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Opt Lett. 2003 Mar 1;28(5):346-8.

Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases.

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  • 1JILA and the Department of Physics, University of Colorado, Boulder, Colorado 80309-0440, USA.


Transient birefringence can be induced in a gas of anisotropic molecules by an intense polarized laser pulse. We propose to use this birefringence to phase match nonlinear optical frequency-conversion processes. The conditions for anisotropic phase matching are derived, and experimental conditions required for phase-matched third-harmonic generation in a gas-filled hollow-core fiber are presented. We show that these conditions are experimentally feasible over a significant parameter range, making possible a new type of nonlinear optics.

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