Quantum Dynamics Simulations of Interfacial Electron Transfer in Sensitized TiO2 Semiconductors
Citations Over TimeTop 10% of 2003 papers
Abstract
Ab initio DFT molecular dynamics simulations are combined with quantum dynamics calculations of electronic relaxation to investigate the interfacial electron transfer in catechol/TiO(2)-anatase nanostructures under vacuum conditions. It is found that the primary process in the interfacial electron-transfer dynamics involves an ultrafast (tau(1) approximately 6 fs) electron-injection event that localizes the charge in the Ti(4+) surface ions next to the catechol adsorbate. The primary event is followed by charge delocalization (i.e., carrier diffusion) through the TiO(2)-anatase crystal, an anisotropic diffusional process that can be up to an order of magnitude slower along the [-101] direction than carrier relaxation along the [010] and [101] directions in the anatase crystal. It is shown that both the mechanism of electron injection and the time scales for interfacial electron transfer are quite sensitive to the symmetry of the electronic state initially populated in the adsorbate molecule. The results are particularly relevant to the understanding of surface charge separation in efficient mechanisms of molecular-based photovoltaic devices.
Related Papers
- → Forming delocalized intermediate states with realistic quantum dots(2012)9 cited
- → On the synthesis of nanostructured TiO2 anatase phase and the development of the photoelectrochemical solar cell(1999)22 cited
- → A study on the interaction of V2O5/TiO2 (anatase) by high-resolution electron microscopy (hrem)(1986)50 cited
- → GROWTH, SURFACE CHARACTERIZATION, AND REACTIVITY OF TIO2 ANATASE FILMS-EPSCOR(2004)
- Carrier dynamics properties of delocalized states in GaN_xAs_(1-x)(2009)