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Discovery of conical intersection mediated photochemistry with growing string methods.

Cody Aldaz1, Joshua A Kammeraad, Paul M Zimmerman

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This study introduces a systematic growing string method to efficiently locate multiple conical intersections (CIs) in photochemistry. This approach overcomes limitations of traditional methods, enabling comprehensive exploration of reaction pathways and uncovering new chemical insights.

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Area of Science:

  • Computational Chemistry
  • Photochemistry
  • Chemical Dynamics

Background:

  • Conical intersections (CIs) are crucial in photochemistry, governing reaction yields and selectivity.
  • Traditional methods for locating CIs are labor-intensive and limit exploration to small regions.
  • A need exists for systematic and efficient methods to explore the complex CI space.

Purpose of the Study:

  • To introduce a systematic approach using the growing string method to locate multiple conical intersections.
  • To enable the discovery of non-intuitive minimum energy conical intersections (MECIs).
  • To facilitate the comprehensive mapping of photochemical reaction pathways.

Main Methods:

  • Utilizing the growing string method for systematic CI location.
  • Employing combinatorial search to generate driving coordinates for MECI discovery.
  • Applying subsequent optimization to identify reaction pathways, transition states, and products.

Main Results:

  • Successfully located multiple CIs and MECIs in prototypical photoisomerization reactions and butadiene dimerization.
  • Uncovered numerous reaction pathways, including the stilbene hula-twist mechanism.
  • Identified a previously unknown product in butadiene dimerization.

Conclusions:

  • The growing string method offers a predictive and systematic strategy for exploring photochemical reaction landscapes.
  • This approach significantly enhances the ability to discover and analyze complex photochemical processes.
  • The findings pave the way for more efficient and comprehensive studies in photochemistry.