tuning-oxide-properties-oxygen-vacancy-control-during-growth

Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing

Electrical, optical, and magnetic properties of oxide materials can often be controlled by varying the oxygen content. Here we outline two approaches for ...

Université Paris-Sud, Université Paris-Saclay

Technical University of Denmark

The discovery of two-dimensional electron gases (2DEGs) in SrTiO3-based heterostructures provides new opportunities for nanoelectronics. Herein, we create a new type of oxide 2DEG by the epitaxial-strain-induced polarization at an otherwise nonpolar perovskite-type interface of CaZrO3/SrTiO3. Remarkably, this heterointerface is atomically sharp and exhibits a high electron mobility exceeding 60,000 cm(2) V(-1) s(-1) at low temperatures. The 2DEG carrier density exhibits a critical dependence on the film thickness, in good agreement with the polarization induced 2DEG scheme.

Creation of high mobility two-dimensional electron gases via strain induced polarization at an otherwise nonpolar complex oxide interface.

The two-dimensional metal forming at the interface between an oxide insulator and SrTiO_{3} provides new opportunities for oxide electronics. However, the quantum Hall effect, one of the most fascinating effects of electrons confined in two dimensions, remains underexplored at these complex oxide heterointerfaces. Here, we report the experimental observation of quantized Hall resistance in a SrTiO_{3} heterointerface based on the modulation-doped amorphous-LaAlO_{3}/SrTiO_{3} heterostructure, which exhibits both high electron mobility exceeding 10,000  cm^{2}/V s and low carrier density on the order of ∼10^{12}  cm^{-2}. Along with unambiguous Shubnikov-de Haas oscillations, the spacing of the quantized Hall resistance suggests that the interface is comprised of a single quantum well with ten parallel conducting two-dimensional sub-bands. This provides new insight into the electronic structure of conducting oxide interfaces and represents an important step towards designing and understanding advanced oxide devices.

Quantization of Hall Resistance at the Metallic Interface between an Oxide Insulator and SrTiO_{3}.

In a solid-state host, attractive electron-electron interactions can lead to the formation of local electron pairs which play an important role in the understanding of prominent phenomena such as high T  superconductivity and the pseudogap phase. Recently, evidence of a paired ground state without superconductivity was demonstrated at the level of single electrons in quantum dots at the interface of LaAlO and SrTiO. Here, we present a detailed study of the excitation spectrum and transport processes of a gate-defined LaAlO/SrTiO quantum dot exhibiting pairing at low temperatures. For weak tunneling, the spectrum agrees with calculations based on the Anderson model with a negative effective charging energy U, and exhibits an energy gap corresponding to the Zeeman energy of the magnetic pair-breaking field. In contrast, for strong coupling, low-bias conductance is enhanced with a characteristic dependence on temperature, magnetic field and chemical potential consistent with the charge Kondo effect.Complex oxide devices provide a platform for studying and making use of strongly correlated electronic behavior. Here the authors present a LaAlO/SrTiO quantum dot and show that its transport behavior is consistent with the presence of attractive electron interactions and the charge Kondo effect.

Transport and excitations in a negative-U quantum dot at the LaAlO/SrTiO interface.

The ability to form freestanding oxide membranes of nanoscale thickness is of great interest for enabling material functionality and for integrating oxides in flexible electronic and photonic technologies. Recently, a route has been demonstrated for forming conducting heterostructure membranes of LaAlO and SrTiO, the canonical system for oxide electronics. In this route, the epitaxial growth of LaAlO on SrTiO resulted in a strained state that relaxed by producing freestanding membranes with random sizes and locations. Here, we extend the method to enable self-formed LaAlO/SrTiO micromembranes with control over membrane position, their lateral sizes from 2 to 20 μm, and with controlled transfer to other substrates of choice. This method opens up the possibility to study and use the two-dimensional electron gas in LaAlO/SrTiO membranes for advanced device concepts.

Size-Controlled Spalling of LaAlO/SrTiO Micromembranes.

Rashba interfaces yield efficient spin-charge interconversion and give rise to nonreciprocal transport phenomena. Here, we report magnetotransport experiments in few-nanometer-thick films of PdCoO, a delafossite oxide known to display a large Rashba splitting and surface ferromagnetism. By analyzing the angle dependence of the first- and second-harmonic longitudinal and transverse resistivities, we identify a Rashba-driven unidirectional magnetoresistance that competes with the anomalous Nernst effect below the Curie point. We estimate a Rashba coefficient of 0.75 ± 0.3 eV Å and argue that our results qualify delafossites as a new family of oxides for nanospintronics and spin-orbitronics, beyond perovskite materials.

Nonreciprocal Transport in a Rashba Ferromagnet, Delafossite PdCoO.

