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Wide-bandgap nonlinear crystal LiGaS<sub>2</sub> for femtosecond mid-infrared spectroscopy with chirped-pulse upconversion.

Applied Optics 2016 November 21
Femtosecond time-resolved mid-infrared (MIR) spectroscopy based on chirped-pulse upconversion is a promising method for observing molecular vibrational dynamics. A quantitative study on nonlinear media for upconversion is still essential for wide applications, particularly at the frequencies below 2000  cm<sup>-1</sup>. We evaluate wide-bandgap nonlinear crystals of Li-containing ternary chalcogenides based on their performance as the upconversion medium for femtosecond MIR spectroscopy. The upconversion efficiency is measured as a function of the MIR pulse frequency and the chirped pulse energy. LiGaS<sub>2</sub> is found to be an efficient crystal for the upconversion of MIR pulses in a wide frequency range of 1100-2700  cm<sup>-1</sup>, especially below 2000  cm<sup>-1</sup>. By using LiGaS<sub>2</sub> as an efficient upconversion crystal, we develop a MIR pump-probe spectroscopy system with a spectral resolution of 2.5  cm<sup>-1</sup>, a time resolution of 0.2 ps, and a probe window of 120  cm<sup>-1</sup>. Vibrational relaxation dynamics of CO stretching modes of Mn<sub>2</sub>(CO)<sub>10</sub> in cyclohexane and bovine serum albumin in D<sub>2</sub>O are demonstrated with a high signal-to-noise ratio.

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