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Physical Review Letters

Radiative Decay Rates in Hg+ from Observations of Quantum Jumps in a Single Ion

Wayne M. Itano, Jonas Bergquist, Randall G. Hulet, David J. Wineland

Published Dec 14, 1987• 117 citations
Publisher

Abstract

Radiative decay rates connecting the lowest four energy levels of $^{198}\mathrm{Hg}^{+}$ have been derived solely from an analysis of the fluctuations (quantum jumps) of the laser-induced fluorescence of the 194-nm first resonance transition of a single ion confined in a Paul trap. The natural linewidth of the 194-nm first resonance transition was also measured. The measured decay rates and branching ratios are in satisfactory agreement with theory.

DOI
10.1103/physrevlett.59.2732

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Radiative decay rates connecting the lowest four energy levels of 198Hg+^{198}\mathrm{Hg}^{+}198Hg+ have been derived solely from an analysis of the fluctuations (quantum jumps) of the laser-induced fluorescence of the 194-nm first resonance transition of a single ion confined in a Paul trap. The natural linewidth of the 194-nm first resonance transition was also measured. The measured decay rates and branching ratios are in satisfactory agreement with theory.
We have used stored ion methods to improve resolution and sensitivity in optical spectroscopy. Single atomic ions have been confined by electric and magnetic fields, cooled by laser radiation pressure to temperatures on the order of 1 mK, and probed spectroscopically with narrowband lasers. The absorption resonance of a single Hg + ion has been observed by a decrease in the transmitted light intensity. An ultraviolet transition in Hg + has been observed with a linewidth of only 30 kHz. Quantum jumps to and from metastable levels of Hg + have been observed and used to determine radiative decay rates and to infer the existence of photon antibunching. Quantum jumps have also been observed in single Mg + ions.
Measurements are reported of the fundamental mode radiative decay rate of the Hg 6 1P1^{1}P_{1}1P1​ population under conditions of low collision rate and large optical thickness of the 184.9-nm resonance line. The measured data extend over a wide range of experimental conditions. The measurements were made using two different experimental methods, both employing low-pressure mercury--noble-gas discharges. In the first method the decay rate of the 6 1P1^{1}P_{1}1P1​ population was measured in the afterglow of the discharge using a dye-laser absorption technique. In the second one the decay was measured of the laser-induced fluorescence at the 184.9-nm line created by pulsed optical pumping. Radiative decay rates obtained with the two independent experimental methods for nominally the same conditions agreed within the experimental error of 5%. For zero perturber gas density the radiative decay rate as a function of the Hg density shows a pronounced minimum. This minimum disappears with the addition of an argon density of more than about 3\ifmmode\times\else\texttimes\fi{}1022{10}^{22}1022 ${\mathrm{m}}^{\mathrm{\ensuremath{-}}3}$, which corresponds with an extra collisional broadening of \ensuremath{\sim}15 MHz. The experimental decay rates differ largely from rates calculated with a complete frequency redistribution theory. Comparison with rates calculated from the partial redistribution theory described in paper I (preceding paper) shows agreement within 25%. The behavior of the experimental rates at the lowest mercury densities could be interpreted as due to a deviation from the natural abundance in the 6 1P1^{1}P_{1}1P1​ excited-state population.
We detect the radiatively driven electric quadrupole transition to the metastable 2D52^{2}D_{\frac{5}{2}}2D25​​ state in a single, laser-cooled Hg II ion by monitoring the abrupt cessation of the fluorescence signal from the laser-excited $^{2}S_{\frac{1}{2}}\ensuremath{\rightarrow}^{2}P_{\frac{1}{2}}$ first resonance line. When the ion "jumps" back from the metastable DDD state to the ground SSS state, the $S\ensuremath{\rightarrow}P$ resonance fluorescence signal immediately returns. The statistical properties of the quantum jumps are investigated; for example, photon antibunching in the emission from the DDD state is observed with 100% efficiency.
The decay rate of the Hg 61P1 level was measured as a function of cold spot temperature (Hg density) and buffer gas pressure in cylindrical, sealed fused silica cells. The decay rates were obtained using a time-resolved laser-induced 185 nm fluorescence experiment with multi-step excitation. Cold spot temperatures from 25 to 100 °C were studied. The Hg densities for this temperature range and with no buffer gas yield the lowest possible decay rates due to radiation trapping with partial frequency redistribution. Decay rates with argon buffer gas pressures of 3 and 30 Torr were also studied. The results are in agreement with published data from a discharge afterglow experiment. Monte Carlo simulations of radiation transport in the cells, including the effects of hyperfine and isotope structure, the effects of foreign gas broadening, and partial frequency redistribution are compared to the experimental data. Reasonably good agreement is obtained, however there is evidence of quenching of Hg 61P1 atoms in collisions with ground state Hg and Ar atoms. An analytic formula for the fundamental mode trapped decay rate of the 61P1 level, which is applicable over a substantial region of parameter space, was devised from the Monte Carlo results.
Measurements are reported of the radiative decay rate of the Hg 6 1{\mathrm{}}^{1}1P1{P}_{1}P1​ population under conditions of strong radiation trapping at the 184.9-nm resonance line. The experiments were made in the afterglow of a low-pressure Hg discharge with a dye-laser absorption method. The radiative decay rate as a function of the Hg pressure shows a pronounced minimum. The value at minimum is lower than the limiting value at higher Hg densities by a factor of 2. Furthermore, the experimental rates are up to a factor of 8 lower than those calculated from theory with the usual assumption of complete redistribution. Indeed, complete redistribution is not expected in the present case, where the optical thickness is large and elastic collision rates are smaller than the single atom spontaneous emission rate. We derived an analytical expression for the fundamental-mode radiative decay rate in a homogeneous medium from a theory based on partial redistribution in frequency. A condition for the existence of a fundamental mode is discussed and is shown to be largely satisfied in our experiments. The expression for the decay rate was obtained for a resonance line with a hyperfine structure, and was elaborated for a cylindrical geometry. The resulting calculated decay rates agree with the experimental ones within 25%.