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Hydrogen Bonds under Electric Fields with Quantum Accuracy.

Alessandro Amadeo1,2, Marco Francesco Torre2, Klaudia Mráziková3,4

  • 1Department of Chemistry, Biology and Biotechnologies, University of Perugia, Via dell'Elce di sotto, 8, 06123 Perugia, Italy.

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Electric fields strengthen hydrogen bonds in water, HF, H2S, and NH3 dimers. This study reveals how these fields impact molecular structure, vibrations, and energies, with implications for catalysis and hydrogen technologies.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Molecular Spectroscopy

Background:

  • Hydrogen bonds (H-bonds) are fundamental to chemical and biological systems.
  • External perturbations, such as electric fields, can significantly alter H-bond properties.
  • Understanding these alterations is crucial for applications in catalysis and energy.

Purpose of the Study:

  • To investigate the effects of static and homogeneous electric fields (EFs) on H-bonded dimers (water, HF, H2S, NH3) and their monomers.
  • To elucidate field-induced modifications in structural, vibrational, and energetic properties.
  • To analyze charge-transfer mechanisms and intermolecular interactions under EFs.

Main Methods:

  • Employed the explicitly correlated singles and doubles coupled cluster method (CCSD) for equilibrium geometries and harmonic vibrational frequencies.
  • Utilized the perturbative triples CCSD(T) method for energy calculations.
  • Applied symmetry-adapted perturbation theory (SAPT) for dimer analysis and perturbation theory for vibrational Stark effect calculations.

Main Results:

  • Electric fields induce geometry relaxation in monomers, primarily governed by dipole derivatives.
  • A universal strengthening of intermolecular interactions was observed with increasing field intensity.
  • Electrostatics dominate H-bond stabilization, with induction contributions increasing at higher fields, especially in polarizable systems.

Conclusions:

  • Electric fields significantly modulate H-bond properties, including lengths, binding energies, and vibrational frequencies (vibrational Stark effect).
  • A direct correlation exists between binding energies, vibrational Stark effect, and charge-transfer energy terms across investigated dimers.
  • Findings offer insights into EF-driven H-bond modulation, relevant for catalysis, hydrogen technologies, and biological processes.