Discovery of conical intersection mediated photochemistry with growing string methods
文献情報
Cody Aldaz, Joshua A. Kammeraad, Paul M. Zimmerman
Conical intersections (CIs) are important features of photochemistry that determine yields and selectivity. Traditional CI optimizers require significant human effort and chemical intuition, which typically restricts searching to only a small region of the CI space. Herein, a systematic approach utilizing the growing string method is introduced to locate multiple CIs. Unintuitive MECI are found using driving coordinates that can be generated using a combinatorial search, and subsequent optimization allows reaction pathways, transition states, products, and seam-space pathways to be located. These capabilities are demonstrated by application to two prototypical photoisomerization reactions and the dimerization of butadiene. In total, many reaction pathways were uncovered, including the elusive stilbene hula-twist mechanism, and a previously unidentified product in butadiene dimerization. Overall, these results suggest that growing string methods provide a predictive strategy for exploring photochemistry.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.














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