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arXiv:2506.04504 · Physical Review A

Doppler-free Rydberg spectroscopy in a warm vapor

Jeremy Glick, Brielle E. Anderson, T. Nathan Nunley, Josiah Bingaman, Jian Jun Liu, David H. Meyer, Paul Kunz

Published Oct 2, 2025• 3 citations
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Abstract

The common approach for producing Rydberg atoms in warm vapor cells is with lasers arranged in a counterpropagating, collinear configuration. Doppler effects in these configurations reduce the efficiency of excitation to the Rydberg state while also producing broadened spectral features. In this work, we demonstrate a three-laser Doppler-free excitation using laser beams whose k vectors sum to 0, resulting in an enhancement in the Rydberg density and narrowed spectral features. A three-times enhancement to Rydberg density along with a near four-times reduction in spectroscopic linewidths are observed compared to a collinear configuration. This Doppler-free configuration could prove beneficial to Rydberg atomic technologies, such as electric field sensing with small volumes or deterministic photon sources.

DOI
10.1103/qzwk-2g33

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The common approach for producing Rydberg atoms in warm vapor cells is with lasers arranged in a counterpropagating, collinear configuration. Doppler effects in these configurations reduce the efficiency of excitation to the Rydberg state while also producing broadened spectral features. In this work, we demonstrate a three-laser Doppler-free excitation using laser beams whose k vectors sum to 0, resulting in an enhancement in the Rydberg density and narrowed spectral features. A three-times enhancement to Rydberg density along with a near four-times reduction in spectroscopic linewidths are observed compared to a collinear configuration. This Doppler-free configuration could prove beneficial to Rydberg atomic technologies, such as electric field sensing with small volumes or deterministic photon sources.
Three-photon laser excitation of Rydberg states by three different laser beams can be arranged in a starlike geometry that simultaneously eliminates the recoil effect and Doppler broadening. Our analytical and numerical calculations for a particular laser excitation scheme $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}6{S}_{1/2}\ensuremath{\rightarrow}nP$ in Rb atoms have shown that, compared to the one- and two-photon laser excitation, this approach provides much narrower linewidth and longer coherence time for both cold atom samples and hot vapors, if the intermediate one-photon resonances of the three-photon transition are detuned by more than respective single-photon Doppler widths. This method can be used to improve fidelity of Rydberg quantum gates and precision of spectroscopic measurements in Rydberg atoms.
The self-calibration of rf sensors using Rydberg-atom vapor cells is a major advantage over conventional rf antennas, but has been limited by Doppler broadening. In this study, ultranarrow linewidths comparable to those in ultracold gases are obtained in a room-temperature vapor cell, by overcoming Doppler shifts via a three-photon scheme to reduce the spectral linewidth to less than 200 kHz. This narrow linewidth extends the self-calibrated regime of such sensors by over an order of magnitude, compared to what has been achieved in standard two-photon schemes.
We demonstrate coherent Doppler-free three-photon excitation of the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ optical clock transition and the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ intercombination transition in free-space thermal clouds of 88Sr^{88}\mathrm{Sr}88Sr atoms. By appropriate orientation of the wave vectors of three lasers incident on the atoms, the first-order Doppler shift can be eliminated for all velocity classes. Three-photon excitation of the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ transition enables high-contrast Ramsey spectroscopy with interrogation times comparable to the $21\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ natural lifetime using a single near-resonant laser source. Three-photon spectroscopy on the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ clock transition, using only laser frequencies nearly resonant with the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ and $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ transitions, enables a reduction in Doppler broadening by two orders of magnitude and a corresponding $\ensuremath{\sim}470\phantom{\rule{0.16em}{0ex}}\mathrm{Hz}$ linewidth without a confining potential.
We demonstrate Rydberg atom-based radio frequency sensing with a colinear three-photon scheme in a room temperature cesium vapor cell that minimizes residual Doppler broadening of the probe laser absorption feature. A sub-200 kHz spectral linewidth is observed and extends the self-calibrated Autler-Townes sensing regime to weaker fields by a factor of ~18 compared to the theoretical limit of the most commonly used two-photon scheme. The sensitivity of the method to microsecond pulses is shown to be sufficient to detect radio frequency Rabi frequencies of 2πππ x 0.44 MHz using a 480 kHz bandwidth at 108.9 GHz, demonstrating the ability to sense time-dependent signals suitable for radar and communications.
We demonstrate the single-photon excitation spectra of cesium Rydberg atoms by means of a Doppler-free purely all-optical detection with a room-temperature vapor cell and a 319 nm ultra-violet (UV) laser. We excite atoms directly from 6S1/2 ground state to 71P3/2 Rydberg state with a narrow-linewidth 319 nm UV laser. The detection of Rydberg states is performed by monitoring the absorption of an 852 nm probe beam in a V-type three-level system. With a strong coupling light, we observe the Autler-Townes (AT) doublet, and the dependences of the separation and linewidths on the coupling intensity are experimentally investigated, which is consistent with the prediction based on the dressed state theory. Moreover, the AT splitting can be used to measure the Rabi frequency. In an external magnetic field, the Rydberg spectra of nondegenerate Zeeman sublevels are demonstrated. The splitting of the spectrum is of great significance for studying the characteristics of Rydberg atoms.
The sensitivity of electric field sensors based on two-photon electromagnetically induced transparency (EIT) involving highly excited Rydberg states in thermal atoms is often limited by the residual Doppler effect and optical power broadening. Here, we propose a method to reduce the EIT spectral linewidth using a Ramsey interrogation approach, allowing multiple interrogations of atomic coherence, using either temporally or spatially separated laser beams. Our theoretical calculations predict that the linewidth of such Raman-Ramsey spectral features can be substantially reduced compare to a standard Doppler-broadened EIT, opening a possibility to improve sensitivity of Rydberg atomic vapor-based sensors.