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1.
Phys Chem Chem Phys ; 24(12): 7253-7263, 2022 Mar 23.
Article in English | MEDLINE | ID: mdl-35275156

ABSTRACT

The formation of two-dimensional oxide dodecagonal quasicrystals as well as related complex approximant phases was recently reported in thin films derived from BaTiO3 or SrTiO3 perovskites deposited on (111)-oriented Pt single crystals. Here, we use an all-thin-film approach in which the single crystal is replaced by a 10 nm thick Pt(111) buffer layer grown by molecular beam epitaxy on an Al2O3(0001) substrate. An ultra-thin film of SrTiO3 was subsequently deposited by pulsed laser deposition. The film stacking and structure are fully characterized by diffraction and microscopy techniques. We report the discovery of two new complex phases obtained by reduction of this system through high temperature annealing under ultrahigh vacuum conditions. The formation of a new large square approximant with a lattice parameter equal to 44.4 Å is evidenced by low-energy electron diffraction and scanning tunneling microscopy (STM). Additionally, a new 2D hexagonal approximant phase with a lattice parameter of 28 Å has been observed depending on the preparation conditions. Both phases can be described by two different tilings constructed with the same basic square, triangle and rhombus tiles possessing a common edge length of about 6.7 Å. Using the tiling built from high resolution STM images, we propose an atomic model for each approximant which accounts for the experimental observations. Indeed, the STM images simulated using these models are found to be in excellent agreement with the experimental ones, the bright protrusions being attributed to the topmost Sr atoms. In addition our theoretical approach shows that the adhesion of the oxide layer is rather strong (-0.30 eV Å-2). This is attributed to charge transfer, from the most electropositive elements (Sr and Ti) to the most electronegative ones (Pt and O), and to hybridization with Pt-states. Density of states calculations indicate differences in the electronic structure of the two approximants, suggesting different chemical and physical properties. This all-thin-film approach may be useful to explore the formation of complex two-dimensional oxide phases in other metal-oxide combinations.

2.
J Phys Condens Matter ; 27(43): 435601, 2015 Nov 04.
Article in English | MEDLINE | ID: mdl-26444931

ABSTRACT

We study the transport properties in SrVO3/LaVO3 (SVO/LVO) superlattices deposited on SrTiO3 (STO) substrates. We show that the electronic conduction occurs in the metallic LVO layers with a galvanomagnetism typical of a 2D Fermi surface. In addition, a Kondo-like component appears in both the thermal variation of resistivity and the magnetoresistance. Surprisingly, in this system where the STO interface does not contribute to the measured conduction, the Kondo correction is strongly anisotropic. We show that the growth temperature allows a direct control of this contribution. Finally, the key role of vanadium mixed valency stabilized by oxygen vacancies is enlightened.

3.
J Phys Condens Matter ; 27(17): 175001, 2015 May 08.
Article in English | MEDLINE | ID: mdl-25765433

ABSTRACT

While structure refinement is routinely achieved for simple bulk materials, the accurate structural determination still poses challenges for thin films due on the one hand to the small amount of material deposited on the thicker substrate and, on the other hand, to the intricate epitaxial relationships that substantially complicate standard x-ray diffraction analysis. Using both electron and x-ray diffraction, we analyze the crystal structure of epitaxial LaVO3 thin films grown on (1 0 0)-oriented SrTiO3. Transmission electron microscopy study reveals that the thin films are epitaxially grown on SrTiO3 and points to the presence of 90° oriented domains. The mapping of the reciprocal space obtained by high resolution x-ray diffraction permits refinement of the lattice parameters. We finally deduce that strain accommodation imposes a monoclinic structure onto the LaVO3 film. The reciprocal space maps are numerically processed and the extracted data computed to refine the atomic positions, which are compared to those obtained using precession electron diffraction tomography.

