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Updated: Oct 25, 2026

Multimodal Nonlinear Hyperspectral Chemical Imaging Using Line-Scanning Vibrational Sum-Frequency Generation Microscopy
Published on: December 1, 2023
Integrating Local and Normal Modes for Multilevel Vibrational Spectroscopy
Vincenzo Barone1, Luigi Crisci2, Federico Lazzari2
1National Interuniversity Consortium for Materials Science and Technology (INSTM) , Via G. Giusti 9, 50121Firenze, Italy.
Abstract:
We present a multilevel strategy for harmonic vibrational spectroscopy in which a lower cost calculation supplies the complete coupled force field and higher level energy calculations refine selected curvatures. Symmetry-oriented non-redundant internal coordinates retain chemical identity and coupling topology, while concordant normal-mode directions provide an efficient frequency end point. Their sequential use improves mode shapes without requiring a higher level Hessian. Across four validation fixtures, the local-coordinate models recover unsupplied coupling correlations of 0.987-0.999; the complete sequence uses at most 2N independent higher level curvatures for N normal modes.
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