Noncollinear Optical Parametric Amplification of Broadband Infrared Sum Frequency Generation Vibrational Spectroscopy

J Phys Chem Lett. 2024 Mar 7;15(9):2470-2475. doi: 10.1021/acs.jpclett.4c00003. Epub 2024 Feb 26.

Abstract

Sum-frequency generation (SFG) vibrational spectroscopy is an invaluable tool in surface science, known for its specificity to surfaces and interfaces. Despite its wide application, it is often hampered by weak signal detection. Here, we present an innovative enhancement technique of postsample amplification, using a picosecond noncollinear optical parametric amplifier (NOPA). We conducted a systematical investigation into the impact of different intensities of pump and SFG seed light, as the input signal in NOPA, and demonstrated this method on the octadecanethiol (ODT) molecules on gold films. The amplified SFG by NOPA reproduced the SFG vibrational spectra, enhanced by about 4 orders of magnitude but with broader spectral resolution due to the short pulse width of the pump light in NOPA. This study makes it possible to realize highly sensitive SFG measurements, marking a significant advancement in spectroscopic analysis techniques.