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On the Dynamics through a Conical Intersection.

Basile F E Curchod1, Federica Agostini2

  • 1Centre for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, United Kingdom.

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Summary
This summary is machine-generated.

Conical intersections are key to ultrafast deactivation in photoexcited molecules. The exact factorization formalism reveals time-dependent potentials that, while not topologically distinct at intersections, capture complex nuclear wavepacket dynamics.

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Area of Science:

  • Quantum chemistry
  • Molecular dynamics
  • Photochemistry

Background:

  • Conical intersections are crucial topological features on molecular potential energy surfaces.
  • They facilitate ultrafast nonradiative deactivation pathways for photoexcited molecules.
  • The exact factorization (XF) formalism offers an alternative to the Born-Oppenheimer approximation for molecular quantum dynamics.

Purpose of the Study:

  • To investigate the behavior of time-dependent potentials within the exact factorization formalism during dynamics through a conical intersection.
  • To explore the nature of time-dependent potential energy surfaces and time-dependent vector potentials in the context of conical intersections.
  • To compare the insights gained from the XF formalism with the traditional Born-Oppenheimer framework.

Main Methods:

  • Application of the exact factorization formalism to a two-dimensional model system.
  • Simulating the dynamics of a photoexcited molecule passing through a conical intersection.
  • Analysis of the time-dependent potential energy surface and time-dependent vector potential.

Main Results:

  • The time-dependent potential energy surface and time-dependent vector potential do not display unique topological features at the conical intersection.
  • These XF quantities effectively capture the complex dynamics of the nuclear wavepacket in the vicinity of the conical intersection.
  • The behavior of these time-dependent quantities provides a different perspective on the funneling effect at conical intersections.

Conclusions:

  • The exact factorization formalism provides a valuable, albeit different, perspective on molecular dynamics at conical intersections compared to the Born-Oppenheimer approximation.
  • While lacking distinct topological signatures, the time-dependent potentials in XF are sensitive to the intricate nuclear motion through these critical regions.
  • This study highlights the utility of the XF formalism for understanding ultrafast processes in photochemistry.