RESUMEN
The ability to create atomically perfect, epitaxial heterostructures of correlated complex perovskite oxides using state-of-art thin film deposition techniques has generated new physical phenomena at engineered interfaces. Here we report on the impact of growth kinetics on the magnetic structure and exchange coupling at the interface in heterostructures combining layers of antiferromagnetic La1/3Sr2/3FeO3 (LSFO) and ferromagnetic La2/3Sr1/3MnO3 (LSMO) on (0 0 1)-oriented SrTiO3 (STO) substrates. Two growth orders are investigated, (a) LSMO/LSFO/STO(0 0 1) and (b) LSFO/LSMO/STO(0 0 1), where the LSFO layer is grown by molecular beam epitaxy and the LSMO layer by high oxygen pressure sputtering. The interface has been investigated using electron microscopy and polarized neutron reflectometry. Interdiffusion over seven monolayers is observed in LSMO/LSFO (a) with an almost 50% reduction in magnetization at the interface and showing no exchange coupling. However, the exchange bias effect ([Formula: see text] mT at 10 K) could be realized when the interface is atomically sharp, as in LSFO/LSMO (b). Our study therefore reveals that, even for well ordered and lattice-matched structures, the kinetics involved in the growth processes drastically influences the interface quality with a strong correlation to the magnetic properties.
RESUMEN
Nondiffusive phonon thermal transport, extensively observed in nanostructures, has largely been attributed to classical size effects, ignoring the wave nature of phonons. We report localization behavior in phonon heat conduction due to multiple scattering and interference events of broadband phonons, by measuring the thermal conductivities of GaAs/AlAs superlattices with ErAs nanodots randomly distributed at the interfaces. With an increasing number of superlattice periods, the measured thermal conductivities near room temperature increased and eventually saturated, indicating a transition from ballistic to diffusive transport. In contrast, at cryogenic temperatures the thermal conductivities first increased but then decreased, signaling phonon wave localization, as supported by atomistic GreenÈs function simulations. The discovery of phonon localization suggests a new path forward for engineering phonon thermal transport.
RESUMEN
Charge storage and trapping properties of polymer dielectrics govern the charge densities of adjacent semiconductors and greatly influence the on-off switching voltage (threshold voltage, V t h ) of organic field-effect transistors (OFETs) when the polymers are used as gate insulators. Intentional charging of polymer dielectrics in OFETs can change V t h and affect the bias stress. We describe a chemical design and fabrication protocol to construct multilayer-stack dielectrics for pentacene-based OFETs using different polystyrene (PS)-based polymers in each layer, with oxidizable N,N-bis(4-methoxyphenyl)anilino (TPAOMe)-substituted styrene copolymers in arbitrary vertical positions in the stacks. Thermal, byproduct-free cross-linking of benzocyclobutene subunits provides integrity to the multilayer structure by preventing dissolution of the previous deposited layer. Neutron reflectivity data verified the multilayer morphology. We compared the V t h shift before and after charging the stacks by application of ±100 V across 0.5-1 µm total film thicknesses. Bias stress was the dominant effect in bilayer devices with a TPAOMe layer in contact with the pentacene, indicated by the direction of V t h shift associated with either polarity of external electric field. In structures with no TPAOMe subunit in contact with the pentacene, when charging with -100 V on top of the source and drain electrodes, electron injection from pentacene to dielectric was the major charging mechanism, again consistent with the bias stress direction. When charging with +100 V, bilayer devices without TPAOMe showed little change in V t h , suggesting there was no bias stress effect or charge injection in these devices for this charging polarity. For the bilayer devices with the TPAOMe layer in the bottom, and the trilayer devices with TPOMe in the middle, when +100 V was applied, the V t h shifts were opposite those expected from bias stress. Dipole formation or partial ionization of chargeable groups at the interface between the dielectric layers are likely polarization mechanisms in these cases. A simple analytical model levelports the plausibility of these mechanisms. This work provides examples of both stabilization and shifting of V t h , and therefore controlling charge carrier density, in semiconductors overlying the dielectric multilayers.
