Journal
FARADAY DISCUSSIONS
Volume 216, Issue -, Pages 476-493Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8fd00228b
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Funding
- Leverhulme Trust [RPG-2016-055]
- Engineering and Physical Sciences Research Council [EP/R020477/1]
- Energy Global Research Priority at the University of Warwick
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The ground-up design of new molecular sunscreens, with improved photostability, absorbance and spectral coverage, stands as a challenge to fundamental chemical science. Correlating sunscreen molecular structure and function requires detailed insight into the relaxation pathways available following photoexcitation; however, the complex coupled electron/nuclear dynamics in these systems stands as a tough challenge to computational chemistry. To address this challenge, we have recently developed efficient and accurate simulation methods to model non-adiabatic dynamics of general molecular systems as a route to correlating photoinduced dynamics and potential sunscreen activity. Our approach, combining the multi-configuration time-dependent Hartree (MCTDH) method with PESs generated using machine-learning, represents a new on-the-fly strategy for accurate wavefunction propagation, with the potential to provide a new black box strategy for interrogating ultrafast dynamics in general photoinduced energy transport processes. Here, we illustrate our attempts to apply this methodology to study the ultrafast photochemistry of four compounds derived from mycosporine-like amino acids (MAAs), compounds which are believed to act as microbial sunscreens in micro-organisms such as algae. Specifically, we investigate how the choice of active vibrational space and diabatic electronic states in MCTDH strongly influences the predictions of ultrafast dynamic relaxation in representative MAAs. Our results serve to demonstrate that on-the-fly quantum dynamics using MCTDH is increasingly viable, but important barriers relating to coordinate choices and diabatisation remain.
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