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Divine P. Kumah

Publications and source records attributed to Divine P. Kumah.

At least 19 recordsLinked to original sources

Superconductivity in spin-orbit coupled BaBi$_3$ formed by in situ reduction of bismuthate films

Oxygen-scavenging at oxide heterointerfaces has emerged as a powerful route for stabilizing metastable phases that exhibit interesting phenomena, including high-mobility two-dimensional electron gases and high T$_{c}$ superconductivity. We investigate structural and chemical interactions at the heterointerface formed between Al or Eu and the charged-ordered insulator, BaBiO$_3$, leading to emergent superconductivity at 6 K. A combination of X-ray diffraction and electron microscopy measurements shows that oxygen scavenging by the Eu and Al adlayers leads to the formation of superconducting intermetallic BaBi$_3$ in nominal Eu/BaBiO$_3$ and Al/BaBiO$_3$ bilayers. Anisotropic magnetotransport measurements and current-voltage signatures of quasi two-dimensional superconductivity are observed. The mechanisms behind quasi-two-dimensional superconductivity and the role of disorder remain to be clarified. These findings highlight the potential for the use of in situ reduction of bismuthate heterostructures as a platform for stabilizing materials with exotic functional properties. Additionally, the strong spin-orbit coupling at the Bi sites may pave the way for the realization of high T$_{c}$ topological superconductivity.

cond-mat.supr-con

Electrostatic control of quantum phases in KTaO3-based planar constrictions

Two-dimensional electron gases (2DEGs) formed at complex oxide interfaces offer a unique platform to engineer quantum nanostructures. However, scalable fabrication of locally addressable devices in these materials remains challenging. Here, we demonstrate an efficient fabrication approach by patterning narrow constrictions in a superconducting KTaO3-based heterostructure. The constrictions are individually tunable via the coplanar side gates formed within the same 2DEG plane. Our technique leverages the high dielectric permittivity of KTaO3 (epsilon_r ~ 5000) to achieve strong electrostatic modulation of the superconducting 2DEG. Transport measurements through the constriction reveal a range of transport regimes: Within the superconducting state, we demonstrate efficient modulation of the critical current and Berezinskii Kosterlitz Thouless (BKT) transition temperature at the weak link. Further tuning of the gate voltage reveals an unexpectedly regular Coulomb blockade pattern. All of these states are achievable with a side gate voltage |V_SG| < 1 V. The fabrication process is scalable and versatile, enabling a platform both to make superconducting field-effect transistors and to study a wide array of physical phenomena present at complex oxide interfaces.

cond-mat.supr-con

Spin-to-charge conversion at KTaO3(111) interfaces

Rashba spin-orbit coupling locks the spin with momentum of charge carriers at the broken inversion interfaces, which could generate a large spin galvanic response. Here, we demonstrate spin-to-charge conversion (inverse Rashba-Edelstein effect) in KTaO3(111) two-dimensional electron systems. We explain the results in the context of electronic structure, orbital character, and spin texture at the KTaO3(111) interfaces. We also show that the angle dependence of the spin-to-charge conversion on in-plane magnetic field exhibits a nontrivial behavior which matches the symmetry of the Fermi states. Results point to opportunities to use spin-to-charge conversion as a tool to investigate the electronic structure and spin texture.

cond-mat.mtrl-sci

Violation of Pauli Limit at KTaO3(110) Interfaces

The superconducting order parameter at the KTaO3 interfaces and its dependence on interface orientation remains a subject of debate. The superconductivity at these interfaces exhibits strong resilience against in-plane magnetic field and violates Pauli limit. The interface orientation dependence of critical field and violation of Pauli limit, however, have not been investigated. To address this problem, we grew epitaxial LaMnO3/KTaO3 heterostructures using molecular beam epitaxy. We show that superconductivity is extremely robust against the in-plane magnetic field. Our results indicate that the interface orientation, despite impacting the critical temperature, does not affect the ratio of critical field to the Pauli limiting field. These results offer opportunities to engineer superconductors which are resilient against magnetic field.

cond-mat.supr-con

Tuning the interlayer coupling in La0.7Sr0.3Mn0.95Ru0.05O3 / LaNiO3 multilayers with perpendicular magnetic anisotropy

