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  Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Baldini, E., Chiodo, L., Dominguez, A., Palummo, M., Moser, S., Yazdi-Rizi, M., et al. (2017). Strongly bound excitons in anatase TiO2 single crystals and nanoparticles. Nature Communications, 8: 13. doi:10.1038/s41467-017-00016-6.

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Item Permalink: https://hdl.handle.net/21.11116/0000-0001-7B1A-9 Version Permalink: https://hdl.handle.net/21.11116/0000-0004-AA72-C
Genre: Journal Article

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 Creators:
Baldini, E.1, Author
Chiodo, L.2, 3, Author
Dominguez, A.4, Author           
Palummo, M.5, Author
Moser, S.6, Author
Yazdi-Rizi, M.7, Author
Auböck, G.1, Author
Mallett, B. P. P.7, Author
Berger, H.8, Author
Magrez, A.8, Author
Bernhard, C.7, Author
Grioni, M.6, Author
Rubio, A.4, 9, Author           
Chergui, M.1, Author
Affiliations:
1Laboratory of Ultrafast Spectroscopy, ISIC and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne (EPFL), ou_persistent22              
2Unit of Nonlinear Physics and Mathematical Modelling, Department of Engineering, Università Campus Bio-Medico di Roma, ou_persistent22              
3Center for Life Nano Science @ Sapienza, Istituto Italiano di Tecnologia,, ou_persistent22              
4Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
5Dipartimento di Fisica and INFN, Università Tor Vergata, ou_persistent22              
6Laboratory of Electron Spectroscopy, IPHYS and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne (EPFL), ou_persistent22              
7Department of Physics, University of Fribourg, ou_persistent22              
8Crystal Growth Facility, École Polytechnique Fédérale de Lausanne (EPFL), ou_persistent22              
9Departamento Fisica de Materiales, Universidad del País Vasco, ou_persistent22              

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Free keywords: X-RAY-ABSORPTION; OPTICAL-PROPERTIES; TEMPERATURE-DEPENDENCE; BINDING-ENERGY; GREENS-FUNCTION; QUANTUM-WELLS; AB-INITIO; BAND-GAP; SEMICONDUCTOR; TRANSITIONS
 Abstract: Anatase TiO2 is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. The universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.

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Language(s): eng - English
 Dates: 2016-10-032017-02-052017-04-13
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-017-00016-6
arXiv: 1601.01244
 Degree: -

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Project name : We acknowledge financial support from the Swiss NSF via the NCCR:MUST and the contracts No. 206021_157773, 20020_153660 and 407040_154056 (PNR 70), the European Research Council Advanced Grants H2020 ERCEA 695197 DYNAMOX and QSpec-NewMat (ERC-2015-AdG-694097), Spanish Grant FIS2013-46159-C3-1-P, Grupos Consolidados del Gobierno Vasco (IT578-13), COST Actions CM1204 (XLIC), MP1306 (EUSpec), European Union H2020 programme under GA no.676580 (NOMAD) and the Austrian Science Fund (FWF P25739-N27). M.P. acknowledges the EC for RISE project no CoExAN GA644076 and Cineca for computational resources allocated under Iscra-C initiative. The Advanced Light Source is supported by the Director, Of fice of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
Grant ID : 695197
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : We acknowledge financial support from the Swiss NSF via the NCCR:MUST and the contracts No. 206021_157773, 20020_153660 and 407040_154056 (PNR 70), the European Research Council Advanced Grants H2020 ERCEA 695197 DYNAMOX and QSpec-NewMat (ERC-2015-AdG-694097), Spanish Grant FIS2013-46159-C3-1-P, Grupos Consolidados del Gobierno Vasco (IT578-13), COST Actions CM1204 (XLIC), MP1306 (EUSpec), European Union H2020 programme under GA no.676580 (NOMAD) and the Austrian Science Fund (FWF P25739-N27). M.P. acknowledges the EC for RISE project no CoExAN GA644076 and Cineca for computational resources allocated under Iscra-C initiative. The Advanced Light Source is supported by the Director, Of fice of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
Grant ID : 676580
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 8 Sequence Number: 13 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723