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Topological Insulators (TIs) are promising platforms for Quantum Technology due to their topologically protected surface states (TSS). Plasmonic excitations in TIs are especially interesting both as a method of characterisation for TI heterostructures, and as potential routes to couple optical and spin signals in low-loss devices. Since the electrical properties of the TI surface are critical, tuning TI surfaces is a vital step in developing TI structures that can be applied in real world plasmonic devices. Here, we present a study of Bi 2 Se 3 /graphene heterostructures, prepared using a low-cost transfer method that reliably produces mono-layer graphene coatings on Bi 2 Se 3 flakes. Using both Raman spectroscopy and electron energy loss spectroscopy (EELS), we show that the graphene layer redshifts the energy of the π plasmon mode in Bi 2 Se 3 , creating a distinct surface plasmon that differs significantly from the behaviour of a TI-trivial insulator boundary. We demonstrate that this is likely due to band-bending and electron transfer between the TI surface and the graphene layer. Based on these results, we outline how graphene overlayers can be used to create tuneable, stable plasmonic materials based on topological insulators., Competing Interests: Declarations. Competing interests: The authors declare no competing interests., (© 2024. The Author(s).)

5d metals are used in electronics because of their high spin-orbit coupling (SOC) leading to efficient spin-electric conversion. When C 60 is grown on a metal, the electronic structure is altered due to hybridization and charge transfer. In this work, we measure the spin Hall magnetoresistance for Pt/C 60 and Ta/C 60 , finding that they are up to a factor of 6 higher than those for pristine metals, indicating a 20-60% increase in the spin Hall angle. At low fields of 1-30 mT, the presence of C 60 increased the anisotropic magnetoresistance by up to 700%. Our measurements are supported by noncollinear density functional theory calculations, which predict a significant SOC enhancement by C 60 that penetrates through the Pt layer, concomitant with trends in the magnetic moment of transport electrons acquired via SOC and symmetry breaking. The charge transfer and hybridization between the metal and C 60 can be controlled by gating, so our results indicate the possibility of dynamically modifying the SOC of thin metals using molecular layers. This could be exploited in spin-transfer torque memories and pure spin current circuits.

We show that hybrid MnO x /C 60 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 C 60 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., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).)

Carbon-based molecules offer unparalleled potential for THz and optical devices controlled by pure spin currents: a low-dissipation flow of electronic spins with no net charge displacement. However, the research so far has been focused on the electrical conversion of the spin imbalance, where molecular materials are used to mimic their crystalline counterparts. Here, we use spin currents to access the molecular dynamics and optical properties of a fullerene layer. The spin mixing conductance across Py/C 60 interfaces is increased by 10% (5 × 10 18  m -2 ) under optical irradiation. Measurements show up to a 30% higher light absorbance and a factor of 2 larger photoemission during spin pumping. We also observe a 0.15 THz slowdown and a narrowing of the vibrational peaks. The effects are attributed to changes in the non-radiative damping and energy transfer. This opens new research paths in hybrid magneto-molecular optoelectronics, and the optical detection of spin physics in these materials.Carbon-based molecules could prove useful in terahertz and optical devices controlled by pure spin currents. Here, conversely, the authors use spin currents to probe molecular dynamics and enhance the optical response of a fullerene layer, enabling hybrid magneto-molecular optoelectronic devices.

Charge transfer at metallo-molecular interfaces may be used to design multifunctional hybrids with an emergent magnetization that may offer an eco-friendly and tunable alternative to conventional magnets and devices. Here, we investigate the origin of the magnetism arising at these interfaces by using different techniques to probe 3d and 5d metal films such as Sc, Mn, Cu, and Pt in contact with fullerenes and rf-sputtered carbon layers. These systems exhibit small anisotropy and coercivity together with a high Curie point. Low-energy muon spin spectroscopy in Cu and Sc-C 60 multilayers show a quick spin depolarization and oscillations attributed to nonuniform local magnetic fields close to the metallo-carbon interface. The hybridization state of the carbon layers plays a crucial role, and we observe an increased magnetization as sp 3 orbitals are annealed into sp 2 -π graphitic states in sputtered carbon/copper multilayers. X-ray magnetic circular dichroism (XMCD) measurements at the carbon K edge of C 60 layers in contact with Sc films show spin polarization in the lowest unoccupied molecular orbital (LUMO) and higher π*-molecular levels, whereas the dichroism in the σ*-resonances is small or nonexistent. These results support the idea of an interaction mediated via charge transfer from the metal and dz -π hybridization. Thin-film carbon-based magnets may allow for the manipulation of spin ordering at metallic surfaces using electrooptical signals, with potential applications in computing, sensors, and other multifunctional magnetic devices., Competing Interests: The authors declare no conflict of interest.

Only three elements are ferromagnetic at room temperature: the transition metals iron, cobalt and nickel. The Stoner criterion explains why iron is ferromagnetic but manganese, for example, is not, even though both elements have an unfilled 3d shell and are adjacent in the periodic table: according to this criterion, the product of the density of states and the exchange integral must be greater than unity for spontaneous spin ordering to emerge. Here we demonstrate that it is possible to alter the electronic states of non-ferromagnetic materials, such as diamagnetic copper and paramagnetic manganese, to overcome the Stoner criterion and make them ferromagnetic at room temperature. This effect is achieved via interfaces between metallic thin films and C60 molecular layers. The emergent ferromagnetic state exists over several layers of the metal before being quenched at large sample thicknesses by the material's bulk properties. Although the induced magnetization is easily measurable by magnetometry, low-energy muon spin spectroscopy provides insight into its distribution by studying the depolarization process of low-energy muons implanted in the sample. This technique indicates localized spin-ordered states at, and close to, the metal-molecule interface. Density functional theory simulations suggest a mechanism based on magnetic hardening of the metal atoms, owing to electron transfer. This mechanism might allow for the exploitation of molecular coupling to design magnetic metamaterials using abundant, non-toxic components such as organic semiconductors. Charge transfer at molecular interfaces may thus be used to control spin polarization or magnetization, with consequences for the design of devices for electronic, power or computing applications (see, for example, refs 6 and 7).

Nanostructured materials often have properties widely different from bulk, imposed by quantum limits to a physical property of the material. This includes, for example, superparamagnetism and quantized conductance, but original properties such as magnetoresistance in nonmagnetic molecular structures may also emerge. In this Letter, we report on the atomic manipulation of platinum nanocontacts in order to induce magnetoresistance. Platinum is a paramagnetic 5d metal, but atomic chains of this material have been predicted to be magnetically ordered with a large anisotropy. Remarkably, we find that a gas flow stabilizes Pt atomic structures in a break junction experiment, where we observe extraordinary resistance changes over 30,000% in a temperature range up to 77 K. Simulations indicate that this behavior may stem from a previously unknown magnetically ordered, low-energy state in platinum oxide atomic chains. This is supported by measurements in Pt/PtOx superlattices revealing the presence of a ferromagnetic moment. These properties open new paths of research for atomic scale "dirty" magnetic sensors and quantum devices.