A DFT+U description of oxygen vacancies at the TiO2 rutile (110) surface. Morgan, B. J. & Watson, G. W. Surface Science, 601(21):5034–5041, November, 2007. ![A DFT+U description of oxygen vacancies at the TiO2 rutile (110) surface [link]](https://bibbase.org/img/filetypes/link.svg "link")
Paper doi abstract bibtex Experimental observations indicate that removing bridging oxygen atoms from the TiO2 rutile (1�1�0) surface produces a localised state approximately 0.7�eV below the conduction band. The corresponding excess electron density is thought to localise on the pair of Ti atoms neighbouring the vacancy; formally giving two Ti3+ sites. We consider the electronic structure and geometry of the oxygen deficient TiO2 rutile (1�1�0) surface using both gradient-corrected density functional theory (GGA DFT) and DFT corrected for on-site Coulomb interactions (GGA�+�U) to allow a direct comparison of the two methods. We show that GGA fails to predict the experimentally observed electronic structure, in agreement with previous uncorrected DFT calculations on this system. Introducing the +U term encourages localisation of the excess electronic charge, with the qualitative distribution depending on the value of U. For low values of U ([less-than-or-equals, slant]4.0�eV) the charge localises in the sub-surface layers occupied in the GGA solution at arbitrary Ti sites, whereas higher values of U ([greater-or-equal, slanted]4.2�eV) predict strong localisation with the excess electronic charge mainly on the two Ti atoms neighbouring the vacancy. The precise charge distribution for these larger U values is found to differ from that predicted by previous hybrid-DFT calculations.
@article{morgan_dft+u_2007,
title = {A {DFT}+{U} description of oxygen vacancies at the {TiO2} rutile (110) surface},
volume = {601},
url = {http://www.sciencedirect.com/science/article/B6TVX-4PN05JX-3/2/d28396fc107af800f5b76c5fd1ff1a82},
doi = {10.1016/j.susc.2007.08.025},
abstract = {Experimental observations indicate that removing bridging oxygen atoms from the TiO2 rutile (1�1�0) surface produces a localised state approximately 0.7�eV below the conduction band. The corresponding excess electron density is thought to localise on the pair of Ti atoms neighbouring the vacancy; formally giving two Ti3+ sites. We consider the electronic structure and geometry of the oxygen deficient TiO2 rutile (1�1�0) surface using both gradient-corrected density functional theory (GGA DFT) and DFT corrected for on-site Coulomb interactions (GGA�+�U) to allow a direct comparison of the two methods. We show that GGA fails to predict the experimentally observed electronic structure, in agreement with previous uncorrected DFT calculations on this system. Introducing the +U term encourages localisation of the excess electronic charge, with the qualitative distribution depending on the value of U. For low values of U ([less-than-or-equals, slant]4.0�eV) the charge localises in the sub-surface layers occupied in the GGA solution at arbitrary Ti sites, whereas higher values of U ([greater-or-equal, slanted]4.2�eV) predict strong localisation with the excess electronic charge mainly on the two Ti atoms neighbouring the vacancy. The precise charge distribution for these larger U values is found to differ from that predicted by previous hybrid-DFT calculations.},
number = {21},
urldate = {2008-09-03},
journal = {Surface Science},
author = {Morgan, Benjamin J. and Watson, Graeme W.},
month = nov,
year = {2007},
keywords = {Ab initio quantum chemical methods and calculations, Density functional calculations, Self-interaction correction, Surface electronic phenomena, Surface defects, Titanium oxide},
pages = {5034--5041},
}
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We consider the electronic structure and geometry of the oxygen deficient TiO2 rutile (1�1�0) surface using both gradient-corrected density functional theory (GGA DFT) and DFT corrected for on-site Coulomb interactions (GGA�+�U) to allow a direct comparison of the two methods. We show that GGA fails to predict the experimentally observed electronic structure, in agreement with previous uncorrected DFT calculations on this system. Introducing the +U term encourages localisation of the excess electronic charge, with the qualitative distribution depending on the value of U. For low values of U ([less-than-or-equals, slant]4.0�eV) the charge localises in the sub-surface layers occupied in the GGA solution at arbitrary Ti sites, whereas higher values of U ([greater-or-equal, slanted]4.2�eV) predict strong localisation with the excess electronic charge mainly on the two Ti atoms neighbouring the vacancy. The precise charge distribution for these larger U values is found to differ from that predicted by previous hybrid-DFT calculations.","number":"21","urldate":"2008-09-03","journal":"Surface Science","author":[{"propositions":[],"lastnames":["Morgan"],"firstnames":["Benjamin","J."],"suffixes":[]},{"propositions":[],"lastnames":["Watson"],"firstnames":["Graeme","W."],"suffixes":[]}],"month":"November","year":"2007","keywords":"Ab initio quantum chemical methods and calculations, Density functional calculations, Self-interaction correction, Surface electronic phenomena, Surface defects, Titanium oxide","pages":"5034–5041","bibtex":"@article{morgan_dft+u_2007,\n\ttitle = {A {DFT}+{U} description of oxygen vacancies at the {TiO2} rutile (110) surface},\n\tvolume = {601},\n\turl = {http://www.sciencedirect.com/science/article/B6TVX-4PN05JX-3/2/d28396fc107af800f5b76c5fd1ff1a82},\n\tdoi = {10.1016/j.susc.2007.08.025},\n\tabstract = {Experimental observations indicate that removing bridging oxygen atoms from the TiO2 rutile (1�1�0) surface produces a localised state approximately 0.7�eV below the conduction band. The corresponding excess electron density is thought to localise on the pair of Ti atoms neighbouring the vacancy; formally giving two Ti3+ sites. We consider the electronic structure and geometry of the oxygen deficient TiO2 rutile (1�1�0) surface using both gradient-corrected density functional theory (GGA DFT) and DFT corrected for on-site Coulomb interactions (GGA�+�U) to allow a direct comparison of the two methods. We show that GGA fails to predict the experimentally observed electronic structure, in agreement with previous uncorrected DFT calculations on this system. Introducing the +U term encourages localisation of the excess electronic charge, with the qualitative distribution depending on the value of U. For low values of U ([less-than-or-equals, slant]4.0�eV) the charge localises in the sub-surface layers occupied in the GGA solution at arbitrary Ti sites, whereas higher values of U ([greater-or-equal, slanted]4.2�eV) predict strong localisation with the excess electronic charge mainly on the two Ti atoms neighbouring the vacancy. The precise charge distribution for these larger U values is found to differ from that predicted by previous hybrid-DFT calculations.},\n\tnumber = {21},\n\turldate = {2008-09-03},\n\tjournal = {Surface Science},\n\tauthor = {Morgan, Benjamin J. and Watson, Graeme W.},\n\tmonth = nov,\n\tyear = {2007},\n\tkeywords = {Ab initio quantum chemical methods and calculations, Density functional calculations, Self-interaction correction, Surface electronic phenomena, Surface defects, Titanium oxide},\n\tpages = {5034--5041},\n}\n\n\n\n","author_short":["Morgan, B. J.","Watson, G. 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