Abstract Control of BO6octahedral rotations at the heterointerfaces of dissimilar ABO3perovskites has emerged as a powerful route for engineering novel physical properties. However, its impact length scale is constrained at 2–6 unit cells close to the interface and the octahedral rotations relax quickly into bulk tilt angles away from interface. Here, a long‐range (up to 12 unit cells) suppression of MnO6octahedral rotations in La0.9Ba0.1MnO3through the formation of superlattices with SrTiO3can be achieved. The suppressed MnO6octahedral rotations strongly modify the magnetic and electronic properties of La0.9Ba0.1MnO3and hence create a new ferromagnetic insulating state with enhanced Curie temperature of 235 K. The emergent properties in La0.9Ba0.1MnO3arise from a preferential occupation of the out‐of‐plane Mnd3z2−r2orbital and a reduced Mn egbandwidth, induced by the suppressed octahedral rotations. The realization of long‐range tuning of BO6octahedra via superlattices can be applicable to other strongly correlated perovskites for exploring new emergent quantum phenomena. 
                        more » 
                        « less   
                    
                            
                            Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films
                        
                    
    
            Abstract Ultrathin epitaxial films of ferromagnetic insulators (FMIs) with Curie temperatures near room temperature are critically needed for use in dissipationless quantum computation and spintronic devices. However, such materials are extremely rare. Here, a room‐temperature FMI is achieved in ultrathin La0.9Ba0.1MnO3films grown on SrTiO3substrates via an interface proximity effect. Detailed scanning transmission electron microscopy images clearly demonstrate that MnO6octahedral rotations in La0.9Ba0.1MnO3close to the interface are strongly suppressed. As determined from in situ X‐ray photoemission spectroscopy, OK‐edge X‐ray absorption spectroscopy, and density functional theory, the realization of the FMI state arises from a reduction of Mn egbandwidth caused by the quenched MnO6octahedral rotations. The emerging FMI state in La0.9Ba0.1MnO3together with necessary coherent interface achieved with the perovskite substrate gives very high potential for future high performance electronic devices. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 1809520
- PAR ID:
- 10458614
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Science
- Volume:
- 7
- Issue:
- 1
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Abstract At crystalline interfaces where a valence-mismatch exists, electronic, and structural interactions may occur to relieve the polar mismatch, leading to the stabilization of non-bulk-like phases. We show that spontaneous reconstructions at polar La0.7Sr0.3MnO3interfaces are correlated with suppressed ferromagnetism for film thicknesses on the order of a unit cell. We investigate the structural and magnetic properties of valence-matched La0.7Sr0.3CrO3/La0.7Sr0.3MnO3interfaces using a combination of high-resolution electron microscopy, first principles theory, synchrotron X-ray scattering and magnetic spectroscopy and temperature-dependent magnetometry. A combination of an antiferromagnetic coupling between the La0.7Sr0.3CrO3and La0.7Sr0.3MnO3layers and a suppression of interfacial polar distortions are found to result in robust long-range ferromagnetic ordering for ultrathin La0.7Sr0.3MnO3. These results underscore the critical importance of interfacial structural and magnetic interactions in the design of devices based on two-dimensional oxide magnetic systems.more » « less
- 
            Abstract Solid‐oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure–property relationships that would enable the rational design of better materials. Here, using epitaxial thin‐film growth, synchrotron radiation, impedance spectroscopy, and density‐functional theory, the impact of structural parameters (i.e., unit‐cell volume and octahedral rotations) on ionic conductivity is delineated in La0.9Sr0.1Ga0.95Mg0.05O3–δ. As compared to the zero‐strain state, compressive strain reduces the unit‐cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit‐cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit‐cell volumes and octahedral rotations decrease migration barriers and create low‐energy migration pathways, respectively. The desired combination of large unit‐cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit‐cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈2.5 at around 600 °C is observed, which sheds new light on the rational design of ion‐conducting perovskite electrolytes.more » « less
- 
            Abstract Solid-state control of the thermal conductivity of materials is of exceptional interest for novel devices such as thermal diodes and switches. Here, we demonstrate the ability tocontinuouslytune the thermal conductivity of nanoscale films of La0.5Sr0.5CoO3-δ(LSCO) by a factor of over 5, via a room-temperature electrolyte-gate-induced non-volatile topotactic phase transformation from perovskite (withδ≈ 0.1) to an oxygen-vacancy-ordered brownmillerite phase (withδ= 0.5), accompanied by a metal-insulator transition. Combining time-domain thermoreflectance and electronic transport measurements, model analyses based on molecular dynamics and Boltzmann transport equation, and structural characterization by X-ray diffraction, we uncover and deconvolve the effects of these transitions on heat carriers, including electrons and lattice vibrations. The wide-range continuous tunability of LSCO thermal conductivity enabled by low-voltage (below 4 V) room-temperature electrolyte gating opens the door to non-volatile dynamic control of thermal transport in perovskite-based functional materials, for thermal regulation and management in device applications.more » « less
- 
            Abstract The superior size and power scaling potential of ferroelectric-gated Mott transistors makes them promising building blocks for developing energy-efficient memory and logic applications in the post-Moore’s Law era. The close to metallic carrier density in the Mott channel, however, imposes the bottleneck for achieving substantial field effect modulation via a solid-state gate. Previous studies have focused on optimizing the thickness, charge mobility, and carrier density of single-layer correlated channels, which have only led to moderate resistance switching at room temperature. Here, we report a record high nonvolatile resistance switching ratio of 38,440% at 300 K in a prototype Mott transistor consisting of a ferroelectric PbZr0.2Ti0.8O3gate and anRNiO3(R: rare earth)/La0.67Sr0.33MnO3composite channel. The ultrathin La0.67Sr0.33MnO3buffer layer not only tailors the carrier density profile inRNiO3through interfacial charge transfer, as corroborated by first-principles calculations, but also provides an extended screening layer that reduces the depolarization effect in the ferroelectric gate. Our study points to an effective material strategy for the functional design of complex oxide heterointerfaces that harnesses the competing roles of charge in field effect screening and ferroelectric depolarization effects.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
