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<p>Molecular systems undergoing <i>Z/E</i> photoisomerizations are important as building blocks for light driven molecular machines. Understanding the effect of chemical substitution on the underlying mechanisms and the isomerization quantum yields is crucial for optimizing their functionality. In this study, we develop, implement, and evaluate the performance of the spin-flip time-dependent density-functional-based tight-binding (SF-TDDFTB) as a cost-effective approach for simulating the excited state potential energy surfaces of several photoisomerizing chromophores. By comparing the results with SF-TDDFTB with all-electron SF-TDDFT, MRSF-TDDFT, and XMS-CASPT2, we investigate the accuracy of the tight-binding formalism in capturing the correct potential energy surface leading to the <i>Z/E</i> photoisomerization pathways for well-known photoisomerization reactions of a protonated Schiff base, an oxidondole molecular motor, the green fluorescent protein chromophore, and a photodrug. Our findings demonstrate that the SF-TDDFTB method offers a balanced trade-off between computational efficiency and accuracy. These results pave the way for more efficient computational models for studying the <i>Z/E</i> photoisomerization reactions of complex molecular systems.</p>

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Assessing spin-flip time-dependent density-functional-based tight-binding for describing Z/E photoisomerization reactions

  • 期刊论文

  • 发表日期：

    2025年5月24日

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  • Miquel Huix-Rotllant,
  • Woojin Park,
  • Mohsen Mazaherifar,
  • Cheol Ho Choi

摘要

Molecular systems undergoing Z/E photoisomerizations are important as building blocks for light driven molecular machines. Understanding the effect of chemical substitution on the underlying mechanisms and the isomerization quantum yields is crucial for optimizing their functionality. In this study, we develop, implement, and evaluate the performance of the spin-flip time-dependent density-functional-based tight-binding (SF-TDDFTB) as a cost-effective approach for simulating the excited state potential energy surfaces of several photoisomerizing chromophores. By comparing the results with SF-TDDFTB with all-electron SF-TDDFT, MRSF-TDDFT, and XMS-CASPT2, we investigate the accuracy of the tight-binding formalism in capturing the correct potential energy surface leading to the Z/E photoisomerization pathways for well-known photoisomerization reactions of a protonated Schiff base, an oxidondole molecular motor, the green fluorescent protein chromophore, and a photodrug. Our findings demonstrate that the SF-TDDFTB method offers a balanced trade-off between computational efficiency and accuracy. These results pave the way for more efficient computational models for studying the Z/E photoisomerization reactions of complex molecular systems.