Photo-induced processes play key roles in photovoltaics and photocatalysis. They require understanding of material’s dynamical response to photo-excitation on atomic and nanometer scales. Our non-adiabatic molecular dynamics techniques,1 implemented within time-dependent density functional theory,2-4 allow us to model such non-equilibrium response in real time. The focus is on several classes of nanoscale interfaces, involving semiconducting5-8 and metallic9 quantum dots, polymers,8 hybrid perovskites,10,11 graphene,12 MoS213 and related two-dimensional materials,14 TiO2,10,12,15 etc.6 Charge and energy transport, Auger-type processes, energy losses and charge recombination create many challenges due to stark differences between molecular and periodic, and organic and inorganic matter. Our simulations provide a unifying description of quantum dynamics on the nanoscale, characterize rates and branching ratios of competing processes, resolve debated issues, and generate theoretical guidelines for development of novel systems for solar energy utilization. 1. Wang, L. J.; Akimov, A.; Prezhdo, O. V. J. Phys. Chem. Lett. 2016, 7, 2100. 2. Akimov, A. V.; Prezhdo, O. V. J. Chem. Theory Comput. 2013, 9, 4959. 3. Akimov, A. V.; Prezhdo, O. V. J. Chem. Theory Comput. 2014, 10, 789. 4. Pal, S.; Trivedi, D. J.; Akimov, A. V.; Aradi, B.; Frauenheim, T.; Prezhdo, O. V. J. Chem. Theory Comput. 2016, 12, 1436. 5. Pal, S.; Nijjar, P.; Frauenheim, T.; Prezhdo, O. V. Nano Lett. 2017, 17, 2389. 6. Dong, S.; Pal, S.; Lian, J.; Chan, Y.; Prezhdo, O. V.; Loh, Z. H. ACS Nano 2016, 10, 9370. 7. Dong, S.; Trivedi, D.; Chakrabortty, S.; Kobayashi, T.; Chan, Y.; Prezhdo, O. V.; Loh, Z. H. Nano Lett. 2015, 15, 6875. 8. Long, R.; Prezhdo, O. V. Nano Lett. 2015, 15, 4274. 9. Ranasingha, O.; Wang, H.; Zobac, V.; Jelinek, P.; Panapitiya, G.; Neukirch, A. J.; Prezhdo, O. V.; Lewis, J. P. J. Phys. Chem. Lett. 2016, 7, 1563. 10. Long, R.; Prezhdo, O. V. ACS Nano 2015, 9,11143. 11. Long, R.; Fang, W. H.; Prezhdo, O. V. J. Phys. Chem. Lett. 2016, 7, 3215. 12. Long, R.; Casanova, D.; Fang, W. H.; Prezhdo, O. V. J. Am. Chem. Soc. 2017, 139, 2619. 13. Li, L. Q.; Long, R.; Prezhdo, O. V. Chem. Mat. 2017, 29, 2466. 14. Chaban, V. V.; Fileti, E. E.; Prezhdo, O. V. ACS Nano 2017, 11, 6459. 15. Chu, W. B.; Saidi, W. A.; Zheng, Q. J.; Xie, Y.; Lan, Z. G.; Prezhdo, O. V.; Petek, H.; Zhao, J. J. Am. Chem. Soc. 2016, 138,13740. 16. Akimov, A. V.; Asahi, R.; Jinnouchi, R.; Prezhdo, O. V. J. Am. Chem. Soc. 2015, 137,11517.

Excited state dynamics at nanoscale interfaces for solar energy harvesting: Time-domain Ab initio studies

255th National Meeting (2018)

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