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Optics and Spectroscopy

Change in the states of optically excited Rb atoms near sapphire surface

T. A. Vartanyan, A. E. Logunov, Anatoly S. Pazgalev, Sergey G. Przhibel'skii, David G. Sarkisyan, V. V. Khromov

Published Jul 1, 2013• 2 citations
Publisher

Abstract

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.

DOI
10.1134/s0030400x13070217

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•May 1, 2009•0 citations
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 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 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.
Enhancement and reduction of the fluorescence intensity in Rb atomic vapor are observed. The reduction is due to a depopulation of the 5P - {3/2 } state upon illumination of a Rb vapor cell with light corresponding to the 5P - {3/2 }→5D - {5/2 } transition. Collisional transfer of the 5D - {5/2 } atoms to the 5D - {3/2 } state, followed by radiative decay to the 5P - {1/2 } state, creates an increase in the population of the 5P - {1/2 } state. The increase in the excited state population results in an increase in the fluorescence intensity of the 5P - {1/2 }→5S - {1/2 } transition. The laser-induced population changes are monitored by the decrease or increase of the corresponding fluorescence signals. Using the steady-state rate equations, the rate constants for the stimulated emission(i.e., 5D - {5/2 }→5P - {3/2 }) is 2.0×10 +8s + {-1 }. The cross section for the fine-structure changing collision(i.e., 5D - {5/2 }→5D - {3/2 }) is 6.4×10 + {-14 }cm +2.
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 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.
A low-power tunable laser was used to populate the Rb(5P(3/2)) hyperfine-structure levels in a pure optically thick vapour in the presence of a dissipative surface. The retrofluorescence intensities and spectrum profile for the 780 nm (5P(3/2)--> 5S(1/2)) and 795 nm (5P(1/2)-->5S(1/2)) lines were measured and analyzed. The glass-vapor interface was considered as two distinct regions, a wavelength-thickness vapor layer adjacent to the surface and a more remote vapor region The first region was analyzed as a spectral filter that annihilated the absorbed photons and the second one as a rich spectral light source. The authors discussed two possible mechanisms for the 5P(1/2) population in the cell [i.e., mechanism(1): collisions Rb(5P(3/2))+Rb(5S(1/2))-->Rb(5P(1/2))+Rb(5S(1/2)); mechanism(2): collisions Rb(5D)+Rb(5S)-->Rb(5P)+Rb(5P)]. For each one of the possible mechanisms considered, the authors gave the theoretical formulation of the retrofluorescence integrated signal associated with 795 nm(5P(1/2)-->5S(1/2)), which was compared with experiment. Two important characteristic aspects of retrofluorescence spectra must be taken into account when dealing with retrofluorescence signals for atomic process investigation: the retrofluorescence intensity dependence on laser power and sensitized laser retrofluorescence line shapes. When the laser frequency is scanned through the hyperfine resonance line, the sensitized retrofluorescence spectra signal corresponding to the 795 nm line has a profile similar to the profile of the retrofluorescence signal at the 780 nm. The authors have pointed out that mechanism(1) gives the linear dependence of the trtrofluorescence as a function of laser power and the spectrum profile. The population of the 5P(1/2) atomic level in an optically thick vapour can be principally explained by the fine-structure excitation transfer process [mechanism(1)]. It appears from our experimental and theoretical investigations that, the spectral properties of the laser-induced Rb 795 nm sensitized retrofluorescence in a pure optically thick vapour near a dissipative surface cannot be explained by the mechanism(2).