First Principles Dynamics Study of Excited Hole Relaxation in DNA
| العنوان: | First Principles Dynamics Study of Excited Hole Relaxation in DNA |
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| المؤلفون: | Jian Cheng Wong, Yosuke Kanai |
| المصدر: | ChemPhysChem. 23 |
| بيانات النشر: | Wiley, 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | Physics, Relaxation (NMR), Surface hopping, DNA, Molecular physics, Atomic and Molecular Physics, and Optics, Dissociation (psychology), Ion, Picosecond, Excited state, Ionization, medicine, Physical and Theoretical Chemistry, medicine.symptom, Order of magnitude |
| الوصف: | A recent theoretical work showed that ion irradiation generates excited holes deep within the valence band of DNA. In this work, we investigate the excited hole relaxation toward HOMO using a first-principles computational method following such ionization events. The excited hole relaxation is found to depend significantly on the energetic position of the excited hole generated. The relaxation process is found to be an order of magnitude slower for holes that are generated deeper than 20 eV than those generated within 10 eV, where the probability for the initial ionization events is the highest. However, the excited holes that are generated in different spatial moieties such as DNA nucleotide bases and phosphate backbones do not show noticeable differences in terms of the relaxation time. Our work also shows that decoherence due to nuclei dynamics slows down the relaxation by a factor of two or more. At the same time, the relaxation time is found to be less than a couple of picoseconds, much shorter than typical timescales associated with chemical bond dissociation. |
| تدمد: | 1439-7641 1439-4235 |
| DOI: | 10.1002/cphc.202100521 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::61686d274baf08afb73c0abb3b16b18e https://doi.org/10.1002/cphc.202100521 |
| Rights: | CLOSED |
| رقم الانضمام: | edsair.doi.dedup.....61686d274baf08afb73c0abb3b16b18e |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 14397641 14394235 |
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| DOI: | 10.1002/cphc.202100521 |