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Scanning-probe Single-electron Capacitance Spectroscopy
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Published on: July 30, 2013

Carbon tunneling from a single quantum state.

Peter S Zuev1, Robert S Sheridan, Titus V Albu

  • 1Department of Chemistry 216, University of Nevada, Reno, NV 89557, USA.

Science (New York, N.Y.)
|February 8, 2003
PubMed
Summary

Carbon tunneling drives the ring expansion of 1-methylcyclobutylfluorocarbene at low temperatures. This quantum effect significantly dominates the reaction rate, even at 8 Kelvin.

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Area of Science:

  • Physical Chemistry
  • Quantum Mechanics
  • Chemical Kinetics

Background:

  • Carbene reactions are fundamental in organic chemistry.
  • Quantum tunneling can significantly influence reaction rates at low temperatures.
  • Understanding low-temperature reaction dynamics is crucial for various chemical processes.

Purpose of the Study:

  • To investigate the ring expansion mechanism of 1-methylcyclobutylfluorocarbene at 8 Kelvin.
  • To quantify the role of carbon tunneling in this reaction.
  • To explore the influence of inert-gas matrices on reaction rates.

Main Methods:

  • Low-temperature experimental observations at 8 Kelvin.
  • Kinetic measurements of carbene ring expansion in nitrogen and argon matrices.
  • Computational calculations to determine reaction pathways and contributions.

Main Results:

  • Observed ring expansion of 1-methylcyclobutylfluorocarbene.
  • Measured rate constants of 4.0 x 10(-6) s⁻¹ in nitrogen and 4 x 10(-5) s⁻¹ in argon.
  • Calculations showed tunneling contribution is 152 orders of magnitude greater than barrier passage.

Conclusions:

  • Carbon tunneling is the dominant mechanism for this reaction at 8 Kelvin.
  • The reaction proceeds from a single quantum state, leading to a temperature-independent rate.
  • The surrounding inert-gas matrix environment affects the reaction rate.