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2D materials offer the ability to expose their electronic structure to manipulations by a proximity effect. This could be harnessed to craft properties of 2D interfaces and van der Waals heterostructures in devices and quantum materials. We explore the possibility to create an artificial spin polarized electrode from graphene through proximity interaction with a ferromagnetic insulator to be used in a magnetic tunnel junction (MTJ). Ferromagnetic insulator/graphene artificial electrodes were fabricated and integrated in MTJs based on spin analyzers. Evidence of the emergence of spin polarization in proximitized graphene layers was observed through the occurrence of tunnel magnetoresistance. We deduced a spin dependent splitting of graphene's Dirac band structure (∼15 meV) induced by the proximity effect, potentially leading to full spin polarization and opening the way to gating. The extracted spin signals illustrate the potential of 2D quantum materials based on proximity effects to craft spintronics functionalities, from vertical MTJs memory cells to logic circuits., This work has received funding from the European Union’s H2020 Future and Emerging Technologies “Graphene Flagship” (Grant Core3 No. 881603), “SINFONIA” (No. 881603) projects and a Grant Agreement Marie Skłodowska Curie “ITN Spinograph” (No. 697904), as well as from EPSRC (EP/P005152/1, EP/K016636/1). This research is supported by a public grant overseen by the French National Research Agency (ANR) as part of the “Investissements d’Avenir” program Labex NanoSaclay (ANR-10-LABX-0035), as well as grants STEM2D (ANR-19-CE24-0015), MIXES (ANR-19-CE09-0028), and by the Flag-ERA JTC 2019 project “SOGraphMEM” (ANR-19-GRFI-0001-07). This work has also received fundings from the “Spanish ministry of Science and Innovation” through “Severo Ochoa” (CEX2019-000917-S) and “OXISOT” (PID2021-128410OB-I00)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).

Despite the high potential of endohedral metallofullerenes (EMFs) for application in biology, medicine and molecular electronics, and recent efforts in EMF synthesis, the variety of EMFs accessible by conventional synthetic methods remains limited and does not include, for example, EMFs of late transition metals. We propose a method in which EMF formation is initiated by electron irradiation in aberration-corrected high-resolution