Hostname: page-component-cd9895bd7-p9bg8 Total loading time: 0 Render date: 2024-12-27T01:52:50.113Z Has data issue: false hasContentIssue false
  • English
  • Français

ATOMISTIC SIMULATION OF DISSIPATIVE CHARGE CARRIER DYNAMICS FOR PHOTOCATALYSIS

Published online by Cambridge University Press:  10 May 2012

Talgat M. Inerbaev ,
Dmitri S. Kilin  and
James Hoefelmeyer
Talgat M. Inerbaev
Affiliation:
Gumilyov Eurasian National University, Astana, Munaitpasov st. 5, 010008, Kazakhstan
Dmitri S. Kilin
Affiliation:
Department of Chemistry, University of South Dakota, Vermillion SD 57069, USA
James Hoefelmeyer
Affiliation:
Department of Chemistry, University of South Dakota, Vermillion SD 57069, USA
Get access

Abstract

Photo-excitation of high surface area semiconductor nanorods decorated with surface catalyst particles are investigated. DFT-based simulation is applied to the charge transfer dynamics at the interface of the supported nanocatalyst by modeling dynamics of photo-excitations. The modeling is performed by reduced density matrix method in the basis of Kohn-Sham orbitals. The energy of photo-excitation is dissipating due to interaction with lattice vibrations, treated through non-adiabatic coupling as the electron/hole pair relaxes to the conduction / valence band edges. The methodology is applied to TiO2 nanorod modeled as a periodic anatase (100) slab functionalized by minimalistic nano-clusters or doping. Simulations of these models demonstrate the formation of charge transfer state in both time and frequency domain. Computed charge dynamics leads to creation of positively charged areas on the nanorod surface that is an important prerequisite for oxidation catalysis. Our computation identifies optimal composition and morphology of nanocatalyst for such applications as water splitting for hydrogen production or solar cells.

Keywords

catalyticnanoscalesurface reaction
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1390: Symposium H/I – Organic Photovoltaics–Materials to Devices , 2012 , mrsf11-1390-i03-03
Copyright
Copyright © Materials Research Society 2012

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Kilin, D.S. and Micha, D.A., Relaxation of Photoexcited Electrons at a Nanostructured Si(111) Surface. Journal of Physical Chemistry Letters, 2010. 1(7): p. 1073–1077.Google Scholar
2. Kilin, D.S. and Micha, D.A., Modeling the Photovoltage of Doped Si Surfaces. Journal of Physical Chemistry C, 2011. 115(3): p. 770–775.Google Scholar
3. Leathers, A.S., Micha, D.A., and Kilin, D.S., Direct and indirect electron transfer at a semiconductor surface with an adsorbate: Theory and application to Ag3Si(111):H. Journal of Chemical Physics, 2010. 132(11).Google Scholar
4. Kilin, D.S., et al. ., Ab initio study of exciton transfer dynamics from a core-shell semiconductor quantum dot to a porphyrin-sensitizer. Journal of Photochemistry and Photobiology a-Chemistry, 2007. 190(2-3): p. 342–351.Google Scholar
5. Harris, L.A. and Quong, A.A., Molecular chemisorption as the theoretically preferred pathway for water adsorption on ideal rutile TiO2(110). Physical Review Letters, 2004. 93(8).Google Scholar
6. Kornherr, A., et al. ., Multilayer adsorption of water at a rutile TiO2(110) surface: Towards a realistic modeling by molecular dynamics. Journal of Chemical Physics, 2004. 121(8): p. 3722–3726.Google Scholar
7. Kowalski, P.M., Meyer, B., and Marx, D., Composition, structure, and stability of the rutile TiO2(110) surface: Oxygen depletion, hydroxylation, hydrogen migration, and water adsorption. Physical Review B, 2009. 79(11).Google Scholar
8. Walle, L.E., et al. ., Experimental evidence for mixed dissociative and molecular adsorption of water on a rutile TiO2(110) surface without oxygen vacancies. Physical Review B, 2009. 80(23).Google Scholar
9. Duzhko, V., et al. ., Photovoltage in nanocrystalline porous TiO2. Physical Review B, 2001. 64(7).Google Scholar
10. Walter, M.G., et al. ., Solar Water Splitting Cells. Chemical Reviews, 2010. 110(11): p. 6446–6473.Google Scholar