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Physical Review A

High-precision measurement of lifetimes and collisional decay parameters in Ca D1 states using the two-photon Hanle effect

L. R. Hunter, G. M. Watson, David S. Weiss, Arthur Zajonc

Published Apr 1, 1985• 20 citations
Publisher

Abstract

We report high-precision measurements of the lifetimes and collisional decay parameters of the (4${p}^{2}$) ${\mathrm{}}^{1}$D and (4s5d) ${\mathrm{}}^{1}$D states of atomic calcium using the two-photon Hanle effect. Modification of the excited-state decay rates due to saturation of the two-photon transition is clearly observed. Spontaneous-emission rates of the possible dipole transitions from these states are deduced through branching-ratio measurements and compared with theory. The (4s4d${)\mathrm{}}^{1}$D lifetime is determined through observation of its exponential decay.

DOI
10.1103/physreva.31.2268

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We present a high-precision measurement of the $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}$--state lifetime in a single trapped $^{40}\mathrm{Ca}^{+}$. The measurement was performed using a high-efficiency quantum-state detection technique to monitor quantum jumps and a high-precision and highly synchronous measurement sequence for laser control. A feature in our measurement is the pumping rate of the 729-nm laser that was corrected in a real-time way. The $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}$--state lifetime was obtained through the measurement of the spontaneous decay rate after incoherent shelving of the ion to the $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}$ state with a wait time. Systematic errors, such as collisions with background gases, heating effects, impurity components, the shelving and pumping rates, and state detection, were carefully analyzed and estimated. We determined an improved value of the $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}$--state lifetime to be ${\ensuremath{\tau}}_{3/2}=1.195(8)$ s. Furthermore, the $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}\ensuremath{\rightarrow}4s\phantom{\rule{4pt}{0ex}}^{2}S_{1/2}$ quadrupole transition matrix element was measured to be ${S}_{ki}=7.936(26)e{a}_{0}^{2}$, and the ratio between the lifetimes of $3d{\phantom{\rule{4pt}{0ex}}}^{2}{D}_{3/2}$ and $3d{\phantom{\rule{4pt}{0ex}}}^{2}{D}_{5/2}$ was determined to be 1.018(11). Our method can be universally applied to lifetime measurements of other single ions and atoms with a similar structure.

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The lifetime of the ${\mathrm{Ca}}^{+}$ $4^{2}P_{\frac{3}{2}}$ state and that of the ${\mathrm{Mg}}^{+}$ $3^{2}P_{\frac{3}{2}}$ state have been measured by the Hanle-effect method with optical excitation from the ground states of the ions. The lifetimes are, respectively, (6.72\ifmmode\pm\else\textpm\fi{}0.20)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}9}$ and (3.67\ifmmode\pm\else\textpm\fi{}0.18)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}9}$ sec. The ions were produced by introducing traces of calcium or magnesium into an argon discharge. "Alignment" depolarization cross sections $\ensuremath{\sigma}$ were obtained for the collisional depolarization of the following states of calcium and magnesium due to collisions with argon: $\ensuremath{\sigma}(\mathrm{Ca} 4^{1}P_{1} \mathrm{state})=(1.9\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}({\mathrm{Ca}}^{+} 4^{2}P_{\frac{3}{2}} \mathrm{state})=(1.4\ifmmode\pm\else\textpm\fi{}0.2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}(\mathrm{Mg} 3^{1}P_{1} \mathrm{state})=(1.9\ifmmode\pm\else\textpm\fi{}0.3){10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}({\mathrm{Mg}}^{+} 3^{2}P_{\frac{3}{2}} \mathrm{state})=(1.3\ifmmode\pm\else\textpm\fi{}0.25)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2}.$The magnitudes of these cross sections are in accord with the theories of Byron and Foley and of Omont; we give a discussion of the extension of these theories to include ion-atom collisions.

