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Applied Physics Letters

Narrow 87Rb hyperfine-structure resonances in an evacuated wall-coated cell

H. G. Robinson, C. E. Johnson

Published May 1, 1982• 82 citations
Publisher

Abstract

Examination of 87Rb δF = 1, δ‖mF‖ = 1 hyperfine resonances in a 200-cm3 evacuated tetracontane wall-coated Pyrex cell which has been sealed since 1968 shows remarkable Dicke-narrowed sub-Doppler Lorentzian line shapes with less than 11 Hz full width. This linewidth is 70 times narrower than that in buffer gas filled cells used in commercial Rb atomic frequency standards. The phase shift per wall collision is 0.058 radians/collision as derived from an observed wall-induced hyperfine frequency shift of −52 Hz at a wall temperature of 26 °C.

DOI
10.1063/1.93279

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Examination of 87Rb δF = 1, δ‖mF‖ = 1 hyperfine resonances in a 200-cm3 evacuated tetracontane wall-coated Pyrex cell which has been sealed since 1968 shows remarkable Dicke-narrowed sub-Doppler Lorentzian line shapes with less than 11 Hz full width. This linewidth is 70 times narrower than that in buffer gas filled cells used in commercial Rb atomic frequency standards. The phase shift per wall collision is 0.058 radians/collision as derived from an observed wall-induced hyperfine frequency shift of −52 Hz at a wall temperature of 26 °C.
Spectral lineshape narrowing of atomic vapor emission in a bufferless, wall-coated absorption cell has been analyzed using the same formalism developed t3 describe sub-Doppler linewidths. Dicke-narrowing, in a buffered cell. Dramatic linewidth reductions in the bufferless cell, compared to the buffered cell, occur because of the high probability that Doppler shifts before and after a particular wall collision will cancel each other. The formalism described allows more physical insight than the classic onedimensional box model previously invoked to explain spectral narrowing in bufferless, wall coated cells. Additionally, this formalism reveals a correlation between post-collision velocities and intercollision times in the buffered cell resulting in modifications of the standard Dicke analysia of these cells. Finally, the computational power of the technique is demonstrated. The effects of varying cell size on Rb and CS hyperfine lineshapes and the results of the presence of an inhomogeneous magnetic field within the cell are analyzed.
Spectral lineshape narrowing of atomic vapour emission in a bufferless, wall-coated absorption cell has been analysed using the same formalism developed to describe sub-Doppler linewidths, Dicke narrowing, in a buffered cell. Within this formalism lineshapes are generated using Monte Carlo techniques. Dramatic linewidth reductions in the bufferless cell, compared with the buffered cell, occur because of the high probability that Doppler shifts before and after a particular wall collision will cancel each other. The formalism described allows more physical insight than the classic one-dimensional box model previously invoked to explain spectra narrowing in bufferless, wall-coated cells. Additionally, this formalism reveals a correlation between post-collision velocities and intercollision times in the buffered cell resulting in modifications of the standard Dicke analysis of these cells.
An alkene-based antirelaxation coating for alkali-metal vapor cells exhibiting Zeeman relaxation times up to 77 s was recently identified by Balabas et al. The long relaxation times, two orders of magnitude longer than in paraffin- (alkane-) coated cells, motivate revisiting the question of what the mechanism is underlying wall-collision-induced relaxation and renew interest in applications of alkali-metal vapor cells to secondary frequency standards. We measure the width and frequency shift of the ground-state hyperfine $m{}_{F}=0\ensuremath{\rightarrow}m{}_{F}^{\ensuremath{'}}=0$ transition (clock resonance) in vapor cells with 85{}^{85}85Rb and 87{}^{87}87Rb atoms, with an alkene antirelaxation coating. We find that the frequency shift is slightly larger than for paraffin-coated cells and that the Zeeman linewidth scales linearly with the hyperfine frequency shift.
In this paper, we present our studies on double resonance using atomic 87Rb in a wall-coated cell, in view of applications in a laser-pumped Rb atomic frequency standard. We study the systematic clock frequency shifts in a wall-coated cell, such as light shift, microwave power shift [11, 12] and shift due to cell temperature [13] (for the cell body, and for the Rb reservoir, also called the cell stem). We also report on our clock stability measurement using the wallcoated cell in DR scheme, and discuss the influence of the shift parameters first on the frequency stability of the clock.
I studied the effect of wall collisions on the electron paramagnetic resonance (EPR) of gas phase alkali metal atoms (87Rb). Two types of walls were studied: antirelaxation-coated walls and RbH-coated walls. I measured the dwell times of spin polarized Rb atoms on the two most common antirelaxation coatings, octadecyltrichlorosilane (OTS)- and paraffin. I found that at a cell temperature of 72 C the dwell times for OTS- and paraffin-coated walls are 0.9 ± 0.1 μs and 1.8 ± 0.2 μs, respectively. The implication of these dwell times, which are much longer than what was previously reported in the literature, is discussed in connection with the relaxing property of these coatings. In cells coated with RbH salt I made the first observation of the EPR frequency shift of the gas phase 87Rb atoms. Due to collisions with the RbH salt, which was nuclear spin polarized by spin exchange with optically pumped Rb vapor. The measured EPR frequency shifts are of the order of several hundred Hz in a millimeter-sized cell. By measuring the dependence of the EPR frequency shifts on cell length and by comparing the EPR frequency shifts in RbH-coated cells with those in OTS-coated cells, I provided convincing evidence that the observed EPR frequency shifts are due to collisions with RbH-coated walls, and not due to gas phase processes. The EPR frequency shift is due to the Fermi contact interaction between the s-electron of the adsorbed 87Rb atom and the polarized nucleus on the salt surface. The measured EPR frequency shifts allowed me to calculate the ensemble-averaged phase shift experienced by the Rb atom while adsorbed on the walls. Under our experimental condition this is about 70 mrad. My experiment opens up the possibility of studying surface NMR using gas phase EPR. The phase shift is proportional to the surface nuclear polarization, thus provides an interesting method for measuring the surface nuclear polarization using gas phase EPR. My observation will alert the high precision miniature atomic magnetometry community that collisions with cell walls may cause a systematic error and line broadening in the magnetic resonance frequency.
Microwave double resonances were measured in a wall-coated Rb vapor cell as a function of additional buffer-gas pressure. These data were compared with similar measurements in an uncoated cell. It was found that the linewidth in the coated spherical cell of diameter 1.6 cm displays a distinct maximum around 0.2 kPa. This agrees well with theoretical solutions of the diffusion equation, assuming a complex reflection coefficient at the wall. It was also found that at intermediate pressures the lineshapes of the microwave resonances become asymmetric with a low-frequency tail. This agrees with the explanation that where the alkali mean free path is substantially smaller than the average distance between wall collisions at zero pressure, there exist two classes of atoms in the cell. The atoms that get trapped near the walls accumulate much larger phase shifts than those toward the center of the cell. This effect is not seen in the longitudinal relaxation rate, indicating that it is related to a phase-shift effect.