In this Tutorial series, we aim to provide an accessible introduction to vibrational sum frequency generation (VSFG) spectroscopy, targeted toward people entering the VSFG world without a rigorous formal background in optical physics or nonlinear spectroscopy. In this article, we discuss in detail the processes of collecting and processing VSFG data, and user-friendly processing software (sfgtools) is provided for use by people new to the field. Some discussion of analyzing VSFG spectra is also given, specifically with a discussion of fitting homodyne VSFG spectra, and a discussion of what can be learned (both qualitatively and quantitatively) from VSFG spectra.
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Frequency-Dependent Vibrational Relaxation Time of OH Stretch at the Air/Isotopically Diluted Water Interface.
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Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198, Japan.
Elucidation of the vibrational relaxation process of interfacial water is indispensable for understanding energy dissipation at the aqueous interface. In this study, the vibrational relaxation dynamics of the hydrogen-bonded OH (HB OH) stretch vibration was investigated at the air/isotopically diluted water (HOD-DO) interface by time-resolved heterodyne-detected vibrational sum frequency generation (TR-HD-VSFG) spectroscopy. We observed the temporal change of the excited-state band ( = 1 → 2 transition), which enables a reliable determination of the time of interfacial water.
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Nanophotonics
January 2025
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Sum-frequency generation (SFG) enables the coherent upconversion of electromagnetic signals and plays a significant role in mid-infrared vibrational spectroscopy for molecular analysis. Recent research indicates that plasmonic nanocavities, which confine light to extremely small volumes, can facilitate the detection of vibrational SFG signals from individual molecules by leveraging surface-enhanced Raman scattering combined with mid-infrared laser excitation. In this article, we compute the degree of second order coherence ( (0)) of the upconverted mid-infrared field under realistic parameters and accounting for the anharmonic potential that characterizes vibrational modes of individual molecules.
View Article and Find Full Text PDFRevealing the Water Structure at Neutral and Charged Graphene/Water Interfaces through Quantum Simulations of Sum Frequency Generation Spectra.
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Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, United States.
The structure and dynamics of water at charged graphene interfaces fundamentally influence molecular responses to electric fields with implications for applications in energy storage, catalysis, and surface chemistry. Leveraging the realism of the MB-pol data-driven many-body potential and advanced path-integral quantum dynamics, we analyze the vibrational sum frequency generation (vSFG) spectrum of graphene/water interfaces under varying surface charges. Our quantum simulations reveal a distinctive dangling OH peak in the vSFG spectrum at neutral graphene, consistent with recent experimental findings yet markedly different from those of earlier studies.
View Article and Find Full Text PDFFrom Antibacterial Activity to Molecular Mechanism: Case Study of Hexapeptide RWWRWW and Its Analogues.
Chembiochem
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Southeast University, School of Biological Science and Medical Engineering, 2 Sipailou, Xuanwu District, 210096, Nanjing, CHINA.
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View Article and Find Full Text PDFOrdered Interfacial Water Generated at Poly(ionic liquid) Membrane Surface Imparts Ultrafast Water Transport and Superoleophobicity.
J Am Chem Soc
January 2025
School of Rare Earths, University of Science and Technology of China, Hefei 230026, China.
Achieving ultrahigh permeance and superoleophobicity is crucial for membrane application. Here, we demonstrated that a poly(ionic liquid)/PES hydrogel membrane can achieve dual goals. The high polarity of the ionic liquids induces the water molecules on the membrane surface to be arranged more ordered, as verified by molecular dynamics (MD) simulation and advanced femtosecond sum frequency generation (SFG) vibrational spectroscopy.
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