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Author: Mero, Mark × Subject: Interferometry ×

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    Compact, high-repetition-rate source for broadband sum-frequency generation spectroscopy
    (Melville, NY : AIP Publishing, 2017) Heiner, Zsuzsanna; Petrov, Valentin; Mero, Mark
    We present a high-efficiency optical parametric source for broadband vibrational sum-frequency generation (BB-VSFG) for the chemically important mid-infrared spectral range at 2800-3600 cm-1 to study hydrogen bonding interactions affecting the structural organization of biomolecules at water interfaces. The source consists of a supercontinuum-seeded, dual-beam optical parametric amplifier with two broadband infrared output beams and a chirped sum-frequency mixing stage providing narrowband visible pulses with adjustable bandwidth. Utilizing a pulse energy of only 60 μJ from a turn-key, 1.03-μm pump laser operating at a repetition rate of 100 kHz, the source delivers 6-cycle infrared pulses at 1.5 and 3.2 μm with pulse energies of 4.6 and 1.8 μJ, respectively, and narrowband pulses at 0.515 μm with a pulse energy of 5.0 μJ. The 3.2-μm pulses are passively carrier envelope phase stabilized with fluctuations at the 180-mrad level over a 10-s time period. The 1.5-μm beamline can be exploited to deliver pump pulses for time-resolved studies after suitable frequency up-conversion. The high efficiency, stability, and two orders of magnitude higher repetition rate of the source compared to typically employed systems offer great potential for providing a boost in sensitivity in BB-VSFG experiments at a reduced cost.
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    Vibrational sum-frequency generation spectroscopy of lipid bilayers at repetition rates up to 100 kHz
    (Melville, NY : American Institute of Physics, 2018) Yesudas, Freeda; Mero, Mark; Kneipp, Janina; Heiner, Zsuzsanna
    Broadband vibrational sum-frequency generation (BB-VSFG) spectroscopy has become a well-established surface analytical tool capable of identifying the orientation and structure of molecular layers. A straightforward way to boost the sensitivity of the technique could be to increase the laser repetition rate beyond that of standard BB-VSFG spectrometers, which rely on Ti:sapphire lasers operating at repetition rates of 1-5 kHz. Nevertheless, possible thermally induced artifacts in the vibrational spectra due to higher laser average powers are unexplored. Here, we discuss laser power induced temperature accumulation effects that distort the BB-VSFG spectra of 1,2-diacyl-sn-glycero-3-phosphocholine at an interface between two transparent phases at repetition rates of 5, 10, 50, and 100 kHz at constant pulse energy. No heat-induced distortions were found in the spectra, suggesting that the increase in the laser repetition rate provides a feasible route to an improved signal-to-noise ratio or shorter data acquisition times in BB-VSFG spectroscopy for thin films on transparent substrates. The results have implications for future BB-VSFG spectrometers pushing the detection limit for molecular layers with low surface coverage.