Flexible high-resolution broadband sum-frequency generation vibrational spectroscopy for intrinsic spectral line widths

The Journal of Chemical Physics
Ruidan ZhangZefeng Ren

Abstract

The difficulty in achieving high spectral resolution and accurate line shape in sum-frequency generation vibrational spectroscopy (SFG-VS) has restricted its use in applications requiring precise detection and quantitative analysis. Recently, the development of high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS) with sub-wavenumber resolution generated by synchronizing two independent amplifier lasers have opened new opportunities for probing an intrinsic SFG response. Here, we present a new flexible approach to achieve HR-BB-SFG-VS. In this system, two regeneration amplifiers shared the same oscillator laser as the seed, and a time-asymmetric visible pulse with a nearly Lorentzian line shape filtered by an etalon was used to overlap with a femtosecond broadband infrared pulse. This Lorentzian line shape of the visible pulse can greatly simplify the spectral fitting and analysis. We also demonstrated that the single-sided long visible pulse provided both high spectral resolution (1.4 cm-1) and effective suppression of the non-resonant background by detuning the time delay between visible and infrared pulses in SFG-VS measurements. With this new SFG setup, a pair of spectral splittings by 3...Continue Reading

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Citations

Oct 24, 2019·The Journal of Chemical Physics·Alexander Benderskii, Akihiro Morita
Sep 3, 2021·The Review of Scientific Instruments·Xinting LiuXueming Yang
Oct 15, 2021·The Journal of Physical Chemistry Letters·Taegon LeeMinhaeng Cho

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