| 1. |
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- 2019
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Tidskriftsartikel (refereegranskat)
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| 2. |
- Arvizu, Miguel A, et al.
(författare)
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Electrochromism in sputter-deposited W-Ti oxide films : Durability enhancement due to Ti
- 2014
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Ingår i: Solar Energy Materials and Solar Cells. - : Elsevier BV. - 0927-0248 .- 1879-3398. ; 125, s. 184-189
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Tidskriftsartikel (refereegranskat)abstract
- Thin films of W-Ti oxide were prepared by reactive DC magnetron sputtering and were characterized by Rutherford bathcattering spectrometry, X-ray diffraction, scanning electron microscopy and atomic force microscopy. The electrochromic properties were studied by cyclic voltammetry in an electrolyte of lithium perchlorate in propylene carbonate and by optical transmittance measurements. The addition of Ti significantly promoted the amorphous nature of the films and stabilized their electrochemical cycling performance and dynamic range for electrochromism. (C) 2014 Elsevier B.V. All rights reserved.
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| 3. |
- Triana, Carlos A., et al.
(författare)
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Disentangling the intricate atomic short-range order and electronic properties in amorphous transition metal oxides
- 2017
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Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 7
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Tidskriftsartikel (refereegranskat)abstract
- Solid state materials with crystalline order have been well-known and characterized for almost a century while the description of disordered materials still bears significant challenges. Among these are the atomic short-range order and electronic properties of amorphous transition metal oxides [aTMOs], that have emerged as novel multifunctional materials due to their optical switching properties and high-capacity to intercalate alkali metal ions at low voltages. For decades, research on aTMOs has dealt with technological optimization. However, it remains challenging to unveil their intricate atomic short-range order. Currently, no systematic and broadly applicable methods exist to assess atomic-size structure, and since electronic localization is structure-dependent, still there are not well-established optical and electronic mechanisms for modelling the properties of aTMOs. We present state-of-the-art systematic procedures involving theory and experiment in a self-consistent computational framework to unveil the atomic short-range order and its role for the electronic properties. The scheme is applied to amorphous tungsten trioxide aWO(3), which is the most studied electrochromic aTMO in spite of its unidentified atomic-size structure. Our approach provides a one-to-one matching of experimental data and corresponding model structure from which electronic properties can be directly calculated in agreement with the electronic transitions observed in the XANES spectra.
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| 4. |
- Triana, Carlos A., et al.
(författare)
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Electrochromism and small-polaron hopping in oxygen deficient and lithium intercalated amorphous tungsten oxide films
- 2015
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 118:2, s. 1-9
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Tidskriftsartikel (refereegranskat)abstract
- Thin films of LixWO3-z with 0 <= x <= 0.27 and 0 <= z <= 0.27 were prepared by sputter deposition followed by electrochemical lithiation. Kramers-Kronig-consistent complex dielectric functions were obtained for these films by numerical inversion of experimental spectra of optical transmittance and reflectance by using a superposition of Tauc-Lorentz and Lorentz oscillator models. Low-energy optical absorption bands were induced by oxygen vacancies and/or by electrochemical intercalation of Li+ species together with charge compensating electrons. The experimental optical conductivity was fitted to a small-polaron model for disordered systems with strong electron-phonon interaction, taking into account transitions near the Fermi level. The optical absorption is due to small-polaron hopping and associated with the formation of W5+ states due to transfer of electrons from oxygen vacancies and/or insertion of Li+ species. The results also show increases in the Fermi level, caused by oxygen deficiency or Li+ insertion, which occur along with a band gap shift towards higher energies for the Li+ intercalated films.
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| 5. |
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| 6. |
- Triana, Carlos A, et al.
(författare)
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Modeling of Electronic Properties of Amorphous Oxides
- 2018
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Ingår i: Encyclopedia of Interfacial Chemistry. - : Elsevier. - 9780128097397 - 9780128098943 ; , s. 319-331
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Bokkapitel (refereegranskat)abstract
- Amorphous transition metal oxides (aTMOs) are used as multifunctional materials in many technological applications. A detailed understanding of the electronic density of states is a necessary prerequisite for modeling their functional properties. The electronic properties, however, are structure-dependent making the description of the electronic structure of disordered and amorphous materials challenging. Here we present a scheme based on obtaining atomic model structures from simulations of experimental X-ray-Absorption spectra, together with first principles electronic structure calculations. This approach provides a self-consistent framework to assess fundamental electronic processes in aTMOs and can be applied to the study of disordered and amorphous materials in general.
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| 7. |
- Triana, Carlos A., et al.
(författare)
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Optical absorption and small-polaron hopping in oxygen deficient and lithium-ion-intercalated amorphous titanium oxide films
- 2016
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 119:1
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Tidskriftsartikel (refereegranskat)abstract
- Optical absorption in oxygen-deficient and Li+-ion inserted titanium oxide films was studied in the framework of small-polaron hopping. Non-stoichiometric TiOy films with 1.68 <= y <= 2.00 were deposited by reactive DC magnetron sputtering and were subjected to electrochemical intercalation of Li+-ions and charge-balancing electrons to obtain LixTiOy films with 0.12 <= x <= 0.34. Dispersion analysis was applied to calculate the complex dielectric function epsilon((h) over bar omega) =epsilon(1) ((h) over bar omega) + i epsilon(2)((h) over bar omega) from numerical inversion of optical transmittance and reflectance spectra; a superposition of Tauc-Lorentz and Lorentz oscillator models was used for this purpose. Data on epsilon(2)((h) over bar omega) were employed to calculate the optical conductivity and fit this property to a small-polaron model for disordered systems with strong electron-phonon interaction and involving transitions near the Fermi level. The introduction of oxygen vacancies and/or Li+ insertion yielded band gap widening by similar to 0.20-0.35 eV, and both processes induced similar low-energy optical absorption. The small-polaron-based analysis indicated increases in the Fermi level by similar to 0.15-0.3 eV for sub-stoichiometric and/or Li+-inserted films. This suggests the existence of polaronic Ti3+ states in the lower part of the conduction band arising from transfer of electrons from oxygen vacancies and/or inserted Li+ species. The present article is a sequel to an earlier paper on oxygen-deficient and/or Li+-inserted amorphous WOy thin films and forms part of a comprehensive investigation of optical absorption in amorphous transition metal oxides with different valence states of the metallic ions.