RESUMEN
Modulation and δ-doping strategies, in which atomically thin layers of charged dopants are precisely deposited within a heterostructure, have played enabling roles in the discovery of new physical behavior in electronic materials. Here, we demonstrate a purely structural "δ-doping" strategy in complex oxide heterostructures, in which atomically thin manganite layers are inserted into an isovalent manganite host, thereby modifying the local rotations of corner-connected MnO_{6} octahedra. Combining scanning transmission electron microscopy, polarized neutron reflectometry, and density functional theory, we reveal how local magnetic exchange interactions are enhanced within the spatially confined regions of suppressed octahedral rotations. The combined experimental and theoretical results illustrate the potential to utilize noncharge-based approaches to "doping" in order to enhance or suppress functional properties within spatially confined regions of oxide heterostructures.
RESUMEN
Here we present polarized neutron reflectometry measurements exploring thin film heterostructures composed of a strongly correlated Mott state, GdTiO_{3}, embedded with SrTiO_{3} quantum wells. Our results reveal that the net ferromagnetism inherent to the Mott GdTiO_{3} matrix propagates into the nominally nonmagnetic SrTiO_{3} quantum wells and tracks the magnetic order parameter of the host Mott insulating matrix. Beyond a well thickness of 5 SrO layers, the magnetic moment within the wells is dramatically suppressed, suggesting that quenched well magnetism comprises the likely origin of quantum critical magnetotransport in this thin film architecture. Our data demonstrate that the interplay between proximate exchange fields and polarity-induced carrier densities can stabilize extended magnetic states within SrTiO_{3} quantum wells.
RESUMEN
The emergence of complex new ground states at interfaces has been identified as one of the most promising routes to highly tunable nanoscale materials. Despite recent progress, isolating and controlling the underlying mechanisms behind these emergent properties remains among the most challenging materials physics problems to date. In particular, generating ferromagnetism localized at the interface of two nonferromagnetic materials is of fundamental and technological interest. Moreover, the ability to turn the ferromagnetism on and off would shed light on the origin of such emergent phenomena and is promising for spintronic applications. We demonstrate that ferromagnetism confined within one unit cell at the interface of CaRuO3 and CaMnO3 can be switched on and off by changing the symmetry of the oxygen octahedra connectivity at the boundary. Interfaces that are symmetry-matched across the boundary exhibit interfacial CaMnO3 ferromagnetism while the ferromagnetism at symmetry-mismatched interfaces is suppressed. We attribute the suppression of ferromagnetic order to a reduction in charge transfer at symmetry-mismatched interfaces, where frustrated bonding weakens the orbital overlap. Thus, interfacial symmetry is a new route to control emergent ferromagnetism in materials such as CaMnO3 that exhibit antiferromagnetism in bulk form.
RESUMEN
Electric field control of magnetism provides a promising route towards ultralow power information storage and sensor technologies. The effects of magneto-ionic motion have been prominently featured in the modification of interface characteristics. Here, we demonstrate magnetoelectric coupling moderated by voltage-driven oxygen migration beyond the interface in relatively thick AlOx/GdOx/Co(15 nm) films. Oxygen migration and Co magnetization are quantitatively mapped with polarized neutron reflectometry under electro-thermal conditioning. The depth-resolved profiles uniquely identify interfacial and bulk behaviours and a semi-reversible control of the magnetization. Magnetometry measurements suggest changes in the microstructure which disrupt long-range ferromagnetic ordering, resulting in an additional magnetically soft phase. X-ray spectroscopy confirms changes in the Co oxidation state, but not in the Gd, suggesting that the GdOx transmits oxygen but does not source or sink it. These results together provide crucial insight into controlling magnetism via magneto-ionic motion, both at interfaces and throughout the bulk of the films.
