Nuclear quadrupole moment-induced Cotton-Mouton effect in molecules

Area of Science:

• Physical Chemistry
• Quantum Chemistry
• Spectroscopy

Background:

• Nuclear magneto-optic effects are crucial for advanced spectroscopic and imaging techniques.
• These methods provide site-specific structural and dynamic information for molecules and materials.

Purpose of the Study:

• To formulate the nuclear quadrupole moment-induced Cotton-Mouton effect using first-principles electronic structure.
• To perform ab initio and density-functional theory calculations for various molecular liquids.

Main Methods:

• Response theory formulation for the Cotton-Mouton effect.
• Ab initio and density-functional theory (DFT) calculations.
• Analysis of basis-set convergence, electron correlation, and relativistic effects.

Main Results:

• Calculated Cotton-Mouton effect for H2O, CH3NO2, CH3CH2OH, C6H6, C6H12, HI, XeF2, WF5Cl, and Pt(C2dtp)2.
• Estimated ellipticities of 10(-3)-10(-7) rad/(M cm) for spin-polarized nuclei.
• Identified potential detectability with modern Voigt magneto-optic setups, especially for heavy nuclei.

Conclusions:

• The study provides a theoretical framework and computational evidence for nuclear quadrupole moment-induced Cotton-Mouton effects.
• The findings suggest experimental feasibility for high-sensitivity spectroscopy and imaging.
• Heavy nuclei are highlighted as promising targets for observable effects.