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Classical Electrostatic Interaction Is the Origin for Blue-Shifting Halogen Bonds.

Changwei Wang1, Yirong Mo2

  • 1Key Laboratory for Macromolecular Science of Shaanxi Province, School of Chemistry and Chemical Engineering , Shaanxi Normal University , Xi'an 710119 , China.

Inorganic Chemistry
|June 12, 2019
PubMed
Summary
This summary is machine-generated.

Blue-shifting halogen bonds, where the bond contracts, are explained by electrostatic interactions, not charge transfer. This finding clarifies the nature of these bonds and their behavior under external electric fields.

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Area of Science:

  • Chemical Physics
  • Computational Chemistry
  • Molecular Interactions

Background:

  • Halogen bonds (D···X-A) involve charge transfer (CT) and electrostatic interactions, with debate on their relative importance.
  • CT interactions typically weaken and lengthen the X-A bond, contrasting with the observed blue-shifting phenomenon.

Purpose of the Study:

  • To investigate the underlying mechanisms of blue-shifting halogen bonds.
  • To elucidate the roles of electrostatic and charge transfer interactions in H₃N···ClNO₂ and analogous systems.

Main Methods:

  • Utilized the block-localized wave function (BLW) method for energy decomposition analysis.
  • Explored energy profiles along halogen-bonding distances.
  • Applied external electric fields to observe transitions in bond behavior.

Main Results:

  • Electrostatic interactions were identified as the dominant factor driving the blue-shifting of X-N bonds.
  • Replacing NH₃ with point charges yielded similar blue-shifting magnitudes, supporting the electrostatic dominance.
  • An external electric field induced a blue-to-red shifting transition due to enhanced polarization and CT interactions.

Conclusions:

  • Classical electrostatic attraction governs blue-shifting halogen bonds.
  • The interplay between electrostatic, polarization, and CT interactions dictates bond behavior under external fields.
  • Force analysis confirmed the roles of individual energy components in these interactions.