RESUMEN
GS-9857, an inhibitor of the hepatitis C virus (HCV) nonstructural protein (NS) 3/4A, demonstrates potent activity against HCV genotypes 1-6 and improved coverage against commonly encountered NS3 resistance-associated variants (RAVs). In this study, the safety, tolerability, antiviral activity and pharmacokinetics (PK) of GS-9857 were evaluated in patients with chronic HCV genotype 1-4 infection. Patients with genotype 1-4 infection received placebo or once-daily GS-9857 at doses ranging from 50 to 300 mg for 3 days under fasting conditions. GS-9857 was well tolerated; all reported adverse events (AEs) were mild or moderate in severity. Diarrhoea and headache were the most commonly reported AEs. Grade 3 or 4 laboratory abnormalities were observed in 17% of patients receiving GS-9857; there were no Grade 3 or 4 abnormalities in alanine aminotransferase, aspartate aminotransferase or alkaline phosphatase levels. GS-9857 demonstrated potent antiviral activity in patients with chronic HCV infection, achieving mean and median maximum reductions in HCV RNA of ≥3 log10 IU/mL following administration of a 100-mg dose in patients with HCV genotype 1a, 1b, 2, 3 or 4 infection. The antiviral activity of GS-9857 was unaffected by the presence of pretreatment NS3 RAVs. In patients with genotype 1-4 infection, GS-9857 exhibited linear PK and was associated with a median half-life of 29-42 h, supporting once-daily dosing. Thus, the tolerability, efficacy and pharmacokinetic profile of GS-9857 support its further evaluation for treatment of patients with chronic HCV infection.
Asunto(s)
Antivirales/administración & dosificación , Genotipo , Hepacivirus/clasificación , Hepacivirus/genética , Hepatitis C Crónica/tratamiento farmacológico , Hepatitis C Crónica/virología , Compuestos Macrocíclicos/administración & dosificación , Sulfonamidas/administración & dosificación , Adolescente , Adulto , Anciano , Ácidos Aminoisobutíricos , Antivirales/efectos adversos , Antivirales/farmacocinética , Antivirales/farmacología , Ciclopropanos , Método Doble Ciego , Efectos Colaterales y Reacciones Adversas Relacionados con Medicamentos/epidemiología , Efectos Colaterales y Reacciones Adversas Relacionados con Medicamentos/patología , Femenino , Hepacivirus/aislamiento & purificación , Humanos , Lactamas Macrocíclicas , Leucina/análogos & derivados , Compuestos Macrocíclicos/efectos adversos , Compuestos Macrocíclicos/farmacocinética , Compuestos Macrocíclicos/farmacología , Masculino , Persona de Mediana Edad , Placebos/administración & dosificación , Prolina/análogos & derivados , Quinoxalinas , Sulfonamidas/efectos adversos , Sulfonamidas/farmacocinética , Sulfonamidas/farmacología , Resultado del Tratamiento , Carga Viral , Adulto JovenRESUMEN
Ionic transport in metal/oxide heterostructures offers a highly effective means to tailor material properties via modification of the interfacial characteristics. However, direct observation of ionic motion under buried interfaces and demonstration of its correlation with physical properties has been challenging. Using the strong oxygen affinity of gadolinium, we design a model system of GdxFe1-x/NiCoO bilayer films, where the oxygen migration is observed and manifested in a controlled positive exchange bias over a relatively small cooling field range. The exchange bias characteristics are shown to be the result of an interfacial layer of elemental nickel and cobalt, a few nanometres in thickness, whose moments are larger than expected from uncompensated NiCoO moments. This interface layer is attributed to a redox-driven oxygen migration from NiCoO to the gadolinium, during growth or soon after. These results demonstrate an effective path to tailoring the interfacial characteristics and interlayer exchange coupling in metal/oxide heterostructures.
