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Updated: May 13, 2026

In situ FTIR Spectroscopy as a Tool for Investigation of Gas/Solid Interaction: Water-Enhanced CO2 Adsorption in UiO-66 Metal-Organic Framework
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Published on: February 1, 2020

Fermi resonance in solid CO2 under pressure.

Olaseni Sode1, Murat Keçeli, Kiyoshi Yagi

  • 1Department of Chemistry, University of Illinois at Urbana-Champaign, 600 South Mathews Avenue, Urbana, Illinois 61801, USA.

The Journal of Chemical Physics
|March 1, 2013
PubMed
Summary
This summary is machine-generated.

Carbon dioxide's (CO2) Fermi resonance Raman bands shift with pressure. This study accurately models these shifts, confirming the ν1 > 2ν2 frequency order, crucial for CO2 spectroscopy.

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Area of Science:

  • Physics
  • Chemistry
  • Spectroscopy

Background:

  • Carbon dioxide (CO2) exhibits Fermi resonance between its symmetric-stretching fundamental (ν1) and bending first overtone (2ν2).
  • This resonance results in two observable Raman bands with a specific frequency difference and intensity ratio.
  • These spectral features are pressure-dependent and have been used as a geobarometer for CO2 inclusions in minerals.

Purpose of the Study:

  • To computationally investigate the pressure dependence of the Fermi dyad frequency difference and intensity ratio in CO2.
  • To validate theoretical models against experimental observations up to 10 GPa.
  • To resolve the long-standing controversy regarding the unperturbed frequency order (ν1 vs. 2ν2).

Main Methods:

  • Combined embedded-fragment second-order Møller-Plesset perturbation (MP2) calculations for solid CO2 harmonic frequencies under pressure.
  • Coupled-cluster singles and doubles with noniterative triples (CCSD(T)) and vibrational configuration interaction (VCI) calculations for molecular CO2 anharmonic frequencies.
  • Analysis of pressure-induced variations in frequency difference and intensity ratio.

Main Results:

  • The study quantitatively reproduced the pressure-dependent frequency difference of the CO2 Fermi dyad.
  • Qualitative agreement was achieved for the intensity ratio up to 10 GPa.
  • The calculations strongly support the ν1 > 2ν2 ordering of unperturbed frequencies in both gas and solid phases.

Conclusions:

  • The theoretical approach accurately models the pressure-dependent spectral behavior of the CO2 Fermi dyad.
  • The findings provide robust evidence for the ν1 > 2ν2 frequency ordering, settling a decades-old debate.
  • This work enhances the understanding and application of CO2 spectroscopy in condensed phases and geobarometry.