Freestanding oxide membranes constitute an intriguing material platform for new functionalities and allow integration of oxide electronics with technologically important platforms such as silicon. Sambri et al. recently reported a method to fabricate freestanding LaAlO/SrTiO (LAO/STO) membranes by spalling of strained heterostructures. Here, we first develop a scheme for the high-yield fabrication of membrane devices on silicon. Second, we show that the membranes exhibit metallic conductivity and a superconducting phase below ∼200 mK. Using anisotropic magnetotransport we extract the superconducting phase coherence length ξ ≈ 36-80 nm and establish an upper bound on the thickness of the superconducting electron gas  ≈ 17-33 nm, thus confirming its two-dimensional character. Finally, we show that the critical current can be modulated using a silicon-based backgate. The ability to form superconducting nanostructures of LAO/STO membranes, with electronic properties similar to those of the bulk counterpart, opens opportunities for integrating oxide nanoelectronics with silicon-based architectures.

A Two-Dimensional Superconducting Electron Gas in Freestanding LaAlO/SrTiO Micromembranes.

Recently, electrically conducting heterointerfaces between dissimilar band insulators (such as lanthanum aluminate and strontium titanate) have attracted considerable research interest. Charge transport and fundamental aspects of conduction have been thoroughly explored. Perhaps surprisingly, similar studies on conceptually much simpler conducting homointerfaces, such as domain walls, are not nearly so well developed. Addressing this disparity, magnetoresistance is herein reported in approximately conical 180° charged domain walls, in partially switched ferroelectric thin-film single-crystal lithium niobate. This system is ideal for such measurements: first, the conductivity difference between domains and domain walls is unusually large (a factor of 10 ) and hence currents driven through the thin film, between planar top and bottom electrodes, are overwhelmingly channeled along the walls; second, when electrical contact is made to the top and bottom of the domain walls and a magnetic field is applied along their cone axes, then the test geometry mirrors that of a Corbino disk: a textbook arrangement for geometric magnetoresistance measurement. Data imply carriers with extremely high room-temperature Hall mobilities of up to ≈3700 cm V s . This is an unparalleled value for oxide interfaces (and for bulk oxides) comparable to mobilities in other systems seen at cryogenic, rather than at room, temperature.

Ultrahigh Carrier Mobilities in Ferroelectric Domain Wall Corbino Cones at Room Temperature.

The integration of dissimilar materials in heterostructures has long been a cornerstone of modern materials science-seminal examples are 2D materials and van der Waals heterostructures. Recently, new methods have been developed that enable the realization of ultrathin freestanding oxide films approaching the 2D limit. Oxides offer new degrees of freedom, due to the strong electronic interactions, especially the 3d orbital electrons, which give rise to rich exotic phases. Inspired by this progress, a new platform for assembling freestanding oxide thin films with different materials and orientations into artificial stacks with heterointerfaces is developed. It is shown that the oxide stacks can be tailored by controlling the stacking sequences, as well as the twist angle between the constituent layers with atomically sharp interfaces, leading to distinct moiré patterns in the transmission electron microscopy images of the full stacks. Stacking and twisting is recognized as a key degree of structural freedom in 2D materials but, until now, has never been realized for oxide materials. This approach opens unexplored avenues for fabricating artificial 3D oxide stacking heterostructures with freestanding membranes across a broad range of complex oxide crystal structures with functionalities not available in conventional 2D materials.

Stacking and Twisting of Freestanding Complex Oxide Thin Films.

Complex oxide heterointerfaces contain a rich playground of novel physical properties and functionalities, which give rise to emerging technologies. Among designing and controlling the functional properties of complex oxide film heterostructures, vertically aligned nanostructure (VAN) films using a self-assembling bottom-up deposition method present great promise in terms of structural flexibility and property tunability. Here, we extend the bottom-up self-assembly to a new approach using a mixture containing a 2D layer-by-layer film growth, followed by a 3D VAN film growth. In this work, the two-phase nanocomposite thin films are based on LaAlO :LaBO , grown on lattice-mismatched SrTiO . The 2D-to-3D transient structural assembly is primarily controlled by the composition ratio, leading to the coexistence of multiple interfacial properties, 2D electron gas and magnetic anisotropy. This approach provides multidimensional film heterostructures which enrich emergent phenomena for multifunctional applications. This article is protected by copyright. All rights reserved.

Article	Year
Creation of high mobility two-dimensional electron gases via strain induced polarization at an otherwise nonpolar complex oxide interface. Nano letters\| PubMed ID: 25692804	2015
Quantization of Hall Resistance at the Metallic Interface between an Oxide Insulator and SrTiO_{3}. Physical review letters\| PubMed ID: 27610874	2016
Transport and excitations in a negative-U quantum dot at the LaAlO/SrTiO interface. Nature communications\| PubMed ID: 28855569	2017
Size-Controlled Spalling of LaAlO/SrTiO Micromembranes. ACS applied materials & interfaces\| PubMed ID: 33661598	2021
Nonreciprocal Transport in a Rashba Ferromagnet, Delafossite PdCoO. Nano letters\| PubMed ID: 34613718	2021
A Two-Dimensional Superconducting Electron Gas in Freestanding LaAlO/SrTiO Micromembranes. Nano letters\| PubMed ID: 35679577	2022
Ultrahigh Carrier Mobilities in Ferroelectric Domain Wall Corbino Cones at Room Temperature. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 35733393	2022
Stacking and Twisting of Freestanding Complex Oxide Thin Films. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 35901262	2022
Controlled Electronic and Magnetic Landscape in Self-Assembled Complex Oxide Heterostructures. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 37154173	2023

Felix Trier

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