RESUMEN
A combination of experiments and numerical modeling was used to study the spatial evolution of the ferromagnetic phase transition in a thin film engineered to have a smooth gradient in exchange strength. Mean-field simulations predict, and experiments confirm, that a 100 nm Ni_{x}Cu_{1-x} alloy film with Ni concentration that varies by 9% as a function of depth behaves predominantly as if composed of a continuum of uncoupled ferromagnetic layers with continuously varying Curie temperatures. A mobile boundary separating ordered and disordered regions emerges as the temperature is increased. We demonstrate continuous control of the boundary position with temperature, and reversible control of the magnetization on both sides of the boundary with the magnetic field.
RESUMEN
New mechanisms for achieving direct electric field control of ferromagnetism are highly desirable in the development of functional magnetic interfaces. To that end, we have probed the electric field dependence of the emergent ferromagnetic layer at CaRuO_{3}/CaMnO_{3} interfaces in bilayers fabricated on SrTiO_{3}. Using polarized neutron reflectometry, we are able to detect the ferromagnetic signal arising from a single atomic monolayer of CaMnO_{3}, manifested as a spin asymmetry in the reflectivity. We find that the application of an electric field of 600 kV/m across the bilayer induces a significant increase in this spin asymmetry. Modeling of the reflectivity suggests that this increase corresponds to a transition from canted antiferromagnetism to full ferromagnetic alignment of the Mn^{4+} ions at the interface. This increase from 1 µ_{B} to 2.5-3.0 µ_{B} per Mn is indicative of a strong magnetoelectric coupling effect, and such direct electric field control of the magnetization at an interface has significant potential for spintronic applications.
RESUMEN
We investigate structural coupling of the MnO6 octahedra across a film/substrate interface and the resultant changes of the physical properties of ultrathin La2/3Sr1/3MnO3 (LSMO) films. In order to isolate the effect of interfacial MnO6 octahedral behavior from that of epitaxial strain, LSMO films are grown on substrates with different symmetry and similar lattice parameters. Ultrathin LSMO films show an increased magnetization and electrical conductivity on cubic (LaAlO3)0.3(Sr2AlTaO6)0.7 (LSAT) compared to those grown on orthorhombic NdGaO3 (NGO) substrates, an effect that subsides as the thickness of the films is increased. This study demonstrates that interfacial structural coupling can play a critical role in the functional properties of oxide heterostructures.
RESUMEN
We observe interfacial ferromagnetism in superlattices of the paramagnetic metal LaNiO3 and the antiferromagnetic insulator CaMnO3. LaNiO3 exhibits a thickness dependent metal-insulator transition and we find the emergence of ferromagnetism to be coincident with the conducting state of LaNiO3. That is, only superlattices in which the LaNiO3 layers are metallic exhibit ferromagnetism. Using several magnetic probes, we have determined that the ferromagnetism arises in a single unit cell of CaMnO3 at the interface. Together these results suggest that ferromagnetism can be attributed to a double exchange interaction among Mn ions mediated by the adjacent itinerant metal.
RESUMEN
We have found ferromagnetism in epitaxially grown superlattices of CaRuO(3)/CaMnO(3) that arises in one unit cell at the interface. Scanning transmission electron microscopy and electron energy loss spectroscopy indicate that the difference in magnitude of the Mn valence states between the center of the CaMnO(3) layer and the interface region is consistent with double exchange interaction among the Mn ions at the interface. Polarized neutron reflectivity and the CaMnO(3) thickness dependence of the exchange bias field together indicate that the interfacial ferromagnetism is only limited to one unit cell of CaMnO(3) at each interface. The interfacial moment alternates between the 1 µ(B)/interface Mn ion for even CaMnO(3) layers and the 0.5 µ(B)/interface Mn ion for odd CaMnO(3) layers. This modulation, combined with the exchange bias, suggests the presence of a modulating interlayer coupling between neighboring ferromagnetic interfaces via the antiferromagnetic CaMnO(3) layers.