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| 8. |
- Chen, Hang, et al.
(författare)
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Modulating Carrier Kinetics in BiVO4 Photoanodes through Molecular Co4O4 Cubane Layers
- 2023
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Ingår i: Advanced Functional Materials. - : Wiley-VCH Verlagsgesellschaft. - 1616-301X .- 1616-3028. ; 33:48
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Tidskriftsartikel (refereegranskat)abstract
- Understanding the role and immobilization of molecular catalysts on photoelectrodes is essential to use their full potential for efficient solar fuel generation. Here, a CoII4O4 cubane with proven catalytic performance and an active H2O─Co2(OR)2─OH2 edge-site moiety is immobilized on BiVO4 photoanodes through a versatile layer-by-layer assembly strategy. This delivers a photocurrent of 3.3 mA cm−2 at 1.23 VRHE and prolonged stability. Tuning the thickness of the Co4O4 layer has remarkable effects on photocurrents, dynamic open circuit potentials, and charge carrier behavior. Comprehensive-time and frequency-dependent perturbation techniques are employed to investigate carrier kinetics in transient and pseudo-steady-state operando conditions. It is revealed that the Co4O4 layer can prolong carrier lifetime, unblock kinetic limitations at the interface by suppressing recombination, and enhance charge transfer. Additionally, its flexible roles are identified as passivation/hole trapping/catalytic layer at respective lower/moderate/higher potentials. These competing functions are under dynamic equilibrium, which fundamentally defines the observed photocurrent trends.
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| 9. |
- Triana, Carlos A, 1981-
(författare)
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Atomic short-range order, optical and electronic properties of amorphous transition metal oxides : An experimental and theoretical study of amorphous titanium aTiO2 and tungsten aWO3 solid thin-film oxides
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Amorphous transition metal oxides [aTMOs], have emerged as innovative functional materials for wide-ranging electronic, optical and energy-related applications. However, no systematic and broadly applicable method exists to assess their atomic-scale correlations, and since the optical and electronic processes are local structure-dependent, still there are not well-stablished mechanisms that suitably explain the physical properties of aTMOs.This thesis presents experimental and theoretical studies of the atomic short-range order, optical and electronic properties, and state-defects induced by Li+-ion-intercalation and oxygen-vacancies in amorphous titanium aTiO2 and tungsten aWO3 thin-film oxides. Those properties play a key role for application in high energy-density Li+-ion batteries and in switchable dynamical modulation of solar-irradiation transmittance for energy efficient "smart windows", where the disorder-dependent Li+-ion-intercalation and oxygen-vacancy-induced defect-states influence charge-carrier transfer mechanisms. After introducing the scope of this thesis, the fundamental theoretical concepts describing the experimental findings on amorphous solids are reviewed. Thereafter, a comprehensive analysis on the optical absorption phenomena experimentally observed in oxygen-deficient and Li+-ion-intercalated aLixTiO2−y and aLixWO3−y thin-films and a discussion on the electrochromic properties are presented. The optical absorption is described in the framework of the small polaron absorption model.Finally, a state-of-the-art systematic procedure involving theory and experiment in a self-consistent computational framework is implemented to unveil the atomic-scale structure of aTiO2 and aWO3, and its role for the electronic properties. The procedure is based in Reverse Monte Carlo [RMC] and Finite Difference Method [FDM] simulations of X-ray-Absorption spectra to construct a disordered theoretical model having the same bonding and coordination distribution as the experimental system. Ab-initio molecular dynamics simulations and density functional theory are then used to assess defect-states induced by Li+-ion-intercalation and oxygen-vacancies in aTiO2 and aWO3 oxides.The schemes introduced in this study offer a consistent route to experimentally and theoretically assess the role of the atomic-scale structure on the optical and electronic properties of aTiO2 and aWO3 and could be extended to the study of other aTMOs. The final results provide crucial insight towards the understanding of optical and electronic mechanisms where disorder-dependent ion-intercalation and oxygen-vacancy-induced localized defect-states influence charge transfer mechanisms of crucial importance for wide ranging optical and energy-related application of aTiO2 and aWO3 oxides.
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| 10. |
- Triana, Carlos A., et al.
(författare)
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Electrochromic Properties of Li+-Intercalated Amorphous Tungsten (aWO(3-x)) and Titanium (aTiO(2-x)) Oxide Thin Films
- 2014
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Ingår i: INERA WORKSHOP. - : IOP Publishing. ; , s. UNSP 012004-
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Konferensbidrag (refereegranskat)abstract
- We report on electrochromic properties of stoichiometric and oxygen-deficient amorphous films, denoted aWO(3-x) and aTiO(2-x), under Li+-ion-electron inter/deintercalation. Optical characterization of the films in their as-deposited, fully intercalated (dark), and bleached states were performed by in-situ optical transmittance measurements. We explore electrochromism and optical absorption phenomena in the context of oxygen deficiency and nanostructure. Studies by cyclic voltammetry suggest good optical modulation and charge capacity upon Li+-ion-electron inter/deintercalation for almost stoichiometric films.
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