Combining optical and magnetic functionalities into memristors is an attractive option to expand applications into image recognition, information storage, and low power processing. Here, we have fabricated ferromagnetic-fullerene-manganese oxide structures that display a hysteretic, nonlinear I-V characteristic and a photovoltaic effect with a photocurrent dependent on the relative alignment of the magnetization and the light polarization vector. Reversible, voltage-induced oxygen migration from manganese oxide into the molecular layer reduces the resistivity of the device by several orders of magnitude, eliminates the nonlinear transport, and quenches the photovoltaic response, giving rise to an optically sensitive memristor where the photocurrent is dependent on both the electrical and magnetic history of the device. Density functional theory calculations attribute the origin of these effects to changes in the electronic structure at the Fermi level and a reduction of the interface dipole upon ionic migration. These results open research pathways towards single-molecule scale memristive memories with optical excitation, electrical readout and magnetic sensing functionalities.

Synthetic antiferromagnetic structures can exhibit the advantages of high velocity similarly to antiferromagnets with the additional benefit of being imaged and read-out through techniques applied to ferromagnets. Here, we explore the potential and limits of synthetic antiferromagnets to uncover ways to harness their valuable properties for applications. Two synthetic antiferromagnetic systems have been engineered and systematically investigated to provide an informed basis for creating devices with maximum potential for data storage, logic devices, and skyrmion racetrack memories. The two systems considered are (system 1) CoB/Ir/Pt of N repetitions with Ir inducing the negative coupling between the ferromagnetic layers and (system 2) two ferromagnetically coupled multilayers of CoB/Ir/Pt, coupled together antiferromagnetically with an Ir layer. From the hysteresis, it is found that system 1 shows stable antiferromagnetic interlayer exchange coupling between each magnetic layer up to N = 7. Using Kerr imaging, the two ferromagnetic multilayers in system 2 are shown to undergo separate maze-like switches during hysteresis. Both systems are also studied as a function of temperature and show different behaviors. Micromagnetic simulations predict that in both systems the skyrmion Hall angle is suppressed with the skyrmion velocity five times higher in system 1 than system 2.

The accurate measurement of the Dzyaloshinskii-Moriya interaction (DMI) in ultrathin ferromagnetic/heavy metal heterostructures was recently shown to require extreme experimental care. In this presentation the current state-of-the-art of measuring interfacial DMI is reviewed, and two of the most popular techniques - non-reciprocity of thermally activated magnetostatic spin wave dispersion and asymmetric bubble domain expansion - are discussed for their reliability and applicability. Furthermore, the large discrepancies observed recently between the two techniques are analyzed, and possible origins are discussed. The presentation aims to achieve a deeper comprehension of the reasons behind the discrepancies and to assess the applicability of various techniques to different heterostructures.

The long-term future of information storage requires the use of sustainable nanomaterials in architectures operating at high frequencies. Interfaces can play a key role in this pursuit via emergent functionalities that break out from conventional operation methods. Here, spin-filtering effects and photocurrents are combined at metal-molecular-oxide junctions in a hybrid magneto-capacitive memory. Light exposure of metal-fullerene-metal oxide devices results in spin-polarized charge trapping and the formation of a magnetic interface. Because the magnetism is generated by a photocurrent, the writing time is determined by exciton formation and splitting, electron hopping, and spin-dependent trapping. Transient absorption spectroscopy measurements show changes in the electronic states as a function of the magnetic history of the device within picoseconds of the optical pumping. The stored information is read using time-resolved scanning magneto optic Kerr effect measurements during microwave irradiation. The emergence of a magnetic interface in the picosecond timescale opens new paths of research to design hybrid magneto-optic structures operating at high frequencies for sensing, computing, and information storage.