4.
J Phys Condens Matter ; 27(9): 095603, 2015 Mar 11.
Article in English | MEDLINE | ID: mdl-25688927

ABSTRACT

A series of 100 nm LaVO3 thin films have been synthesized on (0 0 1)-oriented SrTiO3 substrates using the pulsed laser deposition technique, and the effects of growth temperature are analyzed. Transport properties reveal a large electronic mobility and a non-linear Hall effect at low temperature. In addition, a cross-over from a semiconducting state at high-temperature to a metallic state at low-temperature is observed, with a clear enhancement of the metallic character as the growth temperature increases. Optical absorption measurements combined with the two-bands analysis of the Hall effect show that the metallicity is induced by the diffusion of oxygen vacancies in the SrTiO3 substrate. These results allow us to understand that the film/substrate heterostructure behaves as an original semiconducting-metallic parallel resistor, and electronic transport properties are consistently explained.

5.
J Phys Condens Matter ; 25(49): 492201, 2013 Dec 11.
Article in English | MEDLINE | ID: mdl-24214665

ABSTRACT

The interplay between charge, spin, orbital and lattice degrees of freedom in transition metal oxides has motivated extensive research aiming to understand the coupling phenomena in these multifunctional materials. Among them, rare earth vanadates are Mott insulators characterized by spin and orbital orderings strongly influenced by lattice distortions. Using epitaxial strain as a means to tailor the unit cell deformation, we report here on the first thin films of PrVO3 grown on (001)-oriented SrTiO3 substrate by pulsed laser deposition. An extensive structural characterization of the PrVO3 films, combining x-ray diffraction and high-resolution transmission electron microscopy studies, reveals the presence of oriented domains and a unit cell deformation tailored by the growth conditions. We have also investigated the physical properties of the PrVO3 films. We show that, while PrVO3 exhibits an insulating character, magnetic measurements indicate low-temperature hard-ferromagnetic behavior below 80 K. We discuss these properties in view of the thin-film structure.

6.
Phys Rev Lett ; 109(22): 226601, 2012 Nov 30.
Article in English | MEDLINE | ID: mdl-23368143

ABSTRACT

It is well known that transport in lightly n-doped SrTiO(3) involves light and heavy electron bands. We have found that upon application of moderate quasi-isotropic pressures, the relative positions of these subbands are changed by a few meV and, eventually, a band inversion occurs at ~1 kbar. Such effects are, however, suppressed in the closely related KTaO(3) perovskite. We show that the extremely subtle electronic reconfiguration in SrTiO(3) is triggered by strain-induced structural transformations that are accompanied by remarkable mobility enhancements up to about Δµ/µ≈300%. Our results provide a microscopic rationale for the recently discovered transport enhancement under strain and underscore the role of the internal structural degrees of freedom in the modulation of the perovskite electronic properties.

7.
Nature ; 469(7329): 189-93, 2011 Jan 13.
Article in English | MEDLINE | ID: mdl-21228872

ABSTRACT

As silicon is the basis of conventional electronics, so strontium titanate (SrTiO(3)) is the foundation of the emerging field of oxide electronics. SrTiO(3) is the preferred template for the creation of exotic, two-dimensional (2D) phases of electron matter at oxide interfaces that have metal-insulator transitions, superconductivity or large negative magnetoresistance. However, the physical nature of the electronic structure underlying these 2D electron gases (2DEGs), which is crucial to understanding their remarkable properties, remains elusive. Here we show, using angle-resolved photoemission spectroscopy, that there is a highly metallic universal 2DEG at the vacuum-cleaved surface of SrTiO(3) (including the non-doped insulating material) independently of bulk carrier densities over more than seven decades. This 2DEG is confined within a region of about five unit cells and has a sheet carrier density of ∼0.33 electrons per square lattice parameter. The electronic structure consists of multiple subbands of heavy and light electrons. The similarity of this 2DEG to those reported in SrTiO(3)-based heterostructures and field-effect transistors suggests that different forms of electron confinement at the surface of SrTiO(3) lead to essentially the same 2DEG. Our discovery provides a model system for the study of the electronic structure of 2DEGs in SrTiO(3)-based devices and a novel means of generating 2DEGs at the surfaces of transition-metal oxides.

