Abstract

The coherent anti-Stokes Raman spectroscopy (CARS) of electronic states of the Ce³⁺ ion in a CeF₃ crystal at 3.8 K is reported. CARS resonances involving the ground state of the ²F_5/2 manifold and the Stark components of the ²F_7/2 manifold at 2161 and 2239 cm⁻¹ have been detected. Measurements were made with both visible (λ₁ ≈ 476 nm, λ₂ = 532 nm) and near-ultraviolet (λ₁ = 355 nm, λ₂ ≈ 385 nm) lasers. The enhancement of the third-order susceptibility owing to the electronic transitions, |χ^(3)R/χ^(3)NR|_max, is as great as 4.8. This represents an order-of-magnitude increase over that in singly resonant electronic CARS experiments in other rare-earth crystals. The CARS data also yielded accurate measurements of the Ce³⁺ electronic Raman cross sections. In the visible region, σ_zz(2161 cm⁻¹) = (5.0 ± 1.1) × 10⁻³⁰ cm² and σ_zz(2239 cm⁻¹) = (1.9 ± 0.7) × 10⁻³⁰ cm². One could calculate both the absolute magnitude and the dispersion of |χ^(3)R|_max by modeling the virtual intermediate states as a single degenerate 5d state at 45 000 cm⁻¹.

© 1991 Optical Society of America

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