skip to main content


Title: The Vacancy‐Induced Electronic Structure of the SrTiO 3−δ Surface
Abstract

The emergence of a 2D electron gas (2DEG) on the (001) surface of oxygen‐deficient strontium titanate (SrTiO3−δ) is investigated. Using in situ soft X‐ray spectroscopy and effective mass modeling, a series of quantitative band diagrams are developed to describe the evolution of near‐surface and bulk carrier concentrations, downward band bending, and Fermi level along a lateral gradient of oxygen vacancies formed on SrTiO3−δby direct‐current resistive heating under ultrahigh vacuum conditions. Electrons are accumulated over a 3 nm region near the surface, confined within a potential well with saturated 300 meV downward band bending. The relation between Fermi levels and carrier concentrations near the surface suggests the density of states near the surface is much lower than the bulk density of states, which is consistent with the quantum‐confined subbands of a 2DEG. The quantitative relationship between the surface and bulk electronic structures developed in this work provides a guide for precise engineering of the oxygen‐vacancy‐induced 2DEG in SrTiO3.

 
more » « less
NSF-PAR ID:
10079510
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Electronic Materials
Volume:
5
Issue:
1
ISSN:
2199-160X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    In2O3, an n‐type semiconducting transparent transition metal oxide, possesses a surface electron accumulation layer (SEAL) resulting from downward surface band bending due to the presence of ubiquitous oxygen vacancies. Upon annealing In2O3in ultrahigh vacuum or in the presence of oxygen, the SEAL can be enhanced or depleted, as governed by the resulting density of oxygen vacancies at the surface. In this work, an alternative route to tune the SEAL by adsorption of strong molecular electron donors (specifically here ruthenium pentamethylcyclopentadienyl mesitylene dimer, [RuCp*mes]2) and acceptors (here 2,2′‐(1,3,4,5,7,8‐hexafluoro‐2,6‐naphthalene‐diylidene)bis‐propanedinitrile, F6TCNNQ) is demonstrated. Starting from an electron‐depleted In2O3surface after annealing in oxygen, the deposition of [RuCp*mes]2restores the accumulation layer as a result of electron transfer from the donor molecules to In2O3, as evidenced by the observation of (partially) filled conduction sub‐bands near the Fermi level via angle‐resolved photoemission spectroscopy, indicating the formation of a 2D electron gas due to the SEAL. In contrast, when F6TCNNQ is deposited on a surface annealed without oxygen, the electron accumulation layer vanishes and an upward band bending is generated at the In2O3surface due to electron depletion by the acceptor molecules. Hence, further opportunities to expand the application of In2O3in electronic devices are revealed.

     
    more » « less
  2. Topological surface states (TSSs) coexist with a rapidly formed two-dimensional electron gas (2DEG) at the surface of Bi 2 Se 3 . While this complex band structure has been widely studied for its interactions between the two states in terms of electrical conductivity and carrier density, the resulting thermopower has not been investigated as thoroughly. Here, we report measurements of the temperature dependent Seebeck coefficient ( S) and electrical conductivity ( σ) on an undoped 10 nm thin Bi 2 Se 3 film over the temperature range of 100–300 K to find an overall metal-like behavior. The measured S is consistent with the theory when assuming that both the TSS and the 2DEG contribute to thermoelectric transport. Our analysis further shows that the coefficient corresponds to a Fermi level situated well above the conduction band minima of the 2DEG, resulting in comparable contributions from the TSS and the 2DEG. The thermoelectric power factor ( S 2 σ) at 300 K increases by 10%–30% over the bulk. This work provides insights into understanding and enhancing thermoelectric phenomena in topological insulators. 
    more » « less
  3. Abstract

    Previous high-resolution angle-resolved photoemission (ARPES) studies of URu2Si2have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level (EF) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more globalk-space context for the presence of such states and their relation to the bulk Fermi surface (FS) topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence,f-resonant photoemission, Si 2pcore-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of theEF-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk FS topology is critically compared to density functional theory (DFT) and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry Γ,ZandXpoints, incommensurate 0.6a* nested Fermi-edge states located alongZNZare found to be distinctly different from the DFT FS prediction. The temperature evolution of these states aboveTHO, combined with a more detailed theoretical investigation of this region, suggests a key role of theN-point in the hidden order transition.

