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Condensed-phase isomerization through tunnelling gateways.

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Quantum mechanical tunneling, crucial in condensed-phase chemistry, shows surprising nonmonotonic mass dependence. Specific "gateways" between reactant and product states enhance tunneling, even for heavier particles.

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Area of Science:

  • Physical Chemistry
  • Quantum Mechanics
  • Surface Science

Background:

  • Quantum mechanical tunneling allows particles to traverse energy barriers higher than their energy.
  • Particle mass influences tunneling efficiency; lighter particles typically tunnel more effectively.
  • Condensed-phase reactions involve transitions between bound states, differing from textbook continuum state models.

Purpose of the Study:

  • To investigate the nonmonotonic mass dependence of tunneling rates in condensed-phase reactions.
  • To develop a quantum rate theory explaining tunneling through bound states.
  • To explore the role of environmental interactions and specific state transitions in tunneling.

Main Methods:

  • Experimental measurement of isotopologue-specific tunneling rates for CO rotational isomerization on an NaCl surface.
  • Development of a quantum rate theory incorporating environmental interactions and bound-state transitions.
  • Identification of specific 'gateway' states that facilitate enhanced tunneling.

Main Results:

  • Observed nonmonotonic mass dependence of tunneling rates, contradicting simple mass-tunneling relationships.
  • Demonstrated that tunneling is fastest through specific 'gateway' states, enhancing cross-barrier coupling.
  • Showcased that these gateways accelerate ground-state isomerization, acting as efficient pathways.

Conclusions:

  • A quantum rate theory accounting for bound-state transitions and environmental interactions explains observed tunneling phenomena.
  • The concept of 'gateways' provides a framework for understanding enhanced tunneling, including for heavier particles.
  • Heavy-atom tunneling may be more significant in condensed-phase chemistry than previously assumed.