Conclusions

Skobel’tsyn, D. V.

doi:10.1007/978-1-4684-1578-0_10

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“…Strain engineering has been commonly implemented to indirectly control the metal–oxygen hybridization by changing the Ni–O bond distance in Ni-doped SrTiO 3 thin films and organometallic complexes . However, these methods are limited due to the constant application of strong fields or the irreversible modification of the composition, which can limit device performance via space charge accumulation or unwanted geometric distortion . Therefore, it remains a challenge for the scientific community to modify the hybridization of atomic orbitals in a stable but reversible manner.…”

Section: Introductionmentioning

confidence: 99%

Weak Field Tuning of Transition-Metal Dopant Hybridization in Solid Hosts

et al. 2018

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Transition-metal (TM)-doped solids are one of the most extensively studied compounds in the fields of catalysis, magnetism, solar cells, etc., due to their tunable optoelectronic properties that stem from TM energy-level hybridization. In this work, the hybridization of the Ni–O bond in TiO2:Ni films was controlled in a stable, reversible manner via surface functionalization with polarized molecules. The Ni-doped TiO2 surface was functionalized with para-benzoic acid groups to modify the electron density distribution within the film. The dopant distribution and elemental composition at the interface are probed via high-resolution transmission electron microscopy coupled with electron energy loss spectroscopy mapping. The effect of the surface modification on the dopant, Ni2+, is studied via surface-sensitive electronic characterization techniques, such as X-ray photoelectron spectroscopy and soft X-ray absorption spectroscopy (XAS). The electron density in the valence orbitals of the dopant was observed to be a function of the dipole moment of the para-substituted benzoic acid. The resulting XAS spectra of the Ni2+ after surface modification of TiO2:Ni films were modeled (CTM4XAS) and indicated ligand-dependent symmetry breaking around the Ni2+ at the functionalized interface. Therefore, the modified electron density at the interface due to the polarized molecules is observed to impact the hybridization of the TM dopant energy levels in solid hosts. This phenomenon of adaptive dopant hybridization in a solid host (TiO2) can be exploited to obtain tunable optical responses from TM-doped inorganic phosphors, which have an impact in various fields, such as luminescent displays, solar cells, sensors, telecommunications, counterfeit technologies, and biodetection.

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Section: Introductionmentioning

confidence: 99%