Frequency down-conversion of solid-state laser sources to the mid-infrared spectral range using non-oxide nonlinear crystals

First-principles calculations of the structural, electronic and optical properties of CuGaS2 and AgGaS2

Direct infrared absorption prepares CH4 in two nearly isoenergetic vibrationally excited states, the symmetric stretch–bend combination (ν1+ν4) and the antisymmetric stretch–bend combination (ν3+ν4), for a study of the effect of stretching vibrations of CH4 on the reaction, CH4+Cl(2P3/2)→CH3+HCl. Comparison of intensities in the action spectra with those in the simulated absorption spectra shows that vibrational excitation of methane to the ν1+ν4 state promotes the reaction more efficiently than excitation to the ν3+ν4 state by a factor of 1.9±0.5. The reaction of methane in both vibrational states produces a substantial fraction (35%) of the CH3 products with the umbrella mode (ν2) excited, which we attribute to the presence of the bending vibration (ν4) in the combination states. The similarity of the vibrational population distributions of the products for the two excitations implies that the differences in the action spectra arise from the relative reactivity of the states rather than from population of different product states. This result is consistent with theoretical calculations that predict a stronger coupling of the symmetric stretching vibration to the reaction coordinate than the antisymmetric stretch. Analyzing the infrared laser power dependence of the signal with a simple two state model shows that the reaction cross section of the ν1+ν4 state of methane is 19±5 times larger than that of methane molecules in their ground or thermally populated vibrational states.

The relative reactivity of the stretch–bend combination vibrations of CH4 in the Cl (2P3/2)+CH4 reaction

A high-resolution cw spectrometer based on difference frequency generation (DFG) in a 20-mm-long AgGaS2 crystal pumped by two stabilized single-frequency cw dye–Ti:sapphire lasers is described. Experiments performed with a Rhodamine 6G and DCM dye laser combination pumped by a 20-W argon laser are reported. Informed radiation is generated from 7 to 9 μm with an ultranarrow linewidth (<0.5 MHz) and an output power 1 μW by making use of 90° type I phase matching. The performance of the DFG laser spectrometer is evaluated by using a portion of the ν2 band of NH3 near 1177 cm−1.

Continuous-wave infrared laser spectrometer based on difference frequency generation in AgGaS 2 for high-resolution spectroscopy

High energy and narrow bandwidth mid IR nanosecond laser system

A reliable source of coherent ns pulses of infrared radiation continuously tunable between 1.4 and 22 μm has been designed and built with the aim of developing a time-resolved infrared vibrational spectroscopy for species adsorbed on surfaces. The system is based on a Nd: YAG-laser and dye-laser combination which drive difference mixing processes in a sequence of nonlinear optical crystals (two LiNbO3, and a CdSe or AgGaS2). The system operates at MW peak power levels above 2500 cm−1, at kW power levels from 1000–2500 cm−1 and at 10–100 W levels down to 450 cm−1. These power levels are certainly sufficient for spectroscopic purposes, and at shorter wavelengths molecular pumping and applications requiring high-power should be possible. Vibrational spectra of a monolayer of CO adsorbed on Pt in an electrochemical cell have been obtained in an initial application of this source.

A laser infrared source of nanosecond pulses tunable from 1.4 to 22 μm

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A laser infrared source of nanosecond pulses tunable from 1.4 to 22 μm