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Soviet Journal of Quantum Electronics

Direct determination of the two-photon absorption cross section by the intracavity laser spectroscopy method

Valery M. Baev, T. P. Belikova, V. F. Gamalii, Эдуард Алексеевич Свириденков, A F Suchkov

Published Dec 31, 1984• 3 citations

Abstract

The intracavity laser spectroscopy method was used to determine the two-photon absorption of potassium vapor. The two-photon transitions from the ground state 4 2 S 1/2 to the states 6 2 S 1/2 and 4 2 D 3/2,5/2 were detected from absorption in the output spectrum of a wide-band dye laser emitting in the range 760–770 nm; the absorption occurred at a frequency corresponding to the difference between the energies of the upper state and the energy of a ruby laser photon. The ratio ofthe absorption cross section to the square ofthe field was σ 2 / E 2 = 1.5 × 10 −33 ,1.3 × 10 −35 ,and 2.8 × 10 −36 m 4 /V 2 , in satisfactory agreement with calculations carried out on the basis of perturbation theory.

DOI: 10.1070/qe1984v014n12abeh006230

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The intracavity laser spectroscopy method was used to determine the two-photon absorption of potassium vapor. The two-photon transitions from the ground state 4 2 S 1/2 to the states 6 2 S 1/2 and 4 2 D 3/2,5/2 were detected from absorption in the output spectrum of a wide-band dye laser emitting in the range 760–770 nm; the absorption occurred at a frequency corresponding to the difference between the energies of the upper state and the energy of a ruby laser photon. The ratio ofthe absorption cross section to the square ofthe field was σ 2 / E 2 = 1.5 × 10 −33 ,1.3 × 10 −35 ,and 2.8 × 10 −36 m 4 /V 2 , in satisfactory agreement with calculations carried out on the basis of perturbation theory.

Recently we demonstrated lasing at 420 nm and 455 nm inside of rubidium and cesium vapor cells respectively, by non-resonant, two photon absorption at near infrared pump wavelengths. Two photon absorption from the ground S1/2 state to excited D3/2,5/2 or higher lying S1/2 state via virtual states and subsequent infrared stimulated emission pumps the upper laser levels, the second excited P1/2,3/2 states. To better understand the mechanism and phenomenology of this type of laser, this paper presents a method for determining the two-photon absorption (TPA) cross-section for the 5S1/2 −→ 5D5/2 transition in naturally occurring rubidium. For an incident pump intensity of 392 W cm2 and a rubidium concentration of 3.34 × 10 atoms cm3 , a peak absorbance of 0.10 is observed. The concentration of the Rb in the test cell is determined by one photon absorption spectra of the D2, indicating a vapor curve shifted by 14 C from the exterior wall temperature. The incident laser beam is focused to a waist of 75 μm. The beam quality is consistent with an M = 1.05 − 1.09. A model for the intensity as a function of propagation distance is developed to interpret the observed absorption spectrum and determine a cross-section for the two photon absorption.

Three-photon absorption spectroscopy allows determination of the

\mathrm{nf}^{2}F_{\frac{5}{2},\frac{7}{2}}^{0}

energy levels of alkali metals ($\ensuremath{\Delta}L=+3$). The

3d^{2}D_{\frac{3}{2},\frac{5}{2}}

levels of KI were selectively excited using a narrow-band dye laser. The $3d^{2}D_{\frac{3}{2},\frac{5}{2}}\ensuremath{\rightarrow}\mathrm{nf}^{2}F_{\frac{5}{2},\frac{7}{2}}^{0}$ absorption lines were observed in the background spectrum of another dye laser, and the

\mathrm{nf}^{2}F_{\frac{5}{2},\frac{7}{2}}^{0}

energy levels were deduced, from

n=10

to

n=14

inclusive, with an accuracy better than 0.1 ${\mathrm{cm}}^{\ensuremath{-}1}$. Previously, an experiment was performed for the

7f^{2}F_{\frac{5}{2},\frac{7}{2}}^{0}

levels in order to verify the method. Shifts and systematic errors were entirely negligible. For all lines, the relative intensities of the absorbed doublet peaks are in good agreement with the estimates of the $4s^{2}S_{\frac{1}{2}}\ensuremath{\rightarrow}3d^{2}D_{\frac{3}{2},\frac{5}{2}}$ probabilities.

An experimental investigation was made of the broadening of the D lines and of the two-photon absorption line (4S1/2–6S1/2) of potassium vapor subjected to ruby laser radiation. A dye laser beam was used as a probe and this made it possible to record simultaneously all three absorption lines. The measurements were carried out for different polarizations and geometries of the exciting and probe radiations. The observed broadening was attributed to the high-frequency Stark effect in the strong field of the incident wave.