RESUMEN
We have observed long-range spin-triplet supercurrents in Josephson junctions containing ferromagnetic (F) materials, which are generated by noncollinear magnetizations between a central Co/Ru/Co synthetic antiferromagnet and two outer thin F layers. Here we show that the spin-triplet supercurrent is enhanced up to 20 times after our samples are subject to a large in-plane field. This occurs because the synthetic antiferromagnet undergoes a "spin-flop" transition, whereby the two Co layer magnetizations end up nearly perpendicular to the magnetizations of the two thin F layers. We report direct experimental evidence for the spin-flop transition from scanning electron microscopy with polarization analysis and from spin-polarized neutron reflectometry. These results represent a first step toward experimental control of spin-triplet supercurrents.
RESUMEN
We demonstrate that delta doping can be used to create a dimensionally confined region of metallic ferromagnetism in an antiferromagnetic (AFM) manganite host, without introducing any explicit disorder due to dopants or frustration of spins. Theoretical consideration of these additional carriers shows that they cause a local enhancement of ferromagnetic double exchange with respect to AFM superexchange, resulting in local canting of the AFM spins. This leads to a highly modulated magnetization, as measured by polarized neutron reflectometry. The spatial modulation of the canting is related to the spreading of charge from the doped layer and establishes a fundamental length scale for charge transfer, transformation of orbital occupancy, and magnetic order in these manganites. Furthermore, we confirm the existence of the canted, AFM state as was predicted by de Gennes [Phys. Rev. 118, 141 (1960)] but had remained elusive.
RESUMEN
Due to low charge carrier mobilities in polymer-based solar cells, device performance is dictated by the nanoscale morphology of the active layer components. However, their morphological details are notoriously difficult to distinguish due to the low electron contrast difference between the components. Phase-sensitive neutron reflectivity (PSNR) is uniquely suited to characterize these systems due to the large, natural scattering length density difference between two common device materials, poly(3-hexylthiophene) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM). Using PSNR we find a high concentration of PCBM at the substrate and near but not at the air interface. Herein we discuss the method of applying PSNR to polymer-based solar cells, the results obtained, and an evaluation of its effectiveness.
RESUMEN
We report the antiferromagnetic (AFM) interlayer exchange coupling between Ga0.97Mn0.03As ferromagnetic semiconductor layers separated by Be-doped GaAs spacers. Polarized neutron reflectivity reveals a characteristic splitting at the wave vector corresponding to twice the multilayer period, indicating that the coupling between the ferromagnetic layers is AFM. When the applied field is increased to above the saturation field, this AFM coupling is suppressed. This behavior is not observed when the spacers are undoped, suggesting that the observed AFM coupling is mediated by doped charge carriers.
RESUMEN
Spin echo scattering angle measurement (SESAME) is a sensitive interference technique for measuring neutron diffraction. The method uses waveplates or birefringent prisms to produce a phase separation (the Larmor phase) between the "up" and "down" spin components of a neutron wavefunction that is initially prepared in a state that is a linear combination of in-phase up and down components. For neutrons, uniformly birefringent optical elements can be constructed from closed solenoids with appropriately shaped cross sections. Such elements are inconvenient in practice, however, both because of the precision they demand in the control of magnetic fields outside the elements and because of the amount of material required in the neutron beam. In this paper, we explore a different option in which triangular-cross-section solenoids used to create magnetic fields for SESAME have gaps in one face, allowing the lines of magnetic flux to "leak out" of the solenoid. Although the resulting field inhomogeneity produces aberrations in the Larmor phase, the symmetry of the solenoid gaps causes the aberrations produced by neighboring pairs of triangular solenoids to cancel to a significant extent. The overall symmetry of the SESAME apparatus leads to further cancellations of aberrations, providing an architecture that is easy to construct and robust in performance.
RESUMEN
Numerous reports have documented drug interactions with grapefruit juice (GFJ) that occur via inhibition of CYP3A enzymes. As reported by Glaeser et al. in the March 2007 issue of this journal, there is increasing recognition that GFJ may also affect the activity of influx (e.g., OATPs) and efflux (e.g., P-glycoprotein) transporters. This commentary focuses on these interactions between GFJ and drug transporters.