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Physical Review Letters

Hyperfine Structures of Optically Inaccessible Excited Atomic States

Sharon Chang, R. Gupta, W. Happer

Published Oct 18, 1971• 29 citations
Publisher

Abstract

Cascade transitions have been used to produce polarized atoms in optically inaccessible excited states. The polarized fluorescent light which is emitted when the atoms decay can be used to measure hyperfine structures, lifetimes, and other atomic parameters of these inaccessible states. Preliminary measurements of the hyperfine interval for the second excited $S$ states of ${\mathrm{K}}^{39}$, ${\mathrm{Rb}}^{85}$, ${\mathrm{Rb}}^{87}$, and ${\mathrm{Cs}}^{133}$ are (in MHz) 46(2), 271(15), 565(40), and 684(50), respectively. To our knowledge, these are the first measurements of excited $S$-state hyperfine intervals in alkali atoms.

DOI
10.1103/physrevlett.27.1036

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Hyperfine structure and lifetime measurements of the second-excited D states of rubidium and cesium by cascade fluorescence spectroscopy

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The hyperfine structure of the second-excited $D$ states of $^{85}\mathrm{Rb}$, $^{85}\mathrm{Rb}$, and $^{133}\mathrm{Cs}$ has been measured by the method of cascade-radio-frequency spectroscopy and cascade-level crossing. The sign of the magnetic-dipole coupling constant $A$ is determined by the method of cascade-decoupling and cascade-radio-frequency spectroscopy with narrow-band excitation. Lifetimes $\ensuremath{\tau}$ of some of these states are measured by the cascade-Hanle effect. We find that for $^{87}\mathrm{Rb}$, $A(5^{2}D_{\frac{3}{2}})=14.43\ifmmode\pm\else\textpm\fi{}0.23$ MHz, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}7.44\ifmmode\pm\else\textpm\fi{}0.10$ MHz, $\ensuremath{\tau}(5^{2}D_{\frac{3}{2}})=205\ifmmode\pm\else\textpm\fi{}40$ nsec; for $^{85}\mathrm{Rb}$, $A(5^{2}D_{\frac{3}{2}})=4.18\ifmmode\pm\else\textpm\fi{}0.20$ MHz, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}2.12\ifmmode\pm\else\textpm\fi{}0.20$ MHz; for $^{133}\mathrm{Cs}$, $A(6^{2}D_{\frac{3}{2}})=16.30\ifmmode\pm\else\textpm\fi{}0.15$ MHz, $A(6^{2}D_{\frac{5}{2}})=\ensuremath{-}3.6\ifmmode\pm\else\textpm\fi{}1.0$ MHz, $\ensuremath{\tau}(6^{2}D_{\frac{3}{2}})=57\ifmmode\pm\else\textpm\fi{}15$ nsec.

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Cascade Radio-Frequency Spectroscopy of Excited S and D States of Rubidium; Anomalous D -State Hyperfine Structure

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We report the first successful measurements by cascade radio-frequency spectroscopy of the hyperfine structures of excited $S$ and $D$ states of rubidium. We obtain the following magnetic dipole coupling constants (in MHz): for ${\mathrm{Rb}}^{87}$, $A(7^{2}S_{\frac{1}{2}})=312.5\ifmmode\pm\else\textpm\fi{}3.5$, $A(5^{2}D_{\frac{3}{2}})=14.1\ifmmode\pm\else\textpm\fi{}0.5$, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}8.0\ifmmode\pm\else\textpm\fi{}1.5$; for ${\mathrm{Rb}}^{85}$, $A(7^{2}S_{\frac{1}{2}})=92.6\ifmmode\pm\else\textpm\fi{}1.0$, $A(5^{2}D_{\frac{3}{2}})=4.1\ifmmode\pm\else\textpm\fi{}0.5$. The anomalous, negative value of $A$ for the $5^{2}D_{\frac{5}{2}}$ state may be related to the anomalously small fine-structure interval of the $5D$ state of rubidium.

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Hyperfine-structure investigation of highly excited D2 levels in Rb87 and Cs133 using a cw tunable dye laser in a two-step excitation scheme

