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arXiv · 1310.2929

Geometric phase effects in low-energy dynamics near conical intersections: A study of the multidimensional linear vibronic coupling model

Loic Joubert-Doriol·Ilya G. Ryabinkin·Artur F. Izmaylov
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Abstract

In molecular systems containing conical intersections (CIs), a nontrivial geometric phase (GP) appears in the nuclear and electronic wave-functions in the adiabatic representation. We study GP effects in nuclear dynamics of an N-dimensional linear vibronic coupling (LVC) model. The main impact of GP on low-energy nuclear dynamics is reduction of population transfer between the local minima of the LVC lower energy surface. For the LVC model, we proposed an isometric coordinate transformation that confines non-adiabatic effects within a two-dimensional subsystem interacting with an N-2 dimensional environment. Since environmental modes do not couple electronic states, all GP effects originate from nuclear dynamics within the subsystem. We explored when the GP affects nuclear dynamics of the isolated subsystem, and how the subsystem-environment interaction can interfere with GP effects. Comparing quantum dynamics with and without GP allowed us to devise simple rules to determine significance of the GP for nuclear dynamics in this model.

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Loic Joubert-Doriol, Ilya G. Ryabinkin, Artur F. Izmaylov. 2013-10-10. Geometric phase effects in low-energy dynamics near conical intersections: A study of the multidimensional linear vibronic coupling model. https://doi.org/10.1063/1.4844095

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