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arXiv:2007.08452 · Physical Review Applied

Single-Photon-Level Sub-Doppler Pump-Probe Spectroscopy of Rubidium

Paul Burdekin, Samuele Grandi, Rielly Newbold, Rowan A. Hoggarth, Kyle D. Major, Alex S. Clark

Published Oct 23, 2020• 9 citations
arXivHTMLPDF

Abstract

We propose and demonstrate pump-probe spectroscopy of rubidium absorption that reveals the sub-Doppler hyperfine structure of the ${}^{5}{\mathrm{S}}_{1/2}\ensuremath{\leftrightarrow}{}^{5}{\mathrm{P}}_{3/2}$ (${\mathrm{D}}_{2}$) transitions. The counterpropagating pump and probe lasers are independently tunable in frequency, with the probe operating at the single-photon level. The two-dimensional spectrum measured as the laser frequencies are scanned shows fluorescence, Doppler-broadened absorption dips, and sub-Doppler features. The detuning between the pump and probe lasers allows compensation of the Doppler shift for all atomic velocities in the room-temperature vapor, meaning we observe sub-Doppler features for all atoms in the beam. We detail a theoretical model of the system that incorporates fluorescence, saturation effects, and optical pumping and compare this with the measured spectrum, finding a mean absolute percentage error of 3.11%. This high level of agreement allows us to extract the number density and temperature of the $\mathrm{Rb}$ vapor from the two-dimensional spectrum. In the future this technique could be used as an atomic frequency standard for calibrating and characterising a single-photon or low-light-level source.

