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Register a new userFrom the SrTiO3 Surface to the LAlO3/SrTiO3 Interface: How thickness is critical
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Novel properties arising at interfaces between transition metal oxides, particularly the conductivity at the interface of LaAlO3 (LAO) and SrTiO3 (STO) band insulators, have generated new paradigms, challenges, and opportunities in condensed matter physics. Conventional transport measurements have established that intrinsic conductivity appears in LAO/STO interfaces when the LAO film matches or exceeds a critical thickness of 4 unit cells (uc). Recently, a number of experiments raise important questions about the role of the LAO film, the influence of photons, and the effective differences between vacuum/STO and LAO/STO, both above and below the standard critical thickness. Here, using angle-resolved photoemission spectroscopy (ARPES) on in situ prepared samples, as well as resonant inelastic x-ray scattering (RIXS), we study how the metallic STO surface state evolves during the growth of a crystalline LAO film. In all the samples, the character of the conduction bands, their carrier densities, the Ti3+ crystal fields, and the responses to photon irradiation bear strong similarities. However, LAO/STO interfaces exhibit intrinsic instability toward in-plane folding of the Fermi surface at and above the 4-uc thickness threshold. This ordering distinguishes these heterostructures from bare STO and sub-critical-thickness LAO/STO and coincides with the onset of unique properties such as magnetism and built-in conductivity.
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Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 (LAO/STO) that hosts two-dimensional electron system (2DES). Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here, we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LAO overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures.
In heterostructures of LaAlO3 (LAO) and SrTiO3 (STO), two nonmagnetic insulators, various forms of magnetism have been observed [1-7], which may [8, 9] or may not [10] arise from interface charge carriers that migrate from the LAO to the interface in an electronic reconstruction [11]. We image the magnetic landscape [5] in a series of n-type samples of varying LAO thickness. We find ferromagnetic patches that appear only above a critical thickness, similar to that for conductivity [12]. Consequently we conclude that an interface reconstruction is necessary for the formation of magnetism. We observe no change in ferromagnetism with gate voltage, and detect ferromagnetism in a non-conducting p-type sample, indicating that the carriers at the interface do not need to be itinerant to generate magnetism. The fact that the ferromagnetism appears in isolated patches whose density varies greatly between samples strongly suggests that disorder or local strain induce magnetism in a population of the interface carriers.
Interface engineering is an extremely useful tool for systematically investigating materials and the various ways materials interact with each other. We describe different interface engineering strategies designed to reveal the origin of the electric and magnetic dead-layer at La0.67Sr0.33MnO3 interfaces. La0.67Sr0.33MnO3 is a key example of a strongly correlated peroskite oxide material in which a subtle balance of competing interactions gives rise to a ferromagnetic metallic groundstate. This balance, however, is easily disrupted at interfaces. We systematically vary the dopant profile, the disorder and the oxygen octahedra rotations at the interface to investigate which mechanism is responsible for the dead layer. We find that the magnetic dead layer can be completely eliminated by compositional interface engineering such that the polar discontinuity at the interface is removed. This, however, leaves the electrical dead-layer largely intact. We find that deformations in the oxygen octahedra network at the interface are the dominant cause for the electrical dead layer.
Oxide interfaces, including the LaAlO3/SrTiO3 interface, have been a subject of intense interest for over a decade due to their rich physics and potential as low dimensional nanoelectronic systems. The field has reached the stage where efforts are invested in developing devices. It is critical now to understand the functionalities and limitations of such devices. Recent scanning probe measurements of the LaAlO3/SrTiO3 interface have revealed locally enhanced current flow and accumulation of charge along channels related to SrTiO3 structural domains. These observations raised a key question regarding the role these modulations play in the macroscopic properties of devices. Here we show that the microscopic picture, mapped by scanning superconducting quantum interference device, accounts for a substantial part of the macroscopically measured transport anisotropy. We compared local flux data with transport values, measured simultaneously, over various SrTiO3 domain configurations. We show a clear relation between maps of local current density over specific domain configurations and the measured anisotropy for the same device. The domains divert the direction of current flow, resulting in a direction dependent resistance. We also show that the modulation can be significant and that in some cases up to 95% of the current is modulated over the channels. The orientation and distribution of the SrTiO3 structural domains change between different cooldowns of the same device or when electric fields are applied, affecting the device behavior. Our results, highlight the importance of substrate physics, and in particular, the role of structural domains, in controlling electronic properties of LaAlO3/SrTiO3 devices. Further, these results point to new research directions, exploiting the STO domains ability to divert or even carry current.
The quasi 2D electron system (q2DES) that forms at the interface between LaAlO3 and SrTiO3 has attracted much attention from the oxide electronics community. One of its hallmark features is the existence of a critical LaAlO3 thickness of 4 unit-cells (uc) for interfacial conductivity to emerge. In this paper, the chemical, electronic, and transport properties of LaAlO3/SrTiO3 samples capped with different metals grown in a system combining pulsed laser deposition, sputtering, and in situ X-ray photoemission spectroscopy are investigated. The results show that for metals with low work function a q2DES forms at 1-2 uc of LaAlO3 and is accompanied by a partial oxidation of the metal, a phenomenon that affects the q2DES properties and triggers the formation of defects. In contrast, for noble metals, the critical thickness is increased above 4 uc. The results are discussed in terms of a hybrid mechanism that incorporates electrostatic and chemical effects.
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