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            Abstract Charge ordering (CO), characterized by a periodic modulation of electron density and lattice distortion, has been a fundamental topic in condensed matter physics, serving as a potential platform for inducing novel functional properties. The charge-ordered phase is known to occur in a doped system with highd-electron occupancy, rather than low occupancy. Here, we report the realization of the charge-ordered phase in electron-doped (100) SrTiO3epitaxial thin films that have the lowestd-electron occupancy i.e.,d1-d0. Theoretical calculation predicts the presence of a metastable CO state in the bulk state of electron-doped SrTiO3. Atomic scale analysis reveals that (100) surface distortion favors electron-lattice coupling for the charge-ordered state, and triggering the stabilization of the CO phase from a correlated metal state. This stabilization extends up to six unit cells from the top surface to the interior. Our approach offers an insight into the means of stabilizing a new phase of matter, extending CO phase to the lowest electron occupancy and encompassing a wide range of 3dtransition metal oxides.more » « lessFree, publicly-accessible full text available December 1, 2025
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            KTaO3heterostructures have recently attracted attention as model systems to study the interplay of quantum paraelectricity, spin-orbit coupling, and superconductivity. However, the high and low vapor pressures of potassium and tantalum present processing challenges to creating heterostructure interfaces clean enough to reveal the intrinsic quantum properties. Here, we report superconducting heterostructures based on high-quality epitaxial (111) KTaO3thin films using an adsorption-controlled hybrid PLD to overcome the vapor pressure mismatch. Electrical and structural characterizations reveal that the higher-quality heterostructure interface between amorphous LaAlO3and KTaO3thin films supports a two-dimensional electron gas with substantially higher electron mobility, superconducting transition temperature, and critical current density than that in bulk single-crystal KTaO3-based heterostructures. Our hybrid approach may enable epitaxial growth of other alkali metal–based oxides that lie beyond the capabilities of conventional methods.more » « less
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            The thermoelectric properties of quasi‐1D electron waveguides at the LaAlO3/SrTiO3interface at millikelvin temperatures are investigated. A highly enhanced and oscillating thermopower is found for these electron waveguides, with values exceeding 100 μV K−1at 0.1 K in the electron‐depletion regime. The Mott relation, which governs the band‐term thermopower of noninteracting electrons, agrees well with the experimental findings in and around regimes where strongly attractive electron–electron interactions lead to a previously reported Pascal series of conductance explained by bound states of electrons. These results pave the way for quantized thermal transport studies of emergent electron liquid phases in which transport is governed by quasiparticles with charges that are integer multiples or fractions of an electron.more » « less
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            null (Ed.)In recent years, lanthanum aluminate/strontium titanate (LAO/STO) heterointerfaces have been used to create a growing family of nanoelectronic devices based on nanoscale control of LAO/STO metal-to-insulator transition. The properties of these devices are wide-ranging, but they are restricted by nature of the underlying thick STO substrate. Here, single-crystal freestanding membranes based on LAO/STO heterostructures were fabricated, which can be directly integrated with other materials via van der Waals stacking. The key properties of LAO/STO are preserved when LAO/STO membranes are formed. Conductive atomic force microscope lithography is shown to successfully create reversible patterns of nanoscale conducting regions, which survive to millikelvin temperatures. The ability to form reconfigurable conducting nanostructures on LAO/STO membranes opens opportunities to integrate a variety of nanoelectronics with silicon-based architectures and flexible, magnetic, or superconducting materials.more » « less
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            null (Ed.)The quest to understand, design, and synthesize new forms of quantum matter guides much of contemporary research in condensed matter physics. One-dimensional (1D) electronic systems form the basis for some of the most interesting and exotic phases of quantum matter. Here, we describe a family of quasi-1D nanostructures, based on LaAlO 3 /SrTiO 3 electron waveguides, in which a sinusoidal transverse spatial modulation is imposed. These devices display unique dispersive features in the subband spectra, namely, a sizeable shift (∼7 T) in the spin-dependent subband minima, and fractional conductance plateaus. The first property can be understood as an engineered spin-orbit interaction associated with the periodic acceleration of electrons as they undulate through the nanowire (ballistically), while the second property signifies the presence of enhanced electron-electron scattering in this system. The ability to engineer these interactions in quantum wires contributes to the tool set of a 1D solid-state quantum simulation platform.more » « less
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            This perspective considers the enormous promise of epitaxial functional transition metal oxide thin films for future applications in low power electronic and energy applications since they offer wide-ranging and highly tunable functionalities and multifunctionalities, unrivaled among other classes of materials. It also considers the great challenges that must be overcome for transition metal oxide thin films to meet what is needed in the application domain. These challenges arise from the presence of intrinsic defects and strain effects, which lead to extrinsic defects. Current conventional thin film deposition routes often cannot deliver the required perfection and performance. Since there is a strong link between the physical properties, defects and strain, routes to achieving more perfect materials need to be studied. Several emerging methods and modifications of current methods are presented and discussed. The reasons these methods better address the perfection challenge are considered and evaluated.more » « less
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            One-dimensional electronic systems can support exotic collective phases because of the enhanced role of electron correlations. We describe the experimental observation of a series of quantized conductance steps within strongly interacting electron waveguides formed at the lanthanum aluminate–strontium titanate (LaAlO 3 /SrTiO 3 ) interface. The waveguide conductance follows a characteristic sequence within Pascal’s triangle: (1, 3, 6, 10, 15, …) ⋅ e 2 /h , where e is the electron charge and h is the Planck constant. This behavior is consistent with the existence of a family of degenerate quantum liquids formed from bound states of n = 2, 3, 4, … electrons. Our experimental setup could provide a setting for solid-state analogs of a wide range of composite fermionic phases.more » « less
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            Oxygen vacancies ( V O • • ) play a critical role as defects in complex oxides in establishing functionality in systems including memristors, all-oxide electronics, and electrochemical cells that comprise metal-insulator-metal or complex oxide heterostructure configurations. Improving oxide-oxide interfaces necessitates a direct, spatial understanding of vacancy distributions that define electrochemically active regions. We show vacancies deplete over micrometer-level distances in Nb-doped SrTiO 3 (Nb:SrTiO 3 ) substrates due to deposition and post-annealing processes. We convert the surface potential across a strontium titanate/yttria-stabilized zirconia (STO/YSZ) heterostructured film to spatial (<100 nm) vacancy profiles within STO using ( T = 500°C) in situ scanning probes and semiconductor analysis. Oxygen scavenging occurring during pulsed laser deposition reduces Nb:STO substantially, which partially reoxidizes in an oxygen-rich environment upon cooling. These results (i) introduce the means to spatially resolve quantitative vacancy distributions across oxide films and (ii) indicate the mechanisms by which oxide thin films enhance and then deplete vacancies within the underlying substrate.more » « less
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