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At room temperature, the chair conformer of cyclohexane undergoes rapid ring flipping between two equivalent chair conformers at a rate of approximately 105 times per second. These two chair conformers are in equilibrium. The rapid ring flipping results in the interconversion of the axial proton to an equatorial proton and an equatorial to the axial proton. Such interconversions are too rapid and cannot be detected on the NMR timescale. Hence, the NMR spectrometer cannot distinguish between the...
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Double resonance techniques in Nuclear Magnetic Resonance (NMR) spectroscopy involve the simultaneous application of two different frequencies or radiofrequency pulses to manipulate and observe two distinct nuclear spins. One important application of double resonance is spin decoupling, which selectively suppresses coupling with one type of nucleus while observing the NMR signal from another nucleus, simplifying the spectrum and enhancing resolution.
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Ultrafast and Ultraslow Proton-Transfer Dynamics Induced by Formic Acid Dimer Ionization.

Saroj Barik1, Ester Livshits1,2, Roi Baer1,2

  • 1Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 9190401, Israel.

The Journal of Physical Chemistry. A
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Ultrafast proton transfer in formic acid dimers reveals a transient enhancement of protonated monomers. Ultraslow dynamics on the microsecond timescale were observed in the dimer cation, involving structural rearrangement and ion dissociation.

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Area of Science:

  • Chemical Physics
  • Physical Chemistry
  • Spectroscopy

Background:

  • Proton transfer in hydrogen-bonded dimers is crucial for understanding DNA radiation damage mechanisms.
  • The formic acid dimer serves as a model system for studying these dynamics.

Purpose of the Study:

  • To investigate the ultrafast proton-transfer dynamics in formic acid dimers after ionization.
  • To elucidate the mechanisms and timescales of subsequent fragmentation pathways.

Main Methods:

  • Ultrafast extreme-ultraviolet pump and near-infrared probe experiments.
  • Coincidence photofragment imaging technique.
  • Ab initio molecular dynamics simulations.

Main Results:

  • Observed a transient enhancement of the protonated monomer signal at 150 fs.
  • Revealed ultraslow microsecond dynamics of the metastable dimer cation.
  • Identified a barrier for structural rearrangement (HCOO to OCOH) in the deprotonated moiety.
  • Observed ultraslow dissociation channels for protonated monomer ions (e.g., H3O+, H2O).

Conclusions:

  • Concerted proton transfer and ring opening occur in a metastable dimer following ionization.
  • Ultraslow dynamics are attributed to a significant rearrangement barrier.
  • Dissociation of hot photoions involves complex hydrogen migration pathways.