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Journal of the Optical Society of America B

Laser spectroscopy measurement of radiative lifetimes of highly excited thulium Rydberg states

E. P. Vidolova-Angelova, Dimitar Angelov, T. B. Krustev, S. T. Mincheva

Published Dec 1, 1989• 8 citations
Publisher

Abstract

The radiative lifetimes τrad of the highly excited 4f7/2136s1/2(4)np3/2[11/2](n=21−31) Rydberg Tm states have been measured with the method of multistep laser excitation and electric field ionization. The lifetime values have been obtained with an accuracy of better than 15%. The influence of blackbody radiation on the states with n ≥ 27 has been observed. The experimental results are in good agreement with our previously calculated values obtained by relativistic perturbation theory with a zero-order model approximation. It has been shown that the τrad-versus-n* dependence (n* is the effective principal quantum number) is best described by the relation τrad = 0.0022.(n*)2.46 (μsec). This property may be attributed to the strongly expressed nonhydrogenlike behavior of the investigated states, which is caused by the essentially non-Coulombic core potential acting on the Rydberg electron.

DOI
10.1364/josab.6.002295

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The radiative lifetimes τrad of the highly excited 4f7/2136s1/2(4)np3/211/2 Rydberg Tm states have been measured with the method of multistep laser excitation and electric field ionization. The lifetime values have been obtained with an accuracy of better than 15%. The influence of blackbody radiation on the states with n ≥ 27 has been observed. The experimental results are in good agreement with our previously calculated values obtained by relativistic perturbation theory with a zero-order model approximation. It has been shown that the τrad-versus-n* dependence (n* is the effective principal quantum number) is best described by the relation τrad = 0.0022.(n*)2.46 (μsec). This property may be attributed to the strongly expressed nonhydrogenlike behavior of the investigated states, which is caused by the essentially non-Coulombic core potential acting on the Rydberg electron.
The radiative lifetimes of the Eu 4f 7 6s n p ( 8 P J or 10 P J ) Rydberg states with J = 5/2 and 11/2 are investigated with a combination of multi-step laser excitation and pulsed electric field ionization, from which their dependence on the effective principal quantum number is observed. The lifetimes of 21 states are reported along with an evaluation of their experimental uncertainty. The influence of blackbody radiation, due to the oven temperature, on the lifetime of the higher- n states is detected. The non-hydrogen behavior of the investigated states is also observed.
We have observed fluorescence and ionization signals resulting from two-photon resonant excitation of thallium in an atomic beam. The output of a pulsed dye laser is used to excite the resonance between the ground state (6('2)P(,1/2)) and an excited n('2)P state of thallium. Both two-photon absorption and three-photon absorption occur simultaneously; the latter results in photoionization of the atom. The excited states populated by two-photon absorption decay via cascade fluorescence back to the ground state; one or more of these spectral components constitute our fluorescence signal. The lifetimes of the excited n('2)P states of thallium have been measured directly by observing the exponential decay of this fluorescence. Calculations are included to ascertain the time required for the fluorescence signal to reach within 2% of a simple exponential decay. This decay is a measure of the lifetime of the initial state, under the condition that none of the fluorescence components arise from states which are populated by cascade through longer-lived states. The lifetimes of the n('2)P(,1/2) and n('2)P(,3/2) states of thallium for n = 7 to 11 are determined in this manner and compared with the values deduced from semi-empirical calculations of oscillator strengths by various authors. For calculations employing the effects of core polarizability in the electron wavefunctions and in the transition matrix elements, the agreement is very good--to within our experimental uncertainty, which is typically(, )<5%. Our measurements are also compared to the four other known experimental values for such excited states of thallium. Some of these previous experiments and calculations were carried out in conjunction with parity non-conservation experiments in thallium. Our measurements may provide useful checks on the accuracy of some of the calculations performed in the evaluation of such experiments. The ionization and fluorescence signals are also studied under conditions of strong saturation of the two-photon resonance with the 7('2)P states. The manifestation of saturation in the ionization signal is a broadening of the excitation spectrum, which is found to greatly exceed that of the fluorescence signal. Furthermore, the ratio of the ionization signal to the fluorescence signal at the peak of the resonance is found to vary linearly at intensities below about 10('9) W/cm('2); this too saturates at higher intensities. Various models are employed to simulate the observed behavior, encompassing both rate equations as well as density matrix formulations. The numerical solutions to these models are compared with the observed behavior; the agreement is found to depend strongly on the assumed experi- mental conditions to which the ensemble of atoms is subjected.
New features of the blackbody-induced radiation processes on Rydberg atoms were discovered on the basis of numerical data for the blackbody-induced decay P d nl ( T ), excitation P e nl ( T ) and ionization P ion nl ( T ) rates of n S, n P and n D Rydberg states calculated together with the spontaneous decay rates P sp nl in neutral hydrogen, and singlet and triplet helium atoms for some values of the principal quantum number n from 10 to 500 at temperatures from T = 100 K to 2000 K. The fractional rates R d ( e , ion) nl ( T ) = P nl d ( e , ion) ( T )/ P sp nl equal to the ratio of the induced decay (excitation, ionization) rates to the rate of spontaneous decay were determined as functions of T and n in every series of states with a given angular momentum l = 0, 1, 2. The calculated data reveal an essential difference between the asymptotic dependence of the ionization rate P ion nl ( T ) and the rates of decay and excitation P d ( e ) nl ( T )∝ T / n 2 . The departures appear in each Rydberg series for n > 100 and introduce appreciable corrections to the formula of Cooke and Gallagher. Two different approximation formulae are proposed on the basis of the numerical data, one for R d ( e ) nl ( T ) and another one for R ion nl ( T ), which reproduce the calculated values in wide ranges of principal quantum number from n = 10 to 1000 and temperatures between T = 100 K and T = 2000 K with an accuracy of 2% or better. Modified Fues' model potential approach was used for calculating matrix elements of bound–bound and bound–free radiation transitions in helium.
We present the results of relativistic calculation of the radiative transition probabilities and excited states lifetimes for a heavy Rydberg atomic systems in a black-body (thermal) radiation field on example of the rubidium. As theoretical approach we apply the combined generalized relativistic energy approach and relativistic many-body perturbation theory with ab initio Dirac zeroth approximation. There are obtained the calculational data for the radiative transition probabilities and excited states lifetimes, in particular, the rubidium atom in the Rydberg states with principal quantum number n=10-100. It is carried out the comparison of obtained theoretical data on the effective lifetime for the group of Rydberg nS states of the rubidium atom at a temperature of T = 300K with experimental data as well as data of alternative theoretical calculation based on the improved quasiclassical model. It is shown that the accuracy of the theoretical data on the radiative transition probabilities and excited states lifetimes is provided by a correctness of the corresponding relativistic wave functions and accounting for the exchange-correlation effects.