In ferromagnetic oxide epitaxial multilayers, magnetic properties and interlayer coupling are determined by a variety of factors. Beyond the contribution of interlayer exchange coupling, strain and interfacial effects, such as structural reconstructions or charge transfer, play significant roles, resulting in complex magnetic behaviour. In this study the interlayer coupling of ferromagnetic La0.7Sr0.3Mn0.95Ru0.05O3 (LSMRO) layers (8 nm thick) was investigated, when separated by epitaxial spacers of paramagnetic metallic LaNiO3 (LNO), in stacks exhibiting perpendicular magnetic anisotropy. By varying the thickness of the spacer, it was found that the coupling between two LSMRO layers changes from antiferromagnetic (with a 4 unit cell thick LNO spacer) to ferromagnetic (with a 6 unit cells thick LNO spacer). For multilayers comprising five LSMRO layers and a 4 unit cell thick LNO spacer, the antiferromagnetic coupling was preserved. However, the effective magnetic anisotropy changed, causing the magnetization to cant more towards the in-plane direction. This behavior was corroborated by X-ray magnetic circular dichroism (XMCD) investigations at the Mn and Ni L3-edges. The XMCD results indicated that the 4 unit cells thick LNO spacer in the multilayer become magnetically ordered, closely following the magnetization of adjacent LSMRO layers.

cond-mat.mtrl-sci

The structure of Ferroelectric BaBiO$_3$/BaTiO$_3$ Interfaces grown by Molecular Beam Epitaxy

We investigate the lattice structure of heterostructures comprising of ferroelectric BaTiO$_3$ (BTO) thin films and BaBiO$_3$ (BBO), the insulating parent-compound of the high Tc superconductor. Motivated by theoretical predictions of exotic phenomena in BBO-based heterostructures including interfacial conductivity, superconductivity and topologically-protected states, we synthesize BTO/BBO heterostructures by molecular beam epitaxy and characterize their structural properties by in-situ reflection high energy electron diffraction and ex-situ high-resolution synchrotron X-ray diffraction, Raman spectroscopy and piezoforce microscopy. For heterostructures with 4 uc BBO layers, reciprocal space maps indicate strain relaxation relative to the SrTiO$_3$ substrate. We observe a strong tetragonal distortion for heterostructures with 2 unit cells BBO coherently strained to the BTO layers. Raman spectroscopy measurements indicate a suppression of the breathing mode distortion associated with the charge density wave in bulk BBO. The ferroelectric properties of the system are confirmed by piezoforce microscopy measurements. The coupling between the ferroelectric polarization and the electronic states in BBO may potentially serve as a starting point for tunable electrostatic doping to realize the novel predicted states in the atomically-thin BBO layers.

cond-mat.mtrl-sci

The role of interfacial interactions and oxygen vacancies in tuning magnetic anisotropy in LaCrO$_{3}$/LaMnO$_{3}$ heterostructures

The interplay of lattice, electronic, and spin degrees of freedom at epitaxial complex oxide interfaces provides a route to tune their magnetic ground states. Unraveling the competing contributions is critical for tuning their functional properties. We investigate the relationship between magnetic ordering and magnetic anisotropy and the lattice symmetry, oxygen content, and film thickness in compressively strained LaMnO$_3$/LaCrO$_3$ superlattices. Mn-O-Cr antiferromagnetic superexchange interactions across the heterointerface resulting in a net ferrimagnetic magnetic structure. Bulk magnetometry measurements reveal isotropic in-plane magnetism for as-grown oxygen-deficient thinner thin samples due to equal fractions of orthorhombic a+a-c-, and a-a+c- twin domains. As the superlattice thickness is increased, in-plane magnetic anisotropy emerges as the fraction of the a+a-c- domain increases. On annealing in oxygen, the suppression of oxygen vacancies results in a contraction of the lattice volume, and an orthorhombic to rhombohedral transition leads to isotropic magnetism independent of the film thickness. The complex interactions are investigated using high-resolution synchrotron diffraction and X-ray absorption spectroscopy. These results highlight the role of the evolution of structural domains with film thickness, interfacial spin interactions, and oxygen-vacancy-induced structural phase transitions in tuning the magnetic properties of complex oxide heterostructures.

cond-mat.mtrl-sci

In-situ scattering studies of superconducting vacancy-ordered monoclinic TiO thin films