Sune R. Svanberg, Pericles G. Tsekeris

The hyperfine structure of several highly excited $^{2}D$ states in $^{87}\mathrm{Rb}$ and $^{133}\mathrm{Cs}$ has been measured. The $D$-state atoms were produced in a two-step-excitation process. In the first step, multiple scattering of the strong alkali-metal ${D}_{1}$ and ${D}_{2}$ lines from an rf lamp was used to excite atoms into the first excited $^{2}P$ levels. The intense tunable radiation from a cw dye laser was used in the second step to transfer $P$-state atoms into highly excited $D$ states. Level-crossing and optical-double-resonance techniques were used for the determination of the absolute values of the hyperfine-interaction constants. The following results (in MHz) were obtained for the magnetic dipole and the electric quadrupole interaction constants $a$ and $b$: For $^{87}\mathrm{Rb}$, $|a(6^{2}D_{\frac{3}{2}})|=7.84(5)$, $|b(6^{2}D_{\frac{3}{2}})|=0.53(6)$ ($\frac{b}{a}>0$), $|a(^{2}D_{\frac{5}{2}})|=3.6(7)$, $|a(7^{2}D_{\frac{3}{2}})|=4.53(3)$, $|b(7^{2}D_{\frac{3}{2}})|=0.26(4)$ ($\frac{b}{a}>0$), $|a(7^{2}D_{\frac{5}{2}})|=2.2(5)$. For $^{133}\mathrm{Cs}$, $|a(8^{2}D_{\frac{3}{2}})|=3.98(8)$, $|a(8^{2}D_{\frac{5}{2}})|=0.9(4)$, $|a(9^{2}D_{\frac{3}{2}})|=2.37(3)$, $|a(9^{2}D_{\frac{5}{2}})|=0.5(2)$, $|a(10^{2}D_{\frac{3}{2}})|=1.52(3)$, $|a(10^{2}D_{\frac{5}{2}})|=0.4(2)$. The $a$ factors generally deviate strongly from the values expected in a one-electron picture of the alkali-metal atom indicating the importance of polarization and correlation effects for these states. For $^{87}\mathrm{Rb}$ a comparison with a recent calculation including polarization effects is made. The $b$ factors for $^{87}\mathrm{Rb}$ are the first significant values allowing a calculation of an alkali-metal-atom nuclear quadrupole moment from non-$P$-state data.

Physical Review A•Apr 1, 1975•46 citations

Optical Methods of Atomic Orientation and of Magnetic Resonance*

Alfred Kastler

In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.

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Hyperfine-Structure Studies of Highly Excited D and F Levels in Alkali Atoms Using a cw Tunable Dye Laser

Sune R. Svanberg, Pericles G. Tsekeris, W. Happer

Highly excited $S$, $D$, and $F$ levels in cesium and rubidium have been populated utilizing a two-step optical excitation method. In the first step an rf lamp is used to transfer atoms into the first $P$ states, and the subsequent excitation is performed with the tunable radiation of a cw dye laser. We give results for the hyperfine structure of several $D$ and $F$ states in ${\mathrm{Cs}}^{133}$ and ${\mathrm{Rb}}^{87}$, obtained in level-crossing and optical double resonance experiments.

Physical Review Letters•Apr 30, 1973•89 citations

Fine Structure and Hyperfine Structure Measurements in Excited States of Alkali Atoms by Dye Laser Spectroscopy.

