightarrow}5{P}_{1/2}$ transition. Our measurement is shifted by 560 MHz from the currently accepted value with a twofold improvement in uncertainty. These measurements will enable novel experiments with Rydberg-dressed ultracold Fermi gases composed of 40K^{40}\mathrm{K}40K atoms.
An experimental study of cesium resonance exchange collision, Cs(6P(3/2), v) + Cs(6S(1/2), v')-->Cs(6S(1/2), v) + Cs (6P(3/2), v'), was carried out. Populations of excited atoms that all have the same z component of velocity were produced by pumping a vapor with a narrow-band laser. A counterpropagating single-mode diode laser was used to probe the excited atom velocity distribution in the 6P(3/2)-->8S(1/2) transition. Fluorescence was monitored in the 8S(1/2)-->6P(3/2) transition. The magnitude of the thermalizinng effect of resonance exchange collisions was estimated by measuring the ratio of the intensity in the narrow features to that associated with the Doppler pedestals. The rate coefficient of 9.62 x 10(-7) cm3 x s(-1) for the resonance exchange collisions was yielded. This work demonstrates that, in a pure metal vapor, the thermalization of velocity-selected excited-atom distribution by the mechanism of resonance exchange can be three orders of magnitude greater than that from velocity-changing collisions.