     
    more » « less
  4. Abstract

    Almahata Sitta (AhS), an anomalous polymict ureilite, is the first meteorite observed to originate from a spectrally classified asteroid (2008TC3). However, correlating properties of the meteorite with those of the asteroid is not straightforward because the AhS stones are diverse types. Of those studied prior to this work, 70–80% are ureilites (achondrites) and 20–30% are various types of chondrites. Asteroid 2008TC3was a heterogeneous breccia that disintegrated in the atmosphere, with its clasts landing on Earth as individual stones and most of its mass lost. We describe AhS 91A and AhS 671, which are the first AhS stones to show contacts between ureilitic and chondritic materials and provide direct information about the structure and composition of asteroid 2008TC3. AhS 91A and AhS 671 are friable breccias, consisting of a C1 lithology that encloses rounded to angular clasts (<10 μm to 3 mm) of olivine, pyroxenes, plagioclase, graphite, and metal‐sulfide, as well as chondrules (~130–600 μm) and chondrule fragments. The C1 material consists of fine‐grained phyllosilicates (serpentine and saponite) and amorphous material, magnetite, breunnerite, dolomite, fayalitic olivine (Fo 28‐42), an unidentified Ca‐rich silicate phase, Fe,Ni sulfides, and minor Ca‐phosphate and ilmenite. It has similarities toCI1 but shows evidence of heterogeneous thermal metamorphism. Its bulk oxygen isotope composition (δ18O = 13.53‰, δ17O = 8.93‰) is unlike that of any known chondrite, but similar to compositions of severalCC‐like clasts in typical polymict ureilites. Its Cr isotope composition is unlike that of any known meteorite. The enclosed clasts and chondrules do not belong to the C1 lithology. The olivine (Fo 75‐88), pyroxenes (pigeonite of Wo ~10 and orthopyroxene of Wo ~4.6), plagioclase, graphite, and some metal‐sulfide are ureilitic, based on mineral compositions, textures, and oxygen isotope compositions, and represent at least six distinct ureilitic lithologies. The chondrules are probably derived from type 3OCand/orCC, based on mineral and oxygen isotope compositions. Some of the metal‐sulfide clasts are derived fromEC. AhS 91A and AhS 671 are plausible representatives of the bulk of the asteroid that was lost. Reflectance spectra of AhS 91A are dark (reflectance ~0.04–0.05) and relatively featureless inVNIR, and have an ~2.7 μm absorption band due toOHin phyllosilicates. Spectral modeling, using mixtures of laboratoryVNIRreflectance spectra of AhS stones to fit the F‐type spectrum of the asteroid, suggests that 2008TC3consisted mainly of ureilitic and AhS 91A‐like materials, with as much as 40–70% of the latter, and <10% ofOC,EC, and other meteorite types. The bulk density of AhS 91A (2.35 ± 0.05 g cm−3) is lower than bulk densities of other AhS stones, and closer to estimates for the asteroid (~1.7–2.2 g cm−3). Its porosity (36%) is near the low end of estimates for the asteroid (33–50%), suggesting significant macroporosity. The textures of AhS 91A and AhS 671 (finely comminuted clasts of disparate materials intimately mixed) support formation of 2008TC3in a regolith environment. AhS 91A and AhS 671 could represent a volume of regolith formed when aCC‐like body impacted into already well‐gardened ureilitic + impactor‐derived debris. AhS 91A bulk samples do not show a solar wind component, so they represent subsurface layers. AhS 91A has a lower cosmic ray exposure (CRE) age (~5–9 Ma) than previously studied AhS stones (11–22 Ma). The spread inCREages argues for irradiation in a regolith environment. AhS 91A and AhS 671 show that ureilitic asteroids could have detectable ~2.7 μm absorption bands.

     
    more » « less
  5. Abstract

    Due to the coexistence of many emergent phenomena, including 2D superconductivity and a large Rashba spin‐orbit coupling, 5d transition metal oxides‐based two‐dimensional electron systems (2DESs) have been prospected as one of the potential intrants for modern electronics. However, despite the lighter electron mass, the mobility of carriers, a key requisite for high‐performance devices, in 5d‐oxides devices remains far behind their 3d‐oxides analogs. The carriers’ mobility in these oxides is significantly hampered by the inevitable presence of defects. Here, very high mobility (≈22 650 cm2V−1s−1) of 5d‐2DES confined at the LaAlO3/KTaO3interface is reported. The high mobility, which is beyond the values observed in SrTiO32DESs in the same carrier‐density range, is achieved using the ionic‐liquid gating at room temperature. The authors postulate that the ionic‐liquid gating affects the oxygen vacancies and efficiently reduces any disorder at the interface. Investigating density and mobility in a broad range of back‐gate voltage, the authors reveal that the mobility follows the power‐law µ ∝ n1.2, indicating the very high quality of ionic‐liquid‐gated LaAlO3/KTaO3devices, consistent with the postulate. Furthermore, the analysis of the quantum oscillations confirms that the high‐mobility electrons occupy the electronic sub‐bands emerging from the Ta:5d orbitals of KTaO3.

     
    more » « less