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Using the inherent timing stability of pulses from a mode-locked laser, we have precisely measured the cesium 6P 3/2 excited state lifetime. An initial pump pulse excites cesium atoms in two counterpropagating atomic beams to the 6P 3/2 level. A subsequent synchronized probe pulse ionizes atoms which remain in the excited state, and the photo-ions are collected and counted. By selecting pump pulses which vary in time with respect to the probe pulses, we obtain a sampling of the excited state population in time, resulting in a lifetime value of 30.462(46) ns. The measurement uncertainty (0.15%) is slightly larger than our previous report of 0.12% [Phys. Rev. A 84, 010501(R) (2011)] due to the inclusion of additional data and systematic errors. In this follow-up paper we present details of the primary systematic errors encountered in the measurement, which include atomic motion within the intensity profiles of the laser beams, quantum beating in the photo-ion signal, and radiation trapping. Improvements to further reduce the experimental uncertainty are also discussed.

Utilizing two-photon excitation in hot Rb vapor we demonstrate the generation of collimated optical fields at 420 and 1324 nm. Input laser beams at 780 and 776 nm enter a heated Rb vapor cell collinear and circularly polarized, driving Rb atoms to the 5D 5∕2 state. Under phase-matching conditions coherence among the 5S 1∕2 → 5P 3∕2 → 5D 5∕2 → 6P 3∕2 transitions produces a blue (420 nm) beam by four-wave mixing. We also observe a forward and backward propagating IR (1324 nm) beam, due to cascading decays through the 6S 1∕2 → 5P 1∕2 states. Power saturation of the generated beams is investigated by scaling the input powers to greater than 200 mW, resulting in a coherent blue beam of 9.1 mW power, almost an order of magnitude larger than previously achieved. We measure the dependences of both beams in relation to the Rb density, the frequency detuning between Rb ground-state hyperfine levels, and the input laser intensities. A wide range of phenomena can be created by exploiting nonlinear optical processes in a dense atomic vapor. Large enhancements of these processes are possible through the generation of quantum coherences among atomic states and include effects, such as electromagnetically induced transparency, fast and slow light propagation, four-wave mixing (FWM), and lasing without inversion. FWM in particular has been shown to produce both efficient frequency upconversion [1-3] and downconversion [4] using low-power continuous-wave (cw) lasers. The newly created optical fields are narrowband tunable coherent light sources [5], with wavelengths from the IR to approaching the UV depending upon the atomic states involved. Frequency upconversion by FWM has most often been studied in Rb vapor, first demonstrated using low-power cw lasers by Zibrov et al. in 2002 [6] where 15 μW of coherent radiation at 420 nm was achieved. The method relies upon input lasers at 780 and 776 nm [see Fig. 1(a)] driving Rb atoms from the 5S 1∕2 ground state to the 5D 5∕2 state by two-photon excitation, with the 5P 3∕2 level as an intermediate state. A third optical field between the 5D 5∕2 → 6P 3∕2 levels at 5.23 μm is initiated through spontaneous emission. Strong atomic coherences are thus formed in a diamond-type energy level structure, creating coherent blue light at 420 nm (6P 3∕2 → 5S 1∕2 ) by FWM. Recent experiments achieved first 40 μW of 420 nm light through the additional coupling of both 5S 1∕2 hyperfine ground-state levels [1], and subsequently 1.1 mW by further optimization of input laser polarizations and frequencies [3]. The generated blue beam exhibits a high degree of spatial coherence [2], with a spectral linewidth typically limited by the linewidths of the applied laser fields [7]. The absolute frequency of the blue light has been found to be centered on the 6P 3∕2 → 5S 1∕2 transition, with tunability of ≥100 MHz possible by adjustment of the input laser frequencies [5]. Incorporating an additional laser at 795 nm has been shown to both enhance and suppress the FWM process through control of optical pumping [8]. ...

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Polarization and relaxation of radon isotopes by spin exchange with laser optically pumped rubidium were studied in preparation for electric dipole moment measurements with octupole deformed 223 Rn. γ -ray anisotropies provided a measure of nuclear polarization produced by spin exchange with laser polarized rubidium vapor, and the temperature dependence over the range 130 to 220 • C was measured to parametrize the spin exchange polarization and the quadrupole-dominated wall relaxation rate. These results provide quantitative data for developing electric dipole moment measurements of octupole-deformed 223 Rn and other radon isotopes.