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Conical intersections and bound molecular states embedded in the continuum.

Lorenz S Cederbaum1, Ronald S Friedman, Victor M Ryaboy

  • 1Theoretische Chemie, Physikalisch-Chemisches Institut Universität Heidelberg, D-69120 Heidelberg, Germany. Lorenz.Cederbaum@urz.uni-heidelberg.de

Physical Review Letters
|February 7, 2003
PubMed
Summary

Bound states in the continuum exist due to non-Born-Oppenheimer effects in nuclear dynamics. Coupling between electronic states suppresses potential tunneling, preventing decay and stabilizing these unique quantum states.

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Area of Science:

  • Quantum mechanics
  • Chemical physics
  • Molecular dynamics

Background:

  • Bound states embedded in the continuum (BICs) are unusual quantum phenomena.
  • Conical intersections in potential energy surfaces are critical for understanding molecular behavior.
  • Non-Born-Oppenheimer effects are crucial for describing coupled nuclear and electronic motion.

Purpose of the Study:

  • To provide an explicit proof for the existence of bound states embedded in the continuum in a specific conical intersection scenario.
  • To elucidate the role of non-Born-Oppenheimer effects in the formation and stability of these states.
  • To investigate the decay mechanisms and suppression of tunneling in such systems.

Main Methods:

  • Theoretical analysis of nuclear dynamics on coupled potential energy surfaces.

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  • Explicit mathematical proof for the existence of bound states.
  • Investigation of the impact of the Born-Oppenheimer approximation.
  • Numerical simulation to illustrate the suppression of potential tunneling.

    • Main Results:

    • Demonstrated the existence of bound states embedded in the continuum for a specific conical intersection.
    • Identified non-Born-Oppenheimer effects as the mechanism responsible for binding these states.
    • Showed that these states become resonances decaying via potential tunneling under the Born-Oppenheimer approximation.
    • Confirmed that coupling between electronic states completely suppresses tunneling, preserving the bound nature of the states.

    Conclusions:

    • Non-Born-Oppenheimer effects are essential for the existence of bound states embedded in the continuum in the studied system.
    • Electronic state coupling effectively prevents decay through potential tunneling, stabilizing these states.
    • The findings offer insights into quantum phenomena at conical intersections and the limitations of the Born-Oppenheimer approximation.