10.1186/2228-5326-3-26

Investigation of optoelectronic properties of N3 dye-sensitized TiO2 nano-crystals by hybrid methods: ONIOM (QM/MM) calculations

PDF HTML
  • Mohsen Oftadeh*1,
  • Leila Tavakolizadeh1,
  1. Department of Chemistry, Payame Noor University, Tehran, 19395-4697, IR
Cover Image

Published in Issue 2013-04-23

How to Cite

Oftadeh, M., & Tavakolizadeh, L. (2013). Investigation of optoelectronic properties of N3 dye-sensitized TiO2 nano-crystals by hybrid methods: ONIOM (QM/MM) calculations. International Nano Letters, 3(1 (December 2013). https://doi.org/10.1186/2228-5326-3-26
Crossref
Scopus
Google Scholar
Europe PMC

PDF views: 92

HTML views: 37

Abstract

Abstract In this article, Ru(4,4′-dicarboxy-2,2′-bipyridine) 2 (NCS) 2 dye (N3) and some derivatives were investigated using Density Functional Theory (DFT) calculations in solution to elucidate the influence of the environment and substituted groups on electronic properties. Full geometry optimization and investigation of electronic properties of N3 dye and some derivatives were performed using DFT and HF calculations. The singlet ground state geometries were fully optimized at the B3LYP/3-21G** level of theory through the Gaussian 98 program. Based on the computed results, the optoelectronic properties are sensitive to chemical solvent environments. Moreover, the properties of anatase cluster (TiO 2 ) models have been investigated, and N3 dyes have been adsorbed on TiO 2 nano-particle with diprotonated states. The modified N3 dyes highly affected the electronic structure. This leads to significant changes in the adsorption spectra as compared to the N3 dyes. Through hybrid methods, the properties of interfacial electronic coupling of the combined system were estimated. The results of some combined systems showed that the electronic coupling, lowest lowest unoccupied molecular orbitals, and the TiO 2 conduction band resided in the visible region.

Keywords

  • DFT,
  • Gap energy,
  • Sensitized dye,
  • Optical properties
PDF HTML

References

  1. Ferrere and Gregg (2001) Large increases in photocurrents and solar conversion efficiencies by UV illumination of dye sensitized solar cells (pp. 7602-7605) https://doi.org/10.1021/jp011612o
  2. Derosa and Seminario (2001) Electron transport through single molecules: scattering treatment using density functional and Green function theories (pp. 471-481) https://doi.org/10.1021/jp003033+
  3. O'Regan and Grätzel (1991) A low-cost, high-efficiency solar cell based on dye sensitized colloidal TiO2 films (pp. 737-740) https://doi.org/10.1038/353737a0
  4. Pan et al. (2002) Photoinduced electron transfer between a carotenoid and TiO2 nanoparticle (pp. 13949-13957) https://doi.org/10.1021/ja0279186
  5. Biju et al. (2004) Intermittent single-molecule interfacial electron transfer dynamics (pp. 9374-9381) https://doi.org/10.1021/ja040057b
  6. McConnell (2002) Assessment of the dye-sensitized solar cell (pp. 273-295) https://doi.org/10.1016/S1364-0321(01)00012-0
  7. Anderson and Lian (2005) Ultrafast electron transfer at the molecule-semiconductor nanoparticle interface (pp. 491-519) https://doi.org/10.1146/annurev.physchem.55.091602.094347
  8. Rego and Batista (2003) Quantum dynamics simulations of interfacial electron transfer in sensitized TiO2 semiconductors (pp. 7989-7997) https://doi.org/10.1021/ja0346330
  9. Stier et al. (2003) Ab initio molecular dynamics of ultrafast electron injection from molecular donors to the TiO2 acceptor (pp. 132-146) https://doi.org/10.1117/12.503646
  10. Duncan et al. (2005) Ab initio nonadiabatic molecular dynamics of the ultrafast electron injection across the alizarin-TiO2 interface (pp. 7941-7951) https://doi.org/10.1021/ja042156v
  11. Lundqvist (2006) Uppsala University
  12. Aghtar (2009) Payame Noor University (PNU)
  13. Diebold (2003) Structure and properties of TiO2 surfaces: a brief review (pp. 681-687) https://doi.org/10.1007/s00339-002-2004-5
  14. Nilsing et al. (2005) Phosphonic acid adsorption at the TiO2 anatase (101) surface investigated by periodic hybrid HF-DFT computations (pp. 49-60) https://doi.org/10.1016/j.susc.2005.02.044
  15. Homann et al. (2004) Adsorption of small molecules on the anatase (100) surface (pp. 135-144) https://doi.org/10.1016/j.susc.2003.12.039
  16. Vittadini et al. (2000) Formic acid adsorption on dry and hydrated TiO2 anatase (101) surfaces by DFT calculations (pp. 1300-1306) https://doi.org/10.1021/jp993583b
  17. Nilsing et al. (2005) Anchor group influence on molecule-metal oxide interfaces: periodic hybrid DFT study of pyridine bound to TiO2 via carboxylic and phosphonic acid (pp. 375-380) https://doi.org/10.1016/j.cplett.2005.08.154
  18. Rappoport et al. (2009) Approximate density functionals: which should I choose? (pp. 159-172) Wiley
  19. Nazeeruddin et al. (2005) Combined experimental and DFT-TDDFT computational study of photoelectrochemical cell ruthenium sensitizers (pp. 16835-16847) https://doi.org/10.1021/ja052467l
  20. Wahab et al. (2008) Computational modeling of the adsorption and photodegradation of 4-chlorophenol on anatase TiO2 particles (pp. 84-90) https://doi.org/10.1016/j.theochem.2008.05.019
  21. Lundqvist et al. (2006) DFT Modeling of bare and dye-sensitized TiO2 nanocrystals (pp. 3214-3234) https://doi.org/10.1002/qua.21088
  22. Lundqvist et al. (2007) Calculated optoelectronic properties of ruthenium tris-bipyridine dyes containing oligophenyleneethynylene rigid rod linkers in different chemical environments (pp. 1487-1497) https://doi.org/10.1021/jp064219x
  23. Iozzi (2006) Napoli University
  24. Frisch et al. (1999) Gaussian Inc