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Physical Review A

Measured third-order susceptibility and excited-state oscillator strengths for atomic mercury

W. J. Alford, Arlee V. Smith

Published Jul 1, 1987• 14 citations
Publisher

Abstract

We have measured the null positions in the third-order susceptibility for two-photon resonant (6 $^{1}7$ $^{1}$,3S) sum-frequency mixing in atomic mercury. In addition, we have made measurements of some 7S-nP oscillator strengths using a fluorescence-dip technique. Combined with earlier results we are able to obtain a set of 7S-nP (n=7--13) oscillator strengths which gives a good description of the third-order susceptibility. The uncertainty in the 7S-nP oscillator strengths is typically 35--50%. The absolute third-order susceptibility has been determined for energies less than 83 000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with an uncertainty of typically 20--30%.

DOI
10.1103/physreva.36.641

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Optics Express•Jun 22, 2009•37 citations
We have measured the null positions in the third-order susceptibility for two-photon resonant (6 17^{1}717 1^{1}1,3S) sum-frequency mixing in atomic mercury. In addition, we have made measurements of some 7S-nP oscillator strengths using a fluorescence-dip technique. Combined with earlier results we are able to obtain a set of 7S-nP (n=7--13) oscillator strengths which gives a good description of the third-order susceptibility. The uncertainty in the 7S-nP oscillator strengths is typically 35--50%. The absolute third-order susceptibility has been determined for energies less than 83 000 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1 with an uncertainty of typically 20--30%.
We have measured oscillator strengths for the transitions 6 1S^{1}S1S to (5${d}^{10}$6s np) n 1^{1}1,3P1{\mathrm{P}}_{1}P1​ for n=6 to 13 and to (5${d}^{9}666{s}^{2}$6p) 6p' 1P^{1}P1P for atomic Hg. Two new techniques for measuring dispersion based on nonlinear-optical sum-frequency mixing are used to achieve 10% accuracy for the stronger transitions. One method uses crossed beams in a Hg heat-pipe cell to map dispersion curves in regions of anomalous dispersion. The second method uses input beams of three separate frequencies and maps regions of normal and anomalous dispersion by tuning one of the input frequencies to the red and blue of the 6 3P1^{3}P_{1}3P1​ level. Because the dispersion of the refractive index near a resonance is determined over a large wavelength range, the oscillator strength of that resonance is determined independent of the strengths of other transitions.
We have developed new techniques based on four-wave mixing for the accurate determination of oscillator strengths and applied them to measure 61S - n1,3P and 71S - n1,3P (n = 6 - 13) matrix elements of atomic Hg. For transitions from the 61S ground state, index matching conditions were used to determine refractive indicies and thus f-values, while the frequency dependence of the nonlinear susceptibility was used to deduce matrix elements for transitions involving 71S. For all measurements, two-photon resonance with the 71S state was maintained.
The ability to introduce additional resonances in the nonlinear optical susceptibility of a medium by the injection of an additional radiation field is an attractive possibility from the standpoint of efficient tunable frequency mixing processes in the VUV. The possibility of such processes suggest themselves in previous observations in atomic mercury where an enhancement of several orders of magnitude in the third harmonic generation efficiency has been reported when the input frequency is four-photon resonant with the 6S → 6D transition(1).
A coherent continuous-wave Lyman-alpha source based on four-wave sum-frequency mixing in mercury vapor has been realized with solid-state lasers. The third-order nonlinear susceptibility is enhanced by the 6(1)S - 7(1)S two-photon resonance and the near 6(1)S-6(3)P one-photon resonance. The phase matching curve for this four-wave mixing scheme is observed for the first time. In addition we investigate the two-photon enhancement of the Lyman-alpha yield and observe that the maxima of Lyman-alpha generation are shifted compared to the two-photon resonances of the different isotopes.