We show that magnetic skyrmions can be stabilised at room temperature in continuous [Ir/Co/Pt]5 multilayers on SiO2/Si substrates without the prior application of electric current or magnetic field. While decreasing the Co thickness, a transition of the magnetic domain patterns from worm-like state to separated stripes is observed. The skyrmions are clearly imaged in both states using magnetic force microscopy. The density of skyrmions can be significantly enhanced after applying the “in-plane field procedure”. Our results provide means to manipulate magnetic skyrmion density, further allowing for the optimised engineering of skyrmion-based devices.

RF-sputtered amorphous carbon (a-C) offers a simple and cheap pathway to tune the magnetic properties of transition metal thin films for magnetic memories and different spintronic applications. This paper describes changes in the magnetic properties of iron thin films with a-C overlayers. In as-deposited samples, hybridisation and intermixing at the Fe/a-C interface leads to magnetic softening (Liu et al., 2006) [1], with a reduction in the coercive field (H-c) up to a factor of five for Fe/a-C/Fe trilayers, and a 10-30% lower saturation magnetization as a function of the metal film thickness. After annealing at 500 ?, inter-diffusion and graphitization of the carbon layer results in up to a factor five increased coercivity due to increased pinning as shown via Kerr microscopy. Therefore, RF-sputtered carbon overlayers and post-processing can tune the anisotropy and domain configuration of metallic thin films in a synthesis methodology that is simple, cheap and sustainable.

Different models have been used to evaluate the interfacial Dzyaloshinskii-Moriya interaction (DMI) from the asymmetric bubble expansion method using magneto-optics. Here, we investigate the most promising candidates over a range of different magnetic multilayers with perpendicular anisotropy. Models based on the standard creep hypothesis are not able to reproduce the domain wall (DW) velocity profile when the DW roughness is high. Our results demonstrate that the DW roughness and the interface roughness of the sample layers are correlated. Furthermore, we give guidance on how to obtain reliable results for the DMI value with this popular method. A comparison of the results with Brillouin light scattering (BLS) measurements on the same samples shows that the BLS approach often results in higher measured values of DMI.

Muonium is a combination of first- and second-generation matter formed by the electrostatic interaction between an electron and an antimuon (mu(+)). Although a well-known physical system, their ability to form collective excitations in molecules had not been observed. Here, we give evidence for the detection of a muonium state that propagates in a molecular semiconductor lattice via thermally activated dynamics: a muonium polaron. By measuring the temperature dependence of the depolarization of the muonium state in C-60, we observe a thermal narrowing of the hyperfine distribution that we attribute to the dynamics of the muonium between molecular sites. As a result of the time scale for muonium decay, the energies involved, charge and spin selectivity, this quasiparticle is a widely applicable experimental tool. It is an excellent probe of emerging electronic, dynamic, and magnetic states at interfaces and in low dimensional systems, where direct spatial probing is an experimental challenge owing to the buried interface, nanoscale elements providing the functionality localization and small magnitude of the effects.

Heavy metals are key to spintronics because of their high spin-orbit coupling (SOC) leading to efficient spin conversion and strong magnetic interactions. When C60 is deposited on Pt, the molecular interface is metallised and the spin Hall angle in YIG/Pt increased, leading to an enhancement of up to 600% in the spin Hall magnetoresistance and 700% for the anisotropic magnetoresistance. This correlates with Density Functional Theory simulations showing changes of 0.46 eV/C60 in the SOC of Pt. This effect opens the possibility of gating the molecular hybridisation and SOC of metals.

Combining magnetic and superconducting functionalities enables lower energy spin transfer and magnetic switching in quantum computing and information storage, owing to the dissipationless nature of quasi-particle mediated supercurrents. Here, we put forward a system where emergent spin-ordering and diffusion of Cooper pairs are achieved at a non-intrinsically magnetic nor superconducting metallo-molecular interface. Electron transport, magnetometry and low-energy muon spin rotation are used to probe time-reversal symmetry breaking in these structures. By comparing the Meissner expulsion in a system including a Cu/C 60 spin-converter interface to one without, we observe a paramagnetic contribution that can be explained due to the conversion of spin-singlet Cooper pair states into odd-frequency triplet states. These results demonstrate the potential of metallo-molecular interfaces to achieve singlet to triplet Cooper pair conversion, a capability not present in either metal or molecule separately that could be used in the generation and controlled diffusion of spin polarised dissipationless currents.