DOI
10.1103/physrevapplied.14.044046

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We propose and demonstrate pump-probe spectroscopy of rubidium absorption that reveals the sub-Doppler hyperfine structure of the 5S1/2\ensuremath↔5P3/2{}^{5}{\mathrm{S}}_{1/2}\ensuremath{\leftrightarrow}{}^{5}{\mathrm{P}}_{3/2}5S1/2​\ensuremath↔5P3/2​ (D2{\mathrm{D}}_{2}D2​) transitions. The counterpropagating pump and probe lasers are independently tunable in frequency, with the probe operating at the single-photon level. The two-dimensional spectrum measured as the laser frequencies are scanned shows fluorescence, Doppler-broadened absorption dips, and sub-Doppler features. The detuning between the pump and probe lasers allows compensation of the Doppler shift for all atomic velocities in the room-temperature vapor, meaning we observe sub-Doppler features for all atoms in the beam. We detail a theoretical model of the system that incorporates fluorescence, saturation effects, and optical pumping and compare this with the measured spectrum, finding a mean absolute percentage error of 3.11%. This high level of agreement allows us to extract the number density and temperature of the Rb\mathrm{Rb}Rb vapor from the two-dimensional spectrum. In the future this technique could be used as an atomic frequency standard for calibrating and characterising a single-photon or low-light-level source.
An ongoing spectroscopic investigation of atomic rubidium utilizes a two-photon, single-laser excitation process. Transitions accessible with our tunable laser include 5P1/2 (F ′ ) ← 5S1/2 (F) and 5P3/2 (F ′ ) ← 5S1/2 (F). The laser is split into a pump and probe beam to allow for Doppler-free measurements of transitions between hyperfine levels. The pump and probe beams are overlapped in a counter-propagating geometry and the laser frequency scans over a transition. Absorption, fluorescence and polarization spectroscopy techniques are applied to this basic experimental setup. The temperature of the vapor cell and the power of the pump and probe beams have been varied to explore line broadening effects and signal-to-noise of each technique. This humble setup will hopefully grow into a more robust experimental arrangement in which double resonance, two-laser excitations are used to explore hyperfine state changing collisions between rubidium atoms and noble gas atoms. Rb-noble gas collisions can transfer population between hyperfine levels, such as 5P3/2 (F ′ = 3) Collision ←− 5P3/2 (F ′ = 2), and the probe beam couples 7S1/2 (F ′′ = 2) ← 5P3/2 (F ′ = 3). Polarization spectroscopy signal depends on the rate of population transfer due to the collision as well as maintaining the orientation created by the pump laser. Fluorescence spectroscopy relies only on transfer of population due to the collision. Comparison of these techniques yields information regarding the change of the magnetic sublevels, mF , during hyperfine state changing collisions.
The goal of this experiment was to measure the hyperfine energy splittings of the ground to first excited state transitions in rubidium using saturated absorption spectroscopy. Using this technique, we measured these transition energy spectra by taking the difference of two photodiode outputs due to multiple beams of a single laser scanned over a range of frequencies and shone through a cell of Rb vapor. When the laser frequency was resonant with an atomic transition, photons of those frequencies were absorbed, leaving a dip in intensity of the beam measured at the photodiode. One of the two laser beams had its excitations saturated by a more intense, counter-propagating pump beam from the same laser. The pump beam saturated the absorption of the velocity equal zero atoms that the counter-propagating probe beam could have also interacted with due to no Doppler shift. At these frequencies the probe beam experienced less absorption that was measured by a photodiode. The photodiode output was calibrated to the change in frequency of the scanned laser using a Fabry-Pérot interferometer. The output of this interferometer served as a reference for how the laser frequency changed. Final results for the 87Rb F=1 spectrum accounted for the largest error with a maximum of 12.2% deviation from accepted energy spacing values due in part to systematic error. Other spectra measurements were in better agreement, possessing error ranging from 2.1% to 10.1% and some agreeing with accepted values to within our uncertainty.
The two-photon transition $5S\ensuremath{-}5P\ensuremath{-}5D$ in rubidium vapor is investigated by detecting the fluorescence from the 6P3/26{P}_{3/2}6P3/2​ state when the atomic system is excited by the combined action of a cw diode laser and a frequency comb. The cw laser plays a role as a velocity-selective filter and allows for sub-Doppler spectroscopy over a large spectral range including the 5D3/25{D}_{3/2}5D3/2​ and 5D5/25{D}_{5/2}5D5/2​ states. For a counterpropagating beam configuration, the response of each atomic velocity group is well characterized within the Doppler profile and the excited hyperfine levels are clearly resolved. The contribution of the optical pumping to the direct two-photon process is also revealed. The results are well described in a frequency domain picture by considering the interaction of each velocity group with the cw laser and the modes of the frequency comb.
Absorption spectra of cold rubidium atoms in an integrating sphere under the influence of a diffuse laser field have been systematically investigated. A pronounced dispersionlike structure centered at the light-shifted pump frequency is observed with a subnatural linewidth. In particular, two clearly resolved absorption resonances on the $5{S}_{1/2}(F=2)\ensuremath{\rightarrow}5{P}_{3/2}({F}^{\ensuremath{'}}=3)$ transitions occur with variable probe beam intensity, which is consistent with our proposed theoretical model. Based on the two absorption resonances,we measure the dependence of light shifts, from which we can directly extract the effective Rabi frequency in a diffuse laser field, on the probe laser intensity, pump laser intensity, and pump laser detuning. Our work helps to identify the physical mechanisms behind these spectral features and is beneficial for studying the corresponding effect in a cold sample.
In this paper the saturation spectra of rubidium vapour at room temperature, obtained with overlapped co-propagating laser beams, were examined. Unlike the standard saturation spectroscopy, here the transmission of the pump laser beam was detected. The pump laser was locked to an atomic transition of the D2 line, while the probe laser frequency was scanned in a wide frequency range. The pump and probe beams had approximately the same intensities; thus the probe laser can saturate transitions and contribute to optical pumping. This, together with Doppler broadening, leads to rich pump transmission spectra, with many lines appearing due to the interaction of lasers with atoms in different velocity groups. The advantages of this method are well-resolved structures and appearance of spectral lines on a flat, Doppler-free background. Agreement between experimental and theoretical results shows the usefulness of this simple model, based on the rate equations, for identification of lines and determination of relative contribution to the observed line intensity from atoms with different velocities. Theoretical spectra are a useful tool for the calibration of experimental spectra obtained by a nonlinear dependence of the laser frequency on the voltage applied to the piezo used for the laser diode frequency scanning.
A scheme of Doppler-free spectroscopy is experimentally demonstrated with a co-propagating control laser locking to an atomic hyperfine transition, and the differential transmission of the probe and the reference laser is detected. Crossover resonances are eliminated by selecting the class of atoms with zero velocity in the direction of beam propagation. In addition, the sub-Doppler spectrum experiences optical gain compared to the conventional saturated-absorption spectrum as a result of optical pumping.