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Domino Tunneling.

Peter R Schreiner1, J Philipp Wagner1, Hans Peter Reisenauer1

  • 1⊥Institute of Organic Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 58, D-35392 Giessen, Germany.

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|June 2, 2015
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Summary
This summary is machine-generated.

Quantum mechanical tunneling drives sequential isomerization in oxalic acid rotamers at cryogenic temperatures. This "domino" tunneling mechanism, observed in matrix-isolation experiments, reveals complex kinetics even at near absolute zero.

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Area of Science:

  • Physical Chemistry
  • Quantum Mechanics
  • Spectroscopy

Background:

  • Oxalic acid exhibits multiple O-H rotamers with varying relative energies.
  • Understanding molecular transformations at cryogenic temperatures is crucial for various scientific fields.

Purpose of the Study:

  • To investigate the quantum mechanical tunneling phenomenon in oxalic acid rotamers.
  • To characterize the sequential isomerization cascade and its kinetics under matrix-isolation conditions.

Main Methods:

  • Matrix-isolation experiments conducted near 3 K.
  • State-of-the-art quantum chemical computations.
  • Infrared (IR) spectroscopy to monitor temporal evolution of rotamers.
  • Development of a general mathematical model for reaction cascade kinetics.

Main Results:

  • Observed a sequential isomerization cascade (1tTt → 1cTt → 1cTc) in oxalic acid rotamers.
  • Identified half-lives ranging from 30 to 360 hours, indicating tunneling across high energy barriers.
  • Revealed distinct classes of fast and slow matrix sites influencing decay rates.
  • Demonstrated agreement between experimental decay rates and theoretical tunneling rates.

Conclusions:

  • Oxalic acid exhibits a novel sequential quantum mechanical tunneling phenomenon.
  • A
  • domino
  • tunneling mechanism governs these transformations.
  • The developed mathematical model accurately describes complex kinetics in distinct matrix sites.