We report on the electrical transport properties of Nb based Josephson junctions with Pt/Co[Formula: see text]B[Formula: see text]/Pt ferromagnetic barriers. The barriers exhibit perpendicular magnetic anisotropy, which has the main advantage for potential applications over magnetisation in-plane systems of not affecting the Fraunhofer response of the junction. In addition, we report that there is no magnetic dead layer at the Pt/Co[Formula: see text]B[Formula: see text] interfaces, allowing us to study barriers with ultra-thin Co[Formula: see text]B[Formula: see text]. In the junctions, we observe that the magnitude of the critical current oscillates with increasing thickness of the Co[Formula: see text]B[Formula: see text] strong ferromagnetic alloy layer. The oscillations are attributed to the ground state phase difference across the junctions being modified from zero to [Formula: see text]. The multiple oscillations in the thickness range [Formula: see text] nm suggests that we have access to the first zero-[Formula: see text] and [Formula: see text]-zero phase transitions. Our results fuel the development of low-temperature memory devices based on ferromagnetic Josephson junctions.

The magnetisation data presented in the main text were acquired in a Quantum Design MPMS3 magnetometer. The magnetometer returns measurements of the total magnetic moment of the sample in emu. The total magnetic moment of the sample contains the contributions due to the substrate, thin film, and any spurious signal such as those described by Garcia et al. [1] . Careful sample handing was used to minimise spurious contributions to the total moment. The linear diamagnetic background due to the substrate was subtracted from the total measured moment. We report the data after substrate subtraction as the area normalised magnetic moment (moment/area) in emu/cm by measuring the area of the sample. For a uniform slab of ferromagnetic material, the volume magnetisation (M) can be determined by dividing the saturation moment/area by the thickness of the ferromagnetic layer. M can also be reliably determined by measuring several samples of varying thickness. If one plots moment/area versus thickness (d), as per Figure S1, then the fitted gradient will be M , moment/area = Md. (S1)

A method for detecting dc spin current propagation through an epitaxial antiferromagnetic (AFM) NiO layer is presented. Spin current is generated by spin pumping from an adjoining ferromagnetic (FM) layer and detected in a non-magnetic metallic layer by the inverse spin Hall effect. Comparison is made with a YIG/Pt bilayer, where only the Pt layer is electrically conducting, but for which spin Hall magnetoresistance makes an additional contribution to the measured signal. The signal obtained from the multilayered stack containing the AFM NiO layer is found to contain additional contributions due to anisotropic magnetoresistance. By exciting the sample with out-of-plane rf magnetic field and making measurements with a static field applied at different orientations within the plane of the sample, a signal associated with the dc spin current may be identified.

Abstract We report on the electrical transport properties of Nb based Josephson junctions with Pt/Co $$_{68}$$ 68 B $$_{32}$$ 32 /Pt ferromagnetic barriers. The barriers exhibit perpendicular magnetic anisotropy, which has the main advantage for potential applications over magnetisation in-plane systems of not affecting the Fraunhofer response of the junction. In addition, we report that there is no magnetic dead layer at the Pt/Co $$_{68}$$ 68 B $$_{32}$$ 32 interfaces, allowing us to study barriers with ultra-thin Co $$_{68}$$ 68 B $$_{32}$$ 32 . In the junctions, we observe that the magnitude of the critical current oscillates with increasing thickness of the Co $$_{68}$$ 68 B $$_{32}$$ 32 strong ferromagnetic alloy layer. The oscillations are attributed to the ground state phase difference across the junctions being modified from zero to $$\pi $$ π . The multiple oscillations in the thickness range $$0.2~\leqslant ~d_\text {CoB}~\leqslant ~1.4$$ 0.2 ⩽ d CoB ⩽ 1.4 nm suggests that we have access to the first zero- $$\pi $$ π and $$\pi $$ π -zero phase transitions. Our results fuel the development of low-temperature memory devices based on ferromagnetic Josephson junctions.

