Transferability and interpretability of vibrational normalizing-flow coordinates.

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Molecular Spectroscopy

Background:

• Vibrational coordinate choice impacts molecular calculation accuracy, efficiency, and interpretability.
• Traditional coordinates can introduce complexity, hindering basis set convergence and motion interpretation.

Purpose of the Study:

• To explore and analyze the utility, interpretation, and constraints of normalizing-flow vibrational coordinates.
• To demonstrate the generalizability of these coordinates across different molecular systems.

Main Methods:

• Utilizing recently proposed normalizing-flow vibrational coordinates.
• Developing molecule-specific coordinate transformations optimized for a given basis set.
• Analyzing the impact of these coordinates on basis-set convergence and interpretability.

Main Results:

• Normalizing-flow coordinates offload complexity from basis functions to the coordinate transformation.
• Improved basis-set convergence and enhanced interpretability of vibrational motions observed.
• Demonstrated generalizability across different isotopologues and structurally related molecules with minimal fine-tuning.

Conclusions:

• Normalizing-flow vibrational coordinates offer a promising approach for accurate and interpretable molecular vibrational calculations.
• These coordinates represent a significant advancement in computational chemistry for analyzing molecular dynamics and spectra.
• The generalizability suggests broad applicability in computational molecular science.