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Direct measurement of the 3 d 2 D 3 / 2 to 3 d 2 D 5 / 2 lifetime ratio in a single trapped 40 Ca +

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Abstract We present for the first time a direct measurement of the lifetime ratio between the 3 d 2 D 3 / 2 and 3 d 2 D 5 / 2 metastable states in a single trapped 40 Ca + . A high-efficiency quantum state detection technique is adopted to monitor the quantum jumps, and a high precision and synchronized measurement sequence is used for laser control to study the rule of spontaneous decay. Our method shows that the lifetime ratio is a constant and is irrelevant to the dwell time; it is only determined by the spontaneous decay probabilities of the two metastable states at one random decay time, independent of the lifetimes of the two metastable states. Systematic errors such as collisions with background gases, heating effects, impurity components, the shelving and pumping rates and the photon counts are analyzed, and the lifetime ratio between the 3 d 2 D 3 / 2 and 3 d 2 D 5 / 2 states is directly measured to be 1.0257(43) with an uncertainty of 0.42%. Our result is in good agreement with the most precise many-body atomic structure calculations. Our method can be used to obtain the lifetime of a state which is usually difficult to measure and can be used to determine the magnetic dipole transition matrix elements in heavy ions such as Ba + and Ra + , and can also be universally applied to lifetime ratio measurements of other single atoms and ions with a similar structure.

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Experimental and theoretical study of the 3 d D 2 –level lifetimes of Ca + 40

Axel Kreuter, Christoph Becher, Gavin P. T. Lancaster +8 more

We report measurements of the lifetimes of the $3d\phantom{\rule{0.3em}{0ex}}^{2}D_{5∕2}$ and $3d\phantom{\rule{0.3em}{0ex}}^{2}D_{3∕2}$ metastable states of a single laser-cooled $^{40}\mathrm{Ca}^{+}$ ion in a linear Paul trap. We introduce a measurement technique based on high-efficiency quantum state detection after coherent excitation to the ${D}_{5∕2}$ state or incoherent shelving in the ${D}_{3∕2}$ state, and subsequent free, unperturbed spontaneous decay. The result for the natural lifetime of the ${D}_{5∕2}$ state of 1168(9) ms agrees excellently with the most precise published value. The lifetime of the ${D}_{3∕2}$ state is measured with a single ion and yields 1176(11) ms which improves the statistical uncertainty of previous results by a factor of four. We compare these experimental lifetimes to high-precision ab initio all order calculations [${D}_{3∕2}$ state: 1196(11) ms; ${D}_{5∕2}$ state: 1165(11) ms] and find a very good agreement. These calculations represent an excellent test of high-precision atomic theory and will serve as a benchmark for the study of parity nonconservation in ${\mathrm{Ba}}^{+}$ which has similar atomic structure.

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Kinetic study of Ca(4 3 PJ) by time-resolved emission, 4 3 P 1 → 4 1 S 0 +hν(λ= 657.3 nm), following dye-laser excitation. Spontaneous emission, diffusion and collisional quenching

