Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 11, Pages 2676-2683Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b00987
Keywords
-
Categories
Funding
- POSCO Science Fellowship of the POSCO TJ Park Foundation
- National Research Foundation (NRF) - Korean government [2016R1A2B4012337]
- KISTI supercomputing center through the strategic program for the supercomputing application research [KSC-2018-CHA-0025]
- U.S. Department of Energy [DE-SC0014429]
Ask authors/readers for more resources
Oxygen vacancies in TiO2 nanoparticles are important for charge carrier dynamics, with recent studies reporting contradictory results on TiO2 nanoparticle photocatalytic activity. We demonstrate that ground state multiplicity, defect levels, and formation energies depend strongly on vacancy location. Quantum dynamics simulations show that charges are trapped within several picoseconds and recombine over a broad range of time scales from tens of picoseconds to nanoseconds. Specifically, nanoparticles with missing partially coordinated surface oxygens showed fast recombination, while nanoparticles with missing highly coordinated subsurface oxygens or singly coordinated oxygens at tips showed slow recombination, even slower than in the pristine system. The results are rationalized by energy gaps and electron-hole localization, the latter determining nonadiabatic coupling and quantum coherence time. The diverse charge recombination scenarios revealed by the nonadiabatic dynamics simulations rationalize the contradictory experimental results for photocatalytic activity and provide guidelines for rational design of nanoscale metal oxides for solar energy harvesting and utilization.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available