We investigate the structural and transport properties of vacancy-ordered monoclinic superconducting $\mathrm{TiO}$ thin films grown by molecular beam epitaxy. The evolution of the crystal structure during growth is monitored by in-situ synchrotron X-ray diffraction. Long-range ordering of Ti and O vacancies in the disordered cubic phase stabilizes the vacancy-ordered monoclinic TiO phase. The reduced structural disorder arising from vacancy-ordering is correlated with a superconductor-metal transition (SMT) in contrast to the superconductor-insulator transition (SIT) observed in cubic TiO, orthorhombic $Ti_2O_3$, and the Magneli $γ-Ti_3O_5$ and $γ-Ti_4O_7$ phase. Magnetoresistance measurements for the SIT phases indicate superconducting fluctuations persisting in the normal phase. These results confirm the role of disorder related to Ti and O vacancies and structural inhomogeneity in determining the electronic properties of the normal state of titanium oxide-based superconductors.

cond-mat.supr-con

Enhanced Critical Field of Superconductivity at an Oxide Interface

The nature of superconductivity and its interplay with strong spin-orbit coupling at the KTaO3(111) interfaces remains a subject of debate. To address this problem, we grew epitaxial LaMnO3/KTaO3(111) heterostructures. We show that superconductivity is robust against the in-plane magnetic field, with the critical field of superconductivity reaching 25 T in optimally doped heterostructures. The superconducting order parameter is highly sensitive to carrier density. We argue that spin-orbit coupling drives the formation of anomalous quasiparticles with vanishing magnetic moment, providing the condensate significant immunity against magnetic fields beyond the Pauli paramagnetic limit. These results offer design opportunities for superconductors with extreme resilience against magnetic field.

cond-mat.supr-con

Oxygen vacancy-induced anomalous Hall effect in a nominally non-magnetic oxide

The anomalous Hall effect, a hallmark of broken time-reversal symmetry and spin-orbit coupling, is frequently observed in magnetically polarized systems. Its realization in non-magnetic systems, however, remains elusive. Here, we report on the observation of anomalous Hall effect in nominally non-magnetic KTaO3. Anomalous Hall effect emerges in reduced KTaO3 and shows an extrinsic to intrinsic crossover. A paramagnetic behavior is observed in reduced samples using first principles calculations and quantitative magnetometry. The observed anomalous Hall effect follows the oxygen vacancy-induced magnetization response, suggesting that the localized magnetic moments of the oxygen vacancies scatter conduction electrons asymmetrically and give rise to anomalous Hall effect. The anomalous Hall conductivity becomes insensitive to scattering rate in the low temperature limit (T<5 K), implying that the Berry curvature of the electrons on the Fermi surface controls the anomalous Hall effect. Our observations describe a detailed picture of many-body interactions, triggering anomalous Hall effect in a non-magnetic system.

cond-mat.mes-hall

Superconducting Phase of $\mathrm{Ti_xO_y}$ Thin Films Grown by Molecular Beam Epitaxy

We investigate the complex relationship between the growth conditions and the structural and transport properties of $\mathrm{Ti_xO_y}$ thin films grown by molecular beam epitaxy. Transport properties ranging from metallicity to superconductivity and insulating states are stabilized by effectively tuning the O/Ti ratio via the Ti flux rate and the O partial pressure, $P_{Ox}$, for films grown on (0001)-$\mathrm{Al_2 O_3}$ substrates at 850$^{\circ}$ C. A cubic $c-\mathrm{TiO_{1\pmδ}}$ buffer layer is formed for low O/Ti ratios while a corundum cr-$\mathrm{Ti_2 O_3}$ layer is formed under higher oxidizing conditions. Metallicity is observed for c-$\mathrm{TiO_{1-δ}}$ buffer layers. The superconducting $\mathrm{γ-Ti_3 O_5}$ Magnéli phase is found to nucleate on a c-$\mathrm{TiO_{1-δ}}$ buffer for intermediate $P_{Ox}$ conditions and an insulator-superconducting transition is observed at 4.5 K (T$_C^{onset}=6 K$) for 85 nm thick films. Strain relaxation of the $\mathrm{γ-Ti_3 O_5}$ occurs with increasing film thickness and correlates with a thickness-dependent increase in T$_C$ observed for $\mathrm{Ti_xO_y}$ thin films.

