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Third-order nonlinearities in molecular hydrogen - Two-photon resonance enhanced third-harmonic generation and Raman scattering

Effects of quantum mechanical interferences on third-order susceptibilities in molecules are studied. First principle calculations for molecular hydrogen are presented and shown to agree with results derived from experimental stimulated Raman gain and spontaneous Raman cross-section data. 10 percent third-harmonic conversion efficiency in H2 at 1 atm without phase matching should require a 150 MW per sq cm at 4.81 microns. As little as 5.9-MW power is sufficient when the beam is properly focused. Resonance Raman scattering (RRS) is proposed for experimentally investigating the interference effects, which tend to reduce the strength of third-order nonlinear susceptibilities.

Pan, C.-L.

Observation of intense Stokes and anti-Stokes lines in CH4 pumped by 355 nm of a Nd:YAG laser

The stimulated Raman scattering (SRS) and four-wave mixing (FWM) processes are studied in detail in CH4 gas pumped by the third-harmonic of Nd:YAG laser at 355 nm. The conversion efficiency and average output energy are measured for the various Stokes and anti-Stokes lines at different experimental conditions. The threshold input energy at various CH4 pressures is calculated for the unguided and capillary waveguide Raman cells. The calculated values for the capillary case are compared with the measured values at different CH4 pressures and the two results are in good agreement.

Sentrayan, K.

IR pumped third-harmonic generation and sum-frequency generation in diatomic molecules

The potential efficiency of using nonlinear up-conversion techniques for the high efficiency type lasers (CO,CO2, and chemical) is assessed. Results indicate that: the small pump photon energy necessitates the use of molecular media for conversion if resonance enhancement is to be used and that molecular systems present several problems. These difficulties include: their levels are complex; their transition probabilities are often unknown; and the oscillator strengths among vibrational levels in the ground electronic state of a molecule are much smaller than those among electronic states of an atom, thus limiting the magnitude of nonlinear interactions. It is shown that this problem can be eliminated by making use of vibronic transitions which, being primarily electronic transitions have much larger matrix elements and efficient conversion can be achieved with molecular systems.

She, C. Y.

Infrared-pumped third-harmonic and sum-frequency generation in diatomic molecules

Using molecular hydrogen as a model system, we present a calculation which demonstrates the feasibility of efficient third-harmonic and sum-frequency generation of IR laser radiation by diatomic molecular gases. A conversion efficiency of 10% without phase matching is achievable with a modest laser intensity of about 20 MW/sq cm. In addition to a two-photon resonance, the efficient conversion depends on a mechanism which makes use of virtual vibronic transitions exclusively. Possible methods for phase matching are also suggested.

She, C. Y.