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Chinese Physics Letters

Cs 5D5/2–6F728 nm Laser Spectroscopy with Single Pumping Laser

Qi Zhou, Pengyuan Chang, Zhongzheng Liu, Xiaogang Zhang, Chuanwen Zhu, Jingbiao Chen

Published Mar 1, 2017• 3 citations
Publisher

Abstract

The sub-Doppler absorption laser spectroscopy at 728 nm transition from the 5 D 5 / 2 state to the 6 F state of cesium with linewidth near 10 MHz is first experimentally performed with indirect pumping from the ground state 6 S 1 / 2 to the state 7 P 3 / 2 by a 455.5 nm diode laser. Using a 455.5 nm diode laser as an indirect pump laser, several excited states will be populated due to spontaneous decay from the 7 P state. We first implement the sub-Doppler absorption laser spectroscopy at 728 nm from the 5 D 5 / 2 state to the 6 F state when Cs atoms within thermal glass cell decay to the 5 D 5 / 2 state. Due to velocity transfer effect, the hyperfine structure of 5 D 5 / 2 shows a mixed and complicated pattern but very clear structure when the 455.5 nm pumping laser is counter-propagating (or co-propagating) with the 728 nm probing laser.

DOI
10.1088/0256-307x/34/3/034208

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The sub-Doppler absorption laser spectroscopy at 728 nm transition from the 5 D 5 / 2 state to the 6 F state of cesium with linewidth near 10 MHz is first experimentally performed with indirect pumping from the ground state 6 S 1 / 2 to the state 7 P 3 / 2 by a 455.5 nm diode laser. Using a 455.5 nm diode laser as an indirect pump laser, several excited states will be populated due to spontaneous decay from the 7 P state. We first implement the sub-Doppler absorption laser spectroscopy at 728 nm from the 5 D 5 / 2 state to the 6 F state when Cs atoms within thermal glass cell decay to the 5 D 5 / 2 state. Due to velocity transfer effect, the hyperfine structure of 5 D 5 / 2 shows a mixed and complicated pattern but very clear structure when the 455.5 nm pumping laser is counter-propagating (or co-propagating) with the 728 nm probing laser.
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 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.
The excited state population distribution created by 6S1/2 --> 6P3/2 laser excitation in room temperature cesium vapor mixed with Ar was quantitatively analyzed applying absorption and saturation spectroscopy. A simple method for the determination of the excited state population in a single excitation step based on the measurements of the saturated and unsaturated absorption coefficients was tested. When the line profile is nearly pure Doppler and the laser linewidth is much smaller than the inhomogeneous linewidth but comparable with homogeneous linewidth, the fraction N(v(z)) of the atoms in the ground state that are able to absorb under inhomogeneous broadening conditions can be determined. The transmission of the medium in the center of the Doppler envelope of the strong h. f. component of the CsD2 line due to hyperfine pumping alone amounts to approximately 5%. The assumption that has been made is that the lower-state hyperfine levels are populated in a statistical ratio. The absorption coefficients were measured for a series of P852 powers between 20 microW and 2. 5 mW. The velocity selective population density in the 6P3/2 state was obtained. The population in the 6P3/2 level obtained from the saturation measurements was also determined by the absorption measurement of narrow spectral line from a Cs hollow cathode lamp. The agreement between the results obtained in these two ways is very good. It was shown that 5% of the ground state population could be transferred to the first excited state by pumping the Doppler broadened line with a single-mode narrow-band laser. The argon caused line broadening and therefore increased the effective pumping rate in the first excitation step. The dependence of the 852 nm line fluorescence intensity was plotted against the population in the 6P3/2 level determined from the saturation absorption. This can serve as confirmation of the reliability of the method used for the determination of the excited state population.
Two-color polarization spectroscopy (TCPS) of cesium 6S1/2-6P3/2-8S1/2 (852.3 nm + 794.6 nm) ladder-type system in a room-temperature vapor cell are investigated. The frequency of 852.3 nm laser used as a pump beam is locked on one of the hyperfine transitions between the ground state 6S1/2 and excited state 6P3/2 by the saturated absorption spectroscopy technique, which can populate some atoms on the 6P3/2 excited state and induce anisotropy in the atomic medium. The frequency of 794.6 nm laser serving as a probe beam is scanned across the whole 6P3/2→8S1/2 transition to ascertain this anisotropy, and thus the TCPS is obtained. In experiment, we measure and analyse the influence of frequency detuning of 852.3 nm pump laser on TCPS, and especially reveal that some of hyperfine energy levels of intermediate excited state 6P3/2, which has no direct interaction with the 852.3 nm pump laser, are also populated by a small fraction of atoms with a specific speed in the direction of pump laser beam due to Doppler effect, so they also have contribution to the TCPS when the 794.6 nm probe laser is scanned to the resonance transition line between the 6P3/2 and 8S1/2 states after the Doppler frequency shift has been considered. In addition, we prove that the atomic coherence like electromagnetically induced transparency effect obviously results in a narrower line width of TCPS in the case of counter-propagating experimental configuration than that in the case of pump beam co-propagating with the probe beam in the Cs vapor cell. Finally, we apply the TCPS with dispersive shaped feature to frequency stabilization with no modulation, and the frequency fluctuations of 794.6 nm laser are ～0.5 MHz and ～9.2 MHz for the frequency-locking and free running in ～225 s, respectively. The above research work is expected to play a role in precisely measuring the atomic energy level structure and its related hyperfine structure constant (magnetic dipole and electric quadrupole coupling constants), and also in stabilizing the laser frequency to the excited state transition especially for the optical fiber communication, two-color laser cooling/trapping neutral atoms, optical filter, etc.
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.
We propose and demonstrate pump-probe spectroscopy of rubidium absorption that reveals the sub-Doppler hyperfine structure of the ${}^{5}{\mathrm{S}}_{1/2}\ensuremath{\leftrightarrow}{}^{5}{\mathrm{P}}_{3/2}$ (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.