Using scanning thermal microscopy, we have mapped the spatial distribution of temperatures in an operating nanoscale device formed from a magnetic injector, an Ag connecting wire, and a magnetic detector. An analytical model explained the thermal diffusion over the measured temperature range (2-300 K) and injector-detector separation (400-3000 nm). The characteristic diffusion lengths of the Peltier and Joule heat differ remarkably below 60 K, a fact that can be explained by the onset of ballistic phonon heat transfer in the substrate.

We show that hybrid MnOx/C60 heterojunctions can be used to design a storage device for spin-polarized charge: a spin capacitor. Hybridization at the carbon-metal oxide interface leads to spin-polarized charge trapping after an applied voltage or photocurrent. Strong electronic structure changes, including a 1-eV energy shift and spin polarization in the C60 lowest unoccupied molecular orbital, are then revealed by x-ray absorption spectroscopy, in agreement with density functional theory simulations. Muon spin spectroscopy measurements give further independent evidence of local spin ordering and magnetic moments optically/electronically stored at the heterojunctions. These spin-polarized states dissipate when shorting the electrodes. The spin storage decay time is controlled by magnetic ordering at the interface, leading to coherence times of seconds to hours even at room temperature.

High coercivity magnets are an important resource for renewable energy, electric vehicles and memory technologies. Most hard magnetic materials incorporate rare-earths such as neodymium and samarium, but the concerns about the environmental impact and supply stability of these materials is prompting research into alternatives. Here, we present a hybrid bilayer of cobalt and the nano-carbon molecule C 60 which exhibits significantly enhanced coercivity with minimal reduction in magnetisation. We demonstrate how this anisotropy enhancing effect cannot be described by ex-isting models of molecule-metal magnetic interfaces. We outline a new form of magnetic anisotropy, arising from asymmetric magneto-electric coupling in the metal-molecule interface. Because this phenomenon arises from π - d hybrid orbitals, we propose calling this effect π - anisotropy. While the critical temperature of this effect is currently limited by the rotational degree of freedom of the chosen molecule, C 60 , we describe how surface functionalisation would allow for the design of room-temperature, carbon based hard magnetic films.

We demonstrate a Josephson junction with a weak link containing two ferromagnets with perpendicular magnetic anisotropy and independent switching fields in which the critical current can be set by the mutual orientation of the two layers. Such pseudospin-valve Josephson junctions are a candidate cryogenic memory in an all superconducting computational scheme. Here, we use Pt/Co/Pt/CoB/Pt as the weak link of the junction with d(Co) = 0:6nm; d(CoB) = 0:3 nm, and d(Pt) = 5nm and obtain a 60% change in the critical current for the two magnetization configurations of the pseudospin-valve. Ferromagnets with perpendicular magnetic anisotropy have advantages over magnetization in-plane systems, which have been exclusively considered at this point, as, in principle, the magnetization and magnetic switching of layers in the junction should not affect the in-plane magnetic flux. Published under license by AIP Publishing.

High coercivity magnets are an important resource for renewable energy, electric vehicles and memory technologies. Most hard magnetic materials incorporate rare-earths such as neodymium and samarium, but the concerns about the environmental impact and supply stability of these materials is prompting research into alternatives. Here, we present a hybrid bilayer of cobalt and the nano-carbon molecule C60 which exhibits significantly enhanced coercivity with minimal reduction in magnetisation. We demonstrate how this anisotropy enhancing effect cannot be described by existing models of molecule-metal magnetic interfaces. We outline a new form of magnetic anisotropy, arising from asymmetric magneto-electric coupling in the metal-molecule interface. Because this phenomenon arises from pi-d hybrid orbitals, we propose calling this effect pi-anisotropy. While the critical temperature of this effect is currently limited by the rotational degree of freedom of the chosen molecule, C60, we describe how surface functionalisation would allow for the design of room-temperature, carbon based hard magnetic films.