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Optics and Spectroscopy

Fine-structure mixing of excited states of cesium atoms upon an impact on the surface of a sapphire single crystal

A. M. Bonch-Bruevich, T. A. Vartanyan, Nikita B. Leonov, Sergey G. Przhibel'skii, Valentin N. Smirnov, V. V. Khromov

Published Feb 1, 2006• 6 citations
Publisher

Abstract

The spectrum of resonantly excited luminescence of Cs atoms in a microcell with sapphire windows has been studied. Spectral wings of atomic luminescence near the windows have been revealed near (±50 cm−1) the D2 line of the excited 6S 1/2–6P 3/2 transition. At the same time, the radiation of the D1 line has been found. The features of the spectrum of the far wings, namely, the exponential shape and the relatively small difference between the static and the antistatic wings, as well as the radiation of the D1 line, have been explained by the mixing of fine-structure states due to interactions of Cs atoms with the sapphire windows. From the relative intensity of the lines, it has been determined that the probability of luminescence quenching at the window surfaces differs from unity by no less than 1/700.

DOI
10.1134/s0030400x06020019

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The shape of the luminescence spectrum of Cs atoms flying near a sapphire surface is described phenomenologically for the detuning from the D 2 line ranging within 5–50 cm −1 . The numerical fitting of one theoretical parameter and a small variation of another parameter ensures a satisfactory agreement with the experimental spectrum. The experimentally determined abnormally high intensity of the antistatic wing is explained by the effect of phase relaxation of the atomic transition, caused by fluctuations of the electric field of oscillating ions of the sapphire crystal lattice.

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The spectrum of the luminescence in the far wing of the atomic spectral line due to the atom-surface collisions between cesium atoms and sapphire surface is obtained experimentally. A cw diode laser operating at the wavelength of 852.1 nm resonant to the 6S1/2 - 6P3/2 transition in the free Cs atoms was used to excite the luminescence of atomic vapors. To avoid atom-atom collisions a specially designed spectroscopic cell with two sapphire windows only 3 μm apart was employed. The wings were measured for the detuning up to 200 cm-1 on both sides ofthe atomic spectral line. Besides the wings, luminescence at the wavelength of 894.3 nm corresponding to the 6S1/2 - 6P1/2 transition was observed. Notwithstanding high quenching probability, more than 0.5% of the atoms leave the surface in the state of another fine-structure component.

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[Fluorescence spectrum of cesium vapor resonantly excited by the 852.3 nm laser line].

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Radiation and Collision Energy Transfer of Excitated Cs(6P) Atoms Mixed with He

Yifan Shen

By applying the laser absorption and fluorescence method,the cross sections for the fine structure mixing and quenching of the Cs(6P) state,induced by collision with He atoms,have been measured.Cesium atoms were optically excited to the 6P3/2 state.The excited atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single mode laser beam,which was tuned to the 6PJ→8S1/2 transitions.The effective radiative rates were calculated for the 6PJ→6S transitions.The fluorescence intensity I895 of the sensitized 6P1/2→6S1/2 emission was measured as a function of He density in the range 0.5×1018～4×1018cm-3 at constant temperature T=337 K.It was found that the quantity N/I895 exhibited a parabolic dependence on N,confirming that the quenching of the 6PJ states was due to collision with He atoms,not ground state Cs atoms.The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ3/2→1/2=(1.46±0.51)×10-19 cm2 and σD=(2.28±0.80)×10-18 cm2 for the 6PJ fine structure mixing and quenching,respectively,due to collision with He atoms.

