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Register a new userEngineering two-dimensional electron gases at the (001) and (101) surfaces of TiO2 anatase using light
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Added by
Andres Felipe Santander-Syro
Publication date
2015
fields
Physics
and research's language is
English
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We report the existence of metallic two-dimensional electron gases (2DEGs) at the (001) and (101) surfaces of bulk-insulating TiO2 anatase due to local chemical doping by oxygen vacancies in the near-surface region. Using angle-resolved photoemission spectroscopy, we find that the electronic structure at both surfaces is composed of two occupied subbands of d_xy orbital character. While the Fermi surface observed at the (001) termination is isotropic, the 2DEG at the (101) termination is anisotropic and shows a charge carrier density three times larger than at the (001) surface. Moreover, we demonstrate that intense UV synchrotron radiation can alter the electronic structure and stoichiometry of the surface up to the complete disappearance of the 2DEG. These results open a route for the nano-engineering of confined electronic states, the control of their metallic or insulating nature, and the tailoring of their microscopic symmetry, using UV illumination at different surfaces of anatase.
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Studies on oxide quasi-two dimensional electron gas (q2DEG) have been a playground for the discovery of novel and sometimes unexpected phenomena, like the reported magnetism at the surface and at the interface between LaAlO$_{3}$ and SrTiO$_{3}$ non-magnetic materials. However, magnetism in this system is weak and there are evidences of a not intrinsic origin. Here, by using in-situ high-resolution angle resolved photoemission we demonstrate that ferromagnetic EuTiO$_{3}$, the magnetic counterpart of SrTiO$_{3}$ in the bulk, hosts a q2DEG at its (001) surface. This is confirmed by density functional theory calculations with Hubbard U terms in the presence of oxygen divacancies in various configurations, all of them leading to a spin-polarized q2DEG related to the ferromagnetic order of Eu-4f magnetic moments. The results suggest EuTiO$_{3}$(001) as a new material platform for oxide q2DEGs, characterized by broken inversion and time reversal symmetries.
We develop a first-principles approach based on many-body perturbation theory to investigate the effects of the interaction between electrons and carrier plasmons on the electronic properties of highly-doped semiconductors and oxides. Through the evaluation of the electron self-energy, we account simultaneously for electron-plasmon and electron-phonon coupling in theoretical calculations of angle-resolved photoemission spectra, electron linewidths, and relaxation times. We apply this methodology to electron-doped anatase TiO2 as an illustrative example. The simulated spectra indicate that electron-plasmon coupling in TiO2 underpins the formation of satellites at energies comparable to those of polaronic spectral features. At variance with phonons, however, the energy of plasmons and their spectral fingerprints depends strongly on the carrier concentration, revealing a complex interplay between plasmon and phonon satellites. The electron-plasmon interaction accounts for approximately 40% of the total electron-boson interaction strength and it is key to improve the agreement with measured quasiparticle spectra.
The discovery of two-dimensional electron gas (2DEG) at well-defined interfaces between insulating complex oxides provides the opportunity for a new generation of all-oxide electronics. Particularly, the 2DEG at the interface between two perovskite insulators represented by the formula of ABO3, such as LaAlO3 and SrTiO3, has attracted significant attention. In recent years, progresses have been made to decipher the puzzle of the origin of interface conduction, to design new types of oxide interfaces, and to improve the interfacial carrier mobility significantly. These achievements open the door to explore fundamental as well as applied physics of complex oxides. Here, we review our recent experimental work on metallic and insulating interfaces controlled by interfacial redox reactions in SrTiO3-based heterostructures. Due to the presence of oxygen-vacancies at the SrTiO3 surface, metallic conduction can be created at room temperature in perovskite-type interfaces when the overlayer oxide ABO3 involves Al, Ti, Zr, or Hf elements at the B-sites. Furthermore, relying on interface-stabilized oxygen vacancies, we have created a new type of 2DEG at the heterointerface between SrTiO3 and a spinel {gamma}-Al2O3 epitaxial film with compatible oxygen ions sublattices. The spinel/perovskite oxide 2DEG exhibits an electron mobility exceeding 100,000 cm2V-1s-1, more than one order of magnitude higher than those of hitherto investigated perovskite-type interfaces. Our findings pave the way for design of high-mobility all-oxide electronic devices and open a route towards studies of mesoscopic physics with complex oxides.
High mobility two-dimensional electron gases (2DEGs) underpin todays silicon based devices and are of fundamental importance for the emerging field of oxide electronics. Such 2DEGs are usually created by engineering band offsets and charge transfer at heterointerfaces. However, in 2011 it was shown that highly itinerant 2DEGs can also be induced at bare surfaces of different transition metal oxides where they are far more accessible to high resolution angle resolved photoemission (ARPES) experiments. Here we review work from this nascent field which has led to a systematic understanding of the subband structure arising from quantum confinement of highly anisotropic transition metal d-states along different crystallographic directions. We further discuss the role of different surface preparations and the origin of surface 2DEGs, the understanding of which has permitted control over 2DEG carrier densities. Finally, we discuss signatures of strong many-body interactions and how spectroscopic data from surface 2DEGs may be related to the transport properties of interface 2DEGs in the same host materials.
Oxygen vacancies created in anatase TiO2 by UV photons (80 - 130 eV) provide an effective electron-doping mechanism and induce a hitherto unobserved dispersive metallic state. Angle resolved photoemission (ARPES) reveals that the quasiparticles are large polarons. These results indicate that anatase can be tuned from an insulator to a polaron gas to a weakly correlated metal as a function of doping and clarify the nature of conductivity in this material.
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