The inverse spinel ferrimagnetic NiCo2O4possesses high magnetic Curie temperature TC, high spin polarization, and strain-tunable magnetic anisotropy. Understanding the thickness scaling limit of these intriguing magnetic properties in NiCo2O4thin films is critical for their implementation in nanoscale spintronic applications. In this work, we report the unconventional magnetotransport properties of epitaxial (001) NiCo2O4films on MgAl2O4substrates in the ultrathin limit. Anomalous Hall effect measurements reveal strong perpendicular magnetic anisotropy for films down to 1.5 unit cell (1.2 nm), while TCfor 3 unit cell and thicker films remains above 300 K. The sign change in the anomalous Hall conductivity [Formula: see text] and its scaling relation with the longitudinal conductivity ([Formula: see text]) can be attributed to the competing effects between impurity scattering and band intrinsic Berry curvature, with the latter vanishing upon the thickness driven metal–insulator transition. Our study reveals the critical role of film thickness in tuning the relative strength of charge correlation, Berry phase effect, spin–orbit interaction, and impurity scattering, providing important material information for designing scalable epitaxial magnetic tunnel junctions and sensing devices using NiCo2O4. 
                        more » 
                        « less   
                    
                            
                            Magnetotransport Anomaly in Room‐Temperature Ferrimagnetic NiCo 2 O 4 Thin Films
                        
                    
    
            Abstract The inverse spinel ferrimagnetic NiCo2O4presents a unique model system for studying the competing effects of crystalline fields, magnetic exchange, and various types of chemical and lattice disorder on the electronic and magnetic states. Here, magnetotransport anomalies in high‐quality epitaxial NiCo2O4thin films resulting from the complex energy landscape are reported. A strong out‐of‐plane magnetic anisotropy, linear magnetoresistance, and robust anomalous Hall effect above 300 K are observed in 5–30 unit cell NiCo2O4films. The anomalous Hall resistance exhibits a nonmonotonic temperature dependence that peaks around room temperature, and reverses its sign at low temperature in films thinner than 20 unit cells. The scaling relation between the anomalous Hall conductivity and longitudinal conductivity reveals the intricate interplay between the spin‐dependent impurity scattering, band intrinsic Berry phase effect, and electron correlation. This study provides important insights into the functional design of NiCo2O4for developing spinel‐based spintronic applications. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 1710461
- PAR ID:
- 10461200
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 31
- Issue:
- 4
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            The ferrimagnetic inverse spinel NiCo 2 O 4 has attracted extensive research interest for its versatile electrochemical properties, robust magnetic order, high conductivity, and fast spin dynamics, as well as its highly tunable nature due to the closely coupled charge, spin, orbital, lattice, and defect effects. Single-crystalline epitaxial thin films of NiCo 2 O 4 present a model system for elucidating the intrinsic physical properties and strong tunability, which are not viable in bulk single crystals. In this Perspective, we discuss the recent advances in epitaxial NiCo 2 O 4 thin films, focusing on understanding its unusual magnetic and transport properties in light of crystal structure and electronic structure. The perpendicular magnetic anisotropy in compressively strained NiCo 2 O 4 films is explained by considering the strong spin–lattice coupling, particularly on Co ions. The prominent effect of growth conditions reveals the complex interplay between the crystal structure, cation stoichiometry, valence state, and site occupancy. NiCo 2 O 4 thin films also exhibit various magnetotransport anomalies, including linear magnetoresistance and sign change in anomalous Hall effect, which illustrate the competing effects of band-intrinsic Berry phase and impurity scattering. The fundamental understanding of these phenomena will facilitate the functional design of NiCo 2 O 4 thin films for nanoscale spintronic applications.more » « less
- 
            Abstract Understanding intrinsic exchange bias in nominally single‐component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo2O4, the origin of intrinsic exchange bias in NiCo2O4(111) films deposited on Al2O3(0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X‐ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo2O4(111)/Al2O3(0001) arises from a reconstructed antiferromagnetic rock‐salt NixCo1‐xO layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo2O4, an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.more » « less
- 
            Abstract X-ray photoelectron spectroscopy (XPS) shows that dramatic changes in the core level binding energies can provide strong indications of transitions between more dielectric and more metallic CoFe2O4and NiCo2O4thin films. These significant variations in the XPS core level binding energies are possible with a combination of annealing and oxygen exposure; however, the behaviors of the CoFe2O4and NiCo2O4thin films are very different. The XPS Co and Fe 2p3/2core levels for the CoFe2O4thin film at room temperature show large photovoltaic surface charging, leading to binding energy shifts, characteristic of a highly dielectric (or insulating) surface at room temperature. The photovoltaic charging, observed in the XPS binding energies of the Co and Fe 2p3/2core levels, decreases with increasing temperature. The XPS core level binding energies of CoFe2O4thin film saturated at lower apparent binding energies above 455 K. This result shows that the prepared CoFe2O4thin film can be dielectric at room temperature but become more metallic at elevated temperatures. The dielectric nature of the CoFe2O4thin film was restored only when the film was annealed in sufficient oxygen, indicating that oxygen vacancies play an important role in the transition of the film from dielectric (or insulating) to metallic. In contrast, the XPS studies of initially metallic NiCo2O4thin film demonstrated that annealing NiCo2O4thin film led to a more dielectric or insulating film. The original more metallic character of the NiCo2O4film was restored when the NiCo2O4was annealed in sufficient oxygen. Effective activation energies are estimated for the carriers from a modified Arrhenius-type model applied to the core level binding energy changes of the CoFe2O4and NiCo2O4thin films, as a function of temperature. The origin of the carriers, however, is not uniquely identified. This work illustrates routes to regulate the surface metal-to-insulator transition of dielectric oxides, especially in the case of insulating NiCo2O4thin film that can undergo reversible metal-to-insulator transition with temperature.more » « less
- 
            Abstract In an effort to reconcile the various interpretations for the cation components of the 2p3/2observed in x-ray photoelectron spectroscopy (XPS) of several spinel oxide materials, the XPS spectra of both spinel alloy nanoparticles and crystalline thin films are compared. We observed that different components of the 2p3/2core level XPS spectra, of these inverse spinel thin films, are distinctly surface and bulk weighted, indicating surface-to-bulk core level shifts in the binding energies. Surface-to-bulk core level shifts in binding energies of Ni and Fe 2p3/2core levels of NiFe2O4thin film are observed in angle-resolved XPS. The ratio between surface-weighted components and bulk-weighted components of the Ni and Fe core levels shows appreciable dependency on photoemission angle, with respect to surface normal. XPS showed that the ferrite nanoparticles NixCo1−xFe2O4(x= 0.2, 0.5, 0.8, 1) resemble the surface of the NiFe2O4thin film. Surface-to-bulk core level shifts are also observed in CoFe2O4and NiCo2O4thin films but not as significantly as in NiFe2O4thin film. Estimates of surface stoichiometry of some spinel oxide nanoparticles and thin films suggested that the apportionment between cationic species present could be farther from expectations for thin films as compared to what is seen with nanoparticles.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