Chinese Journal of Lasers•Jan 1, 2007•0 citations
The spectrum of resonantly excited luminescence of Cs atoms in a microcell with sapphire windows has been studied. Spectral wings of atomic luminescence near the windows have been revealed near (±50 cm−1) the D2 line of the excited 6S 1/2–6P 3/2 transition. At the same time, the radiation of the D1 line has been found. The features of the spectrum of the far wings, namely, the exponential shape and the relatively small difference between the static and the antistatic wings, as well as the radiation of the D1 line, have been explained by the mixing of fine-structure states due to interactions of Cs atoms with the sapphire windows. From the relative intensity of the lines, it has been determined that the probability of luminescence quenching at the window surfaces differs from unity by no less than 1/700.
The shape of the luminescence spectrum of Cs atoms flying near a sapphire surface is described phenomenologically for the detuning from the D 2 line ranging within 5–50 cm −1 . The numerical fitting of one theoretical parameter and a small variation of another parameter ensures a satisfactory agreement with the experimental spectrum. The experimentally determined abnormally high intensity of the antistatic wing is explained by the effect of phase relaxation of the atomic transition, caused by fluctuations of the electric field of oscillating ions of the sapphire crystal lattice.
The spectrum of the luminescence in the far wing of the atomic spectral line due to the atom-surface collisions between cesium atoms and sapphire surface is obtained experimentally. A cw diode laser operating at the wavelength of 852.1 nm resonant to the 6S1/2 - 6P3/2 transition in the free Cs atoms was used to excite the luminescence of atomic vapors. To avoid atom-atom collisions a specially designed spectroscopic cell with two sapphire windows only 3 μm apart was employed. The wings were measured for the detuning up to 200 cm-1 on both sides ofthe atomic spectral line. Besides the wings, luminescence at the wavelength of 894.3 nm corresponding to the 6S1/2 - 6P1/2 transition was observed. Notwithstanding high quenching probability, more than 0.5% of the atoms leave the surface in the state of another fine-structure component.
The shape of the luminescence spectrum of Cs atoms flying near a sapphire surface is explored experimentally and described phenomenologically for the detuning range of 5 to 50 cm-1 on both sides of D2 line. The numerical fitting of one theoretical parameter and a small variation of another parameter ensure a satisfactory agreement with the experimental spectrum. The experimentally determined abnormally high intensity of the antistatic wing is explained by the effect of phase relaxation of the atomic transition, caused by fluctuations of the electric field of oscillating ions of the sapphire crystal lattice.
The changes in the states of excited Rb atoms approaching a single-crystal sapphire surface have been investigated by methods of laser-excitation spectroscopy and luminescence of Rb vapor in a cell with sapphire windows, the gap between which was varied from 250 to 500 nm. Upon resonant excitation of Rb atoms by two semiconductor lasers with powers of 20 and 40 mW, luminescence from optically excited 5D 3/2 and 5D 5/2 states and optically unexcited 6P 1/2 and 6P 3/2 states is observed. It is established that the luminescence intensity from unexcited states is only a few times lower than that from excited states, with allowance for the fact that excited atoms are rapidly and almost completely quenched on the sapphire surface. The found anomalously strong luminescence from optically unexcited 6P J states is explained by their nonradiative occupation near the sapphire surface from optically excited 5P J states, in which atoms fail to reach the sapphire surface because of the repulsion from it. This repulsion is due to the polarization interaction between sapphire and the atoms in the 5P J states near the surface. Nonradiative transition from the 5P J state to the 6P J −1 state is accompanied by excitation of two optical phonons in sapphire.
The fluorescence spectrum of cesium vapor was studied in a cell irradiated with the light of 852.3 nm resonance line from a single mode laser diode. From the intensities and spectra of the Cs and Cs2 fluorescence we identified several collisional and radiative processes in the excited cesium atom-dimer system. The atomic lines of the highly excited states were the result of collisional energy transfer from Cs(6P 3/2) + Cs(6P 3/2) to Cs(6D, 8S) atoms. The Cs2 (B 1 IIu) band formed in Cs (6P) + Cs2 (X1sigmag+) collisions. The fine-structure mixing in 6 2P atoms was studied through excitation transfer, energy-pooling collision, and collisional excitation transfer between Cs2 and Cs. The authors estimated the value of rate coefficient for the collisional energy transfer from 6P3/2 to 6P1/2 to be (5.2+/-2.1) x 10(-11) cm3 x s(-1). For the excitation transfer process Cs2 (B 1 IIu)+ Cs(6S)--> Cs2 (X 1sigmag+) + Cs(6P1/2 ), a rate coefficient of (1.0+/-0.4) x 10(-9) cm3 x s(-1) was yielded.
By applying the laser absorption and fluorescence method,the cross sections for the fine structure mixing and quenching of the Cs(6P) state,induced by collision with He atoms,have been measured.Cesium atoms were optically excited to the 6P3/2 state.The excited atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single mode laser beam,which was tuned to the 6PJ→8S1/2 transitions.The effective radiative rates were calculated for the 6PJ→6S transitions.The fluorescence intensity I895 of the sensitized 6P1/2→6S1/2 emission was measured as a function of He density in the range 0.5×1018～4×1018cm-3 at constant temperature T=337 K.It was found that the quantity N/I895 exhibited a parabolic dependence on N,confirming that the quenching of the 6PJ states was due to collision with He atoms,not ground state Cs atoms.The coefficients of the second-order polynomial fitted through the measured data yielded the cross sections σ3/2→1/2=(1.46±0.51)×10-19 cm2 and σD=(2.28±0.80)×10-18 cm2 for the 6PJ fine structure mixing and quenching,respectively,due to collision with He atoms.