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Abstract
We report the first sub-1 cm⁻¹ resolution high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS) ssp intensity spectra of the air/neat-water interface across the 1500–3900 cm⁻¹ spectral range. Utilizing a direct fitting approach, we reconstruct the phase-resolved spectra that quantitatively agree with previously reported phase-resolved measurements while revealing additional spectral features and phase information. This combined analysis advances molecular-level understanding of water’s vibrational dynamics and orientation at the interface. Our results establish a robust framework linking intensity and phase-resolved SFG data, providing a foundation for future polarization and experimental configuration dependent studies aimed at resolving ongoing debates regarding interfacial water structure.
Supplementary materials
Title
Supplementary Materials for Quantitative consistency between the intensity and phase-resolved Sum Frequency Generation Vibrational Spectra of the air/neat-water interface
Description
Content
S1. Experimental
S1-A. Sub-1 cm-1 High Resolution Broadband Sum-Frequency Generation Vibrational Spectroscopy (HR-BB-SFG-VS)
S1-B. Sample preparation and spectra acquisition
S1-C. Data processing: normalization and fitting
S2. Spectra processing and reliability of fitting
S2-A. HR-BB-SFG-VS spectrum of the air/neat-water interface
S2-B. The normalized ssp spectra and the spectral profiles
S2-C. spectrum can be adequately fitted with 7 Lorentzian peaks
S2-D. Imaginary and real spectral using the fitting parameters
S2-E. Non-resonant imaginary term is insignificant
S3. Comparison with previously reported SFG-VS and PR-SFG-VS data
S3-A. Comparing HR-BB-SFG-VS data and Eric Tyrode Group’s 3 cm-1 resolution data
S3-B. Comparing HR-BB-SFG-VS data and PR-SFG-VS data from Wen and Tahara Group
S4. List of SFG papers on the Air/Neat-water Interface
References
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