David Husain, José Schifino

We present a kinetic study of the low-lying electronically excited state of atomic calcium, Ca[4s4p(3PJ)], 1.885 eV above the 4s2(1S0) ground state. Ca(4 3P1) was generated by dye-laser pulsed excitation at λ= 657.3 nm of calcium vapour [Ca(4 3P1)â†� Ca(4 1S0)] at elevated temperatures (1000 K), in equilibrium with solid calcium, in a slow-flow system, kinetically equivalent to a static system. Following rapid Boltzmann equilibration within Ca(4 3PJ) through collisions, the forbidden time-resolved atomic resonance fluorescence at the same wavelength was monitored using boxcar integration. The decay of Ca(4 3PJ) in the presence of all the noble gases, He, Ne, Ar, Kr and Xe, was studied, yielding measurements of relative diffusion coefficients. Extrapolation of the diffusional component of the decay in each noble gas to infinite pressure yields an independent value of the mean radiative lifetime for Ca(4 3P1)→ Ca(4 1S0)+hν(λ= 657.3 nm), the average of which from the measurements in all the noble gases yields τe= 0.34 ± 0.02 ms (error 2σ). This result is compared with values reported from previous measurements, particularly atomic beams and time-resolved measurements. The kinetic analysis also gives rise to data for the collisional quenching of Ca(4 3PJ), which is found to be insignificant for most of the noble gases [kHe,Ne,Ar,Kr⩽ 4 × 10–15 cm3 molecule–1 s–1(1000 K)], in contrast to measurements from earlier work using phase-shift techniques. Xenon, however, exhibited measurable rates of collisional quenching of Ca(4 3PJ) characterised by kXe= 2.4 ± 0.3 × 10–14 cm3 molecule–1 s–1(1000 K). The time-resolved emission technique is further applied to the study of the removal of Ca(4 3PJ) by added gases, for which we report (errors 1σ)kN2=(8.9 ± 0.9)× 10–13 cm3 molecule–1 s–1(1000 K), kH2=(6.0 ± 0.6)× 10–14 cm3 molecule–1 s–1(1000 K), kD2=(2.7 ± 0.3)× 10–14 cm3 molecule–1 s–1(1000 K).