8.
Phys Rev Lett ; 104(15): 156807, 2010 Apr 16.
Article in English | MEDLINE | ID: mdl-20482010

ABSTRACT

With infrared ellipsometry and transport measurements we investigated the electrons at the interface between LaAlO3 and SrTiO3. We obtained a sheet carrier concentration of N(s) approximately = 5-9x10(13) cm(-2), an effective mass of m*=3.2+/-0.4m(e), and a strongly frequency dependent mobility. The latter are similar as in bulk SrTi(1-x)Nb(x)O3 and therefore suggestive of polaronic correlations. We also determined the vertical concentration profile which has a strongly asymmetric shape with a rapid initial decay over the first 2 nm and a pronounced tail that extends to about 11 nm.

9.
Phys Rev Lett ; 102(21): 216804, 2009 May 29.
Article in English | MEDLINE | ID: mdl-19519126

ABSTRACT

Using a low-temperature conductive-tip atomic force microscope in cross-section geometry we have characterized the local transport properties of the metallic electron gas that forms at the interface between LaAlO3 and SrTiO3. At low temperature, we find that the carriers do not spread away from the interface but are confined within approximately 10 nm, just like at room temperature. Simulations taking into account both the large temperature and electric-field dependence of the permittivity of SrTiO3 predict a confinement over a few nm for sheet carrier densities larger than approximately 6x10(13) cm(-2). We discuss the experimental and simulations results in terms of a multiband carrier system. Remarkably, the Fermi wavelength estimated from Hall measurements is approximately 16 nm, indicating that the electron gas in on the verge of two dimensionality.

10.
J Phys Condens Matter ; 21(40): 406001, 2009 Oct 07.
Article in English | MEDLINE | ID: mdl-21832426

ABSTRACT

We report a study of Co-doped La(0.37)Sr(0.63)TiO(3-δ) thin films grown by pulsed laser deposition in various oxygen pressure conditions. X-ray absorption spectroscopy and magnetic circular dichroism measurements at the Co L(2,3) edges reveal that the cobalt mainly substitutes for the titanium and is in an ionic state. Nevertheless, in some films, indications of additional cobalt metallic impurities were found, suggesting that the intrinsic character of this magnetic system remains questionable.

11.
Phys Rev Lett ; 101(14): 147003, 2008 Oct 03.
Article in English | MEDLINE | ID: mdl-18851561

ABSTRACT

We use angle resolved photoemission spectroscopy to study the momentum dependence of the superconducting gap in NdFeAsO0.9F0.1 single crystals. We find that the Gamma hole pocket is fully gapped below the superconducting transition temperature. The value of the superconducting gap is 15+/-1.5 meV and its anisotropy around the hole pocket is smaller than 20% of this value-consistent with an isotropic or anisotropic s-wave symmetry of the order parameter. This is a significant departure from the situation in the cuprates, pointing to the possibility that the superconductivity in the iron arsenic based system arises from a different mechanism.

12.
Nat Mater ; 7(8): 621-5, 2008 Aug.
Article in English | MEDLINE | ID: mdl-18587402

ABSTRACT

At the interface between complex insulating oxides, novel phases with interesting properties may occur, such as the metallic state reported in the LaAlO(3)/SrTiO(3) system . Although this state has been predicted and reported to be confined at the interface, some studies indicate a much broader spatial extension, thereby questioning its origin. Here, we provide for the first time a direct determination of the carrier density profile of this system through resistance profile mappings collected in cross-section LaAlO(3)/SrTiO(3) samples with a conducting-tip atomic force microscope (CT-AFM). We find that, depending on specific growth protocols, the spatial extension of the high-mobility electron gas can be varied from hundreds of micrometres into SrTiO(3) to a few nanometres next to the LaAlO(3)/SrTiO(3) interface. Our results emphasize the potential of CT-AFM as a novel tool to characterize complex oxide interfaces and provide us with a definitive and conclusive way to reconcile the body of experimental data in this system.

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