John W. Farley

•May 1, 1977•0 citations
Cascade transitions have been used to produce polarized atoms in optically inaccessible excited states. The polarized fluorescent light which is emitted when the atoms decay can be used to measure hyperfine structures, lifetimes, and other atomic parameters of these inaccessible states. Preliminary measurements of the hyperfine interval for the second excited SSS states of K39{\mathrm{K}}^{39}K39, Rb85{\mathrm{Rb}}^{85}Rb85, Rb87{\mathrm{Rb}}^{87}Rb87, and Cs133{\mathrm{Cs}}^{133}Cs133 are (in MHz) 46(2), 271(15), 565(40), and 684(50), respectively. To our knowledge, these are the first measurements of excited SSS-state hyperfine intervals in alkali atoms.
The hyperfine structure of the second-excited DDD states of 85Rb^{85}\mathrm{Rb}85Rb, 85Rb^{85}\mathrm{Rb}85Rb, and 133Cs^{133}\mathrm{Cs}133Cs has been measured by the method of cascade-radio-frequency spectroscopy and cascade-level crossing. The sign of the magnetic-dipole coupling constant AAA is determined by the method of cascade-decoupling and cascade-radio-frequency spectroscopy with narrow-band excitation. Lifetimes $\ensuremath{\tau}$ of some of these states are measured by the cascade-Hanle effect. We find that for 87Rb^{87}\mathrm{Rb}87Rb, $A(5^{2}D_{\frac{3}{2}})=14.43\ifmmode\pm\else\textpm\fi{}0.23$ MHz, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}7.44\ifmmode\pm\else\textpm\fi{}0.10$ MHz, $\ensuremath{\tau}(5^{2}D_{\frac{3}{2}})=205\ifmmode\pm\else\textpm\fi{}40$ nsec; for 85Rb^{85}\mathrm{Rb}85Rb, $A(5^{2}D_{\frac{3}{2}})=4.18\ifmmode\pm\else\textpm\fi{}0.20$ MHz, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}2.12\ifmmode\pm\else\textpm\fi{}0.20$ MHz; for 133Cs^{133}\mathrm{Cs}133Cs, $A(6^{2}D_{\frac{3}{2}})=16.30\ifmmode\pm\else\textpm\fi{}0.15$ MHz, $A(6^{2}D_{\frac{5}{2}})=\ensuremath{-}3.6\ifmmode\pm\else\textpm\fi{}1.0$ MHz, $\ensuremath{\tau}(6^{2}D_{\frac{3}{2}})=57\ifmmode\pm\else\textpm\fi{}15$ nsec.
We report the first successful measurements by cascade radio-frequency spectroscopy of the hyperfine structures of excited SSS and DDD states of rubidium. We obtain the following magnetic dipole coupling constants (in MHz): for Rb87{\mathrm{Rb}}^{87}Rb87, $A(7^{2}S_{\frac{1}{2}})=312.5\ifmmode\pm\else\textpm\fi{}3.5$, $A(5^{2}D_{\frac{3}{2}})=14.1\ifmmode\pm\else\textpm\fi{}0.5$, $A(5^{2}D_{\frac{5}{2}})=\ensuremath{-}8.0\ifmmode\pm\else\textpm\fi{}1.5$; for Rb85{\mathrm{Rb}}^{85}Rb85, $A(7^{2}S_{\frac{1}{2}})=92.6\ifmmode\pm\else\textpm\fi{}1.0$, $A(5^{2}D_{\frac{3}{2}})=4.1\ifmmode\pm\else\textpm\fi{}0.5$. The anomalous, negative value of AAA for the 52D525^{2}D_{\frac{5}{2}}52D25​​ state may be related to the anomalously small fine-structure interval of the 5D5D5D state of rubidium.
The hyperfine structure of several highly excited 2D^{2}D2D states in 87Rb^{87}\mathrm{Rb}87Rb and 133Cs^{133}\mathrm{Cs}133Cs has been measured. The DDD-state atoms were produced in a two-step-excitation process. In the first step, multiple scattering of the strong alkali-metal D1{D}_{1}D1​ and D2{D}_{2}D2​ lines from an rf lamp was used to excite atoms into the first excited 2P^{2}P2P levels. The intense tunable radiation from a cw dye laser was used in the second step to transfer PPP-state atoms into highly excited DDD states. Level-crossing and optical-double-resonance techniques were used for the determination of the absolute values of the hyperfine-interaction constants. The following results (in MHz) were obtained for the magnetic dipole and the electric quadrupole interaction constants aaa and bbb: For 87Rb^{87}\mathrm{Rb}87Rb, ∣a(62D32)∣=7.84(5)|a(6^{2}D_{\frac{3}{2}})|=7.84(5)∣a(62D23​​)∣=7.84(5), ∣b(62D32)∣=0.53(6)|b(6^{2}D_{\frac{3}{2}})|=0.53(6)∣b(62D23​​)∣=0.53(6) (ba>0\frac{b}{a}>0ab​>0), ∣a(2D52)∣=3.6(7)|a(^{2}D_{\frac{5}{2}})|=3.6(7)∣a(2D25​​)∣=3.6(7), ∣a(72D32)∣=4.53(3)|a(7^{2}D_{\frac{3}{2}})|=4.53(3)∣a(72D23​​)∣=4.53(3), ∣b(72D32)∣=0.26(4)|b(7^{2}D_{\frac{3}{2}})|=0.26(4)∣b(72D23​​)∣=0.26(4) (ba>0\frac{b}{a}>0ab​>0), ∣a(72D52)∣=2.2(5)|a(7^{2}D_{\frac{5}{2}})|=2.2(5)∣a(72D25​​)∣=2.2(5). For 133Cs^{133}\mathrm{Cs}133Cs, ∣a(82D32)∣=3.98(8)|a(8^{2}D_{\frac{3}{2}})|=3.98(8)∣a(82D23​​)∣=3.98(8), ∣a(82D52)∣=0.9(4)|a(8^{2}D_{\frac{5}{2}})|=0.9(4)∣a(82D25​​)∣=0.9(4), ∣a(92D32)∣=2.37(3)|a(9^{2}D_{\frac{3}{2}})|=2.37(3)∣a(92D23​​)∣=2.37(3), ∣a(92D52)∣=0.5(2)|a(9^{2}D_{\frac{5}{2}})|=0.5(2)∣a(92D25​​)∣=0.5(2), ∣a(102D32)∣=1.52(3)|a(10^{2}D_{\frac{3}{2}})|=1.52(3)∣a(102D23​​)∣=1.52(3), ∣a(102D52)∣=0.4(2)|a(10^{2}D_{\frac{5}{2}})|=0.4(2)∣a(102D25​​)∣=0.4(2). The aaa factors generally deviate strongly from the values expected in a one-electron picture of the alkali-metal atom indicating the importance of polarization and correlation effects for these states. For 87Rb^{87}\mathrm{Rb}87Rb a comparison with a recent calculation including polarization effects is made. The bbb factors for 87Rb^{87}\mathrm{Rb}87Rb are the first significant values allowing a calculation of an alkali-metal-atom nuclear quadrupole moment from non-PPP-state data.
In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.
Highly excited SSS, DDD, and FFF levels in cesium and rubidium have been populated utilizing a two-step optical excitation method. In the first step an rf lamp is used to transfer atoms into the first PPP states, and the subsequent excitation is performed with the tunable radiation of a cw dye laser. We give results for the hyperfine structure of several DDD and FFF states in Cs133{\mathrm{Cs}}^{133}Cs133 and Rb87{\mathrm{Rb}}^{87}Rb87, obtained in level-crossing and optical double resonance experiments.