Journal of the Chemical Society Faraday Transactions 2 Molecular and Chemical Physics•Jan 1, 1983•25 citations
We report high-precision measurements of the lifetimes and collisional decay parameters of the (4p2{p}^{2}p2) 1{\mathrm{}}^{1}1D and (4s5d) 1{\mathrm{}}^{1}1D states of atomic calcium using the two-photon Hanle effect. Modification of the excited-state decay rates due to saturation of the two-photon transition is clearly observed. Spontaneous-emission rates of the possible dipole transitions from these states are deduced through branching-ratio measurements and compared with theory. The (4s4d)1{)\mathrm{}}^{1})1D lifetime is determined through observation of its exponential decay.
We present a high-precision measurement of the 3d2D3/23d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}3d2D3/2​--state lifetime in a single trapped 40Ca+^{40}\mathrm{Ca}^{+}40Ca+. The measurement was performed using a high-efficiency quantum-state detection technique to monitor quantum jumps and a high-precision and highly synchronous measurement sequence for laser control. A feature in our measurement is the pumping rate of the 729-nm laser that was corrected in a real-time way. The 3d2D3/23d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}3d2D3/2​--state lifetime was obtained through the measurement of the spontaneous decay rate after incoherent shelving of the ion to the 3d2D3/23d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}3d2D3/2​ state with a wait time. Systematic errors, such as collisions with background gases, heating effects, impurity components, the shelving and pumping rates, and state detection, were carefully analyzed and estimated. We determined an improved value of the 3d2D3/23d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}3d2D3/2​--state lifetime to be ${\ensuremath{\tau}}_{3/2}=1.195(8)$ s. Furthermore, the $3d\phantom{\rule{4pt}{0ex}}^{2}D_{3/2}\ensuremath{\rightarrow}4s\phantom{\rule{4pt}{0ex}}^{2}S_{1/2}$ quadrupole transition matrix element was measured to be Ski=7.936(26)ea02{S}_{ki}=7.936(26)e{a}_{0}^{2}Ski​=7.936(26)ea02​, and the ratio between the lifetimes of 3d2D3/23d{\phantom{\rule{4pt}{0ex}}}^{2}{D}_{3/2}3d2D3/2​ and 3d2D5/23d{\phantom{\rule{4pt}{0ex}}}^{2}{D}_{5/2}3d2D5/2​ was determined to be 1.018(11). Our method can be universally applied to lifetime measurements of other single ions and atoms with a similar structure.
The lifetime of the Ca+{\mathrm{Ca}}^{+}Ca+ 42P324^{2}P_{\frac{3}{2}}42P23​​ state and that of the Mg+{\mathrm{Mg}}^{+}Mg+ 32P323^{2}P_{\frac{3}{2}}32P23​​ state have been measured by the Hanle-effect method with optical excitation from the ground states of the ions. The lifetimes are, respectively, (6.72\ifmmode\pm\else\textpm\fi{}0.20)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}9}$ and (3.67\ifmmode\pm\else\textpm\fi{}0.18)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}9}$ sec. The ions were produced by introducing traces of calcium or magnesium into an argon discharge. "Alignment" depolarization cross sections $\ensuremath{\sigma}$ were obtained for the collisional depolarization of the following states of calcium and magnesium due to collisions with argon: $\ensuremath{\sigma}(\mathrm{Ca} 4^{1}P_{1} \mathrm{state})=(1.9\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}({\mathrm{Ca}}^{+} 4^{2}P_{\frac{3}{2}} \mathrm{state})=(1.4\ifmmode\pm\else\textpm\fi{}0.2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}(\mathrm{Mg} 3^{1}P_{1} \mathrm{state})=(1.9\ifmmode\pm\else\textpm\fi{}0.3){10}^{\ensuremath{-}14}{\mathrm{cm}}^{2};$ $\ensuremath{\sigma}({\mathrm{Mg}}^{+} 3^{2}P_{\frac{3}{2}} \mathrm{state})=(1.3\ifmmode\pm\else\textpm\fi{}0.25)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}{\mathrm{cm}}^{2}.$The magnitudes of these cross sections are in accord with the theories of Byron and Foley and of Omont; we give a discussion of the extension of these theories to include ion-atom collisions.
The lifetimes of the 5p2P325p^{2}P_{\frac{3}{2}}5p2P23​​ and 5p2P125p^{2}P_{\frac{1}{2}}5p2P21​​ states of Sr+{\mathrm{Sr}}^{+}Sr+ and the 6p2P326p^{2}P_{\frac{3}{2}}6p2P23​​ and 6p2P126p^{2}P_{\frac{1}{2}}6p2P21​​ states of Ba+{\mathrm{Ba}}^{+}Ba+ have been measured by the Hanle-effect technique with optical excitation from the ion ground state. (The lifetimes of the Mg+{\mathrm{Mg}}^{+}Mg+ 3p2P323p^{2}P_{\frac{3}{2}}3p2P23​​ and Ca+{\mathrm{Ca}}^{+}Ca+ 4p2P324p^{2}P_{\frac{3}{2}}4p2P23​​ states were obtained by the same technique and reported previously.) These Ca+{\mathrm{Ca}}^{+}Ca+, Sr+{\mathrm{Sr}}^{+}Sr+, and Ba+{\mathrm{Ba}}^{+}Ba+ states each decay to a 2D32,52^{2}D_{\frac{3}{2},\frac{5}{2}}2D23​,25​​ doublet as well as to the ground 2S12^{2}S_{\frac{1}{2}}2S21​​ state, and the branching ratios for these transitions have been measured. The ions were produced by introducing traces of the atomic vapor into an argon discharge. Consequently, the cross sections for collisional depolarization of these 2PJ^{2}P_{J}2PJ​ states due to collisions with argon were also obtained from the measurements. The experimental results are given in Tables I and II. A discussion of the ion-atom collisional depolarization cross sections is included.
Abstract We present for the first time a direct measurement of the lifetime ratio between the 3 d 2 D 3 / 2 and 3 d 2 D 5 / 2 metastable states in a single trapped 40 Ca + . A high-efficiency quantum state detection technique is adopted to monitor the quantum jumps, and a high precision and synchronized measurement sequence is used for laser control to study the rule of spontaneous decay. Our method shows that the lifetime ratio is a constant and is irrelevant to the dwell time; it is only determined by the spontaneous decay probabilities of the two metastable states at one random decay time, independent of the lifetimes of the two metastable states. Systematic errors such as collisions with background gases, heating effects, impurity components, the shelving and pumping rates and the photon counts are analyzed, and the lifetime ratio between the 3 d 2 D 3 / 2 and 3 d 2 D 5 / 2 states is directly measured to be 1.0257(43) with an uncertainty of 0.42%. Our result is in good agreement with the most precise many-body atomic structure calculations. Our method can be used to obtain the lifetime of a state which is usually difficult to measure and can be used to determine the magnetic dipole transition matrix elements in heavy ions such as Ba + and Ra + , and can also be universally applied to lifetime ratio measurements of other single atoms and ions with a similar structure.
We report measurements of the lifetimes of the 3d2D5∕23d\phantom{\rule{0.3em}{0ex}}^{2}D_{5∕2}3d2D5∕2​ and 3d2D3∕23d\phantom{\rule{0.3em}{0ex}}^{2}D_{3∕2}3d2D3∕2​ metastable states of a single laser-cooled 40Ca+^{40}\mathrm{Ca}^{+}40Ca+ ion in a linear Paul trap. We introduce a measurement technique based on high-efficiency quantum state detection after coherent excitation to the D5∕2{D}_{5∕2}D5∕2​ state or incoherent shelving in the D3∕2{D}_{3∕2}D3∕2​ state, and subsequent free, unperturbed spontaneous decay. The result for the natural lifetime of the D5∕2{D}_{5∕2}D5∕2​ state of 1168(9) ms agrees excellently with the most precise published value. The lifetime of the D3∕2{D}_{3∕2}D3∕2​ state is measured with a single ion and yields 1176(11) ms which improves the statistical uncertainty of previous results by a factor of four. We compare these experimental lifetimes to high-precision ab initio all order calculations [D3∕2{D}_{3∕2}D3∕2​ state: 1196(11) ms; D5∕2{D}_{5∕2}D5∕2​ state: 1165(11) ms] and find a very good agreement. These calculations represent an excellent test of high-precision atomic theory and will serve as a benchmark for the study of parity nonconservation in Ba+{\mathrm{Ba}}^{+}Ba+ which has similar atomic structure.
We present a kinetic study of the low-lying electronically excited state of atomic calcium, Ca[4s4p(3PJ)], 1.885 eV above the 4s2(1S0) ground state. Ca(4 3P1) was generated by dye-laser pulsed excitation at λ= 657.3 nm of calcium vapour [Ca(4 3P1)â†� Ca(4 1S0)] at elevated temperatures (1000 K), in equilibrium with solid calcium, in a slow-flow system, kinetically equivalent to a static system. Following rapid Boltzmann equilibration within Ca(4 3PJ) through collisions, the forbidden time-resolved atomic resonance fluorescence at the same wavelength was monitored using boxcar integration. The decay of Ca(4 3PJ) in the presence of all the noble gases, He, Ne, Ar, Kr and Xe, was studied, yielding measurements of relative diffusion coefficients. Extrapolation of the diffusional component of the decay in each noble gas to infinite pressure yields an independent value of the mean radiative lifetime for Ca(4 3P1)→ Ca(4 1S0)+hν(λ= 657.3 nm), the average of which from the measurements in all the noble gases yields τe= 0.34 ± 0.02 ms (error 2σ). This result is compared with values reported from previous measurements, particularly atomic beams and time-resolved measurements. The kinetic analysis also gives rise to data for the collisional quenching of Ca(4 3PJ), which is found to be insignificant for most of the noble gases [kHe,Ne,Ar,Kr⩽ 4 × 10–15 cm3 molecule–1 s–1(1000 K)], in contrast to measurements from earlier work using phase-shift techniques. Xenon, however, exhibited measurable rates of collisional quenching of Ca(4 3PJ) characterised by kXe= 2.4 ± 0.3 × 10–14 cm3 molecule–1 s–1(1000 K). The time-resolved emission technique is further applied to the study of the removal of Ca(4 3PJ) by added gases, for which we report (errors 1σ)kN2=(8.9 ± 0.9)× 10–13 cm3 molecule–1 s–1(1000 K), kH2=(6.0 ± 0.6)× 10–14 cm3 molecule–1 s–1(1000 K), kD2=(2.7 ± 0.3)× 10–14 cm3 molecule–1 s–1(1000 K).