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Dynamics at Conical Intersections.

Michael S Schuurman1,2, Albert Stolow1,2,3

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Summary
This summary is machine-generated.

Conical intersections (CIs) in excited molecules control energy flow and photochemistry. This study explores how molecular structure, via chemical substitution, influences the dynamics of passing through CIs, impacting reaction pathways.

Keywords:
conical intersectionelectronic structuremolecular dynamicsnonadiabaticphotochemistryphotoelectronsimulationspectroscopytransition stateultrafast

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Area of Science:

  • Physical Chemistry
  • Theoretical Chemistry
  • Spectroscopy

Background:

  • Nonadiabatic coupling between electronic and vibrational motion is key in excited polyatomic molecules.
  • Conical intersections (CIs) are now recognized as primary drivers of charge and vibrational energy flow in excited states.
  • Passage through CIs converts electronic to vibrational energy, initiating photochemistry like isomerization.

Purpose of the Study:

  • To investigate the dynamical aspects of passing through conical intersections (CIs) in excited states.
  • To explore analogies between excited-state CI dynamics and ground-state reaction dynamics.
  • To understand how chemical substitution affects the direction and velocity of approach to CIs.

Main Methods:

  • Comparison of time-resolved photoelectron spectroscopy (TR-PES) with on-the-fly ab initio multiple spawning (AIMS) calculations.
  • Phenomenological approach focusing on the excited-state dynamics of the C=C bond in unsaturated hydrocarbons.
  • Systematic chemical substitution (e.g., H to methyl group) to vary inertial and potential effects on CI approach.

Main Results:

  • Validation of both experimental TR-PES and theoretical AIMS methods through direct comparison.
  • Demonstration that chemical substituents introduce 'inertial effects' (altering approach direction/velocity) and 'potential effects' (modifying electronic structure and potential energy surfaces).
  • Observation of how these effects systematically influence the dynamics of approaching a CI.

Conclusions:

  • The direction and velocity of approach to a CI significantly influence excited-state dynamics and subsequent photochemistry.
  • Chemical substituents provide a means to tune these dynamical aspects, offering insights into reaction control.
  • There is a need for refined dynamical models and conceptual frameworks for understanding nonadiabatic dynamics at CIs.