cond-mat.supr-con

Thickness and temperature dependence of the atomic-scale structure of SrRuO$_3$ thin films

Due to the strong lattice-property relationships which exist in complex oxide epitaxial layers, their electronic and magnetic properties can be modulated by structural distortions induced at the atomic scale. The modification and control can be affected at coherent heterointerfaces by epitaxial strain imposed by the substrate or by structural modifications to accommodate the film-substrate symmetry mismatch. Often these act in conjunction with a strong dependence on the layer thickness, especially for ultrathin layers. Moreover, as a result of these effects, the temperature dependence of the structure may deviate largely from that of the bulk. The temperature-dependent structure of 3 to 44 unit cell thick ferromagnetic SrRuO$_3$ films grown on Nb-doped SrTiO$_3$ substrates are investigated using a combination of high-resolution synchrotron X-ray diffraction and high-resolution electron microscopy. This aims to shed light on the intriguing magnetic and magnetotransport properties of epitaxial SRO layers, subjected to extensive investigations lately. The oxygen octahedral tilts and rotations are found to be strongly dependent on the temperature, the film thickness, and the distance away from the film-substrate interface. As a striking manifestation of the coupling between magnetic order and lattice structure, the Invar effect is observed below the ferromagnetic transition temperature in epitaxial layers as thin as 8 unit cells, similar to bulk ferromagnetic SrRuO$_3$.

cond-mat.mtrl-sci

Coexistence of superconductivity and weak anti-localization at KTaO3 (111) interfaces

The intersection of two-dimensional superconductivity and topologically nontrivial states hosts a wide range of quantum phenomena, including Majorana fermions. Coexistence of topologically nontrivial states and superconductivity in a single material, however, remains elusive. Here, we report on the observation of two-dimensional superconductivity and weak anti-localization at the TiOx/KTaO3(111) interfaces. A remnant, saturating resistance persists below the transition temperature as superconducting puddles fail to reach phase coherence. Signatures of weak anti-localization are observed below the superconducting transition, suggesting the coexistence of superconductivity and weak anti-localization. The superconducting interfaces show roughly one order of magnitude larger weak anti-localization correction, compared to non-superconducting interfaces, alluding to a relatively large coherence length in these interfaces.

cond-mat.supr-con

Interface-driven magnetic anisotropy in relaxed La$_{0.7}$Sr$_{0.3}$CrO$_3$/La$_{0.7}$Sr$_{0.3}$MnO$_3$ heterostructures on MgO

We investigate the structural and magnetic properties of La$_{0.7}$Sr$_{0.3}$CrO$_3$ (LSCO)/La$_{0.7}$Sr$_{0.3}$MnO$_3$(LSMO) heterostructures grown on (001)-oriented MgO by molecular beam epitaxy. Due to the large film-substrate lattice mismatch, strain relaxation is found to occur within the first 2-3 unit cells (uc) of the film as evidenced by reflection high energy electron diffraction and high-resolution synchrotron X-ray reciprocal space mapping. We find that the presence of the LSCO spacer and capping layers leads to ferromagnetism in ultra-thin LSMO layers with thicknesses on the order of 2 uc with the magnetic easy axis oriented in the film plane. Net magnetic moments of 1.4 and 2.4 $μ_B$/Mn are measured for [2 uc LSCO/ 2 uc LSMO] and [2 uc LSCO/ 4 uc LSMO] superlattices, respectively by SQUID magnetometry. The effective magnetic anisotropy of the relaxed [2 uc LSCO/ 4 uc LSMO] heterostructure is found to be an order of magnitude higher than bulk LSMO highlighting the critical role of interfacial magnetic exchange interactions in tuning magnetic anisotropy at complex oxide interfaces.

cond-mat.mtrl-sci

Effect of strain on magnetic and orbital ordering of LaSrCrO$_3$/LaSrMnO$_3$ heterostructures

We investigate the effect of strain and film thickness on the orbital and magnetic properties of LaSrCrO$_3$ (LSCO)/LaSrMnO$_3$ (LSMO) heterostructures using bulk magnetometry, soft X-ray magnetic spectroscopy, first-principles density functional theory, high-resolution electron microscopy and X-ray diffraction. We observe an anti-parallel ordering of the magnetic moments between the ferromagnetic LSMO layers and the LSCO spacers leading to a strain-independent ferromagnetic ground state of the LSCO/LSMO heterostructures for LSMO layers as thin as 2 unit cells. As the LSMO thickness is increased, a net ferromagnetic state is maintained, however, the average magnetic moment per Mn is found to be dependent on the magnitude of the substrate-induced strain. The differences in the magnetic responses are related to preferential occupation of the Mn $x^2-y^2$ (in-plane) d-orbitals for tensile strain and $3z^2-r^2$ (out-of-plane) orbitals under compressive strain leading to competing ferromagnetic and anti-ferromagnetic exchange interactions within the LSMO layers. These results underscore the relative contributions of orbital, structural and spin degree of freedom and their tunability in atomically-thin crystalline complex oxide layers.

cond-mat.mtrl-sci

Control of hidden ground-state order in NdNiO$_3$ superlattices

The combination of charge and spin degrees of freedom with electronic correlations in condensed matter systems leads to a rich array of phenomena, such as magnetism, superconductivity, and novel conduction mechanisms. While such phenomena are observed in bulk materials, a richer array of behaviors becomes possible when these degrees of freedom are controlled in atomically layered heterostructures, where one can constrain dimensionality and impose interfacial boundary conditions. Here, we unlock a host of unique, hidden electronic and magnetic phase transitions in NdNiO$_3$ while approaching the two-dimensional (2D) limit, resulting from the differing influences of dimensional confinement and interfacial coupling. Most notably, we discover a new phase in fully 2D, single layer NdNiO$_3$, in which all signatures of the bulk magnetic and charge ordering are found to vanish. In addition, for quasi two-dimensional layers down to a thickness of two unit cells, bulk-type ordering persists but separates from the onset of insulating behavior in a manner distinct from that found in the bulk or thin film nickelates. Using resonant x-ray spectroscopies, first-principles theory, and model calculations, we propose that the single layer phase suppression results from a new mechanism of interfacial electronic reconstruction based on ionicity differences across the interface, while the phase separation in multi-layer NdNiO$_3$ emerges due to enhanced 2D fluctuations. These findings provide insights into the intertwined mechanisms of charge and spin ordering in strongly correlated systems in reduced dimensions and illustrate the ability to use atomic layering to access hidden phases.

cond-mat.str-el

Interfacial Structure of SrZr$_{x}$Ti$_{1-x}$O$_3$ films on Ge

The interfacial structure of SrZr$_{x}$Ti$_{1-x}$O$_3$ films grown on semiconducting Ge substrates are investigated by synchrotron X-ray diffraction and first-principles density functional theory. By systematically tuning Zr content x, the effects of bonding at the interface and epitaxial strain on the physical structure of the film can be distinguished. The interfacial perovskite layers are found to be polarized as a result of cation-anion ionic displacements perpendicular to the perovskite/semiconductor interface. We find a correlation between the observed buckling and valence band offsets at the SrZr$_{x}$Ti$_{1-x}$O$_3$/Ge interface. The theoretical valence band offsets for the polar structures are in agreement with reported X-ray photoelectron spectroscopy measurements. These results have important implications for the integration of functional oxide materials with established semiconductor based technologies.

cond-mat.mtrl-sci

Atomic layer control of metal-insulator behavior in oxide quantum wells integrated directly on silicon

We present electrical and structural characterization of epitaxial LaTiO3/SrTiO3 quantum wells integrated directly on Si(100). The quantum wells exhibit metallic transport described by Fermi-liquid behavior. Carriers arise from both charge transfer from the LaTiO3 to SrTiO3 and oxygen vacancies in the latter. By reducing the thickness of the quantum wells, an enhancement in carrier-carrier scattering is observed, and insulating transport emerges. Consistent with a Mott-driven transition in bulk rare-earth titanates, the insulating behavior is described by activated transport, and the onset of insulating transport occurs near 1 electron per Ti occupation within the SrTiO3 well. We also discuss the role that structure and gradients in strain may play in enhancing the carrier density. The manipulation of metal-insulator behavior in oxides grown directly on Si opens the pathway to harnessing strongly correlated phenomena in device technologies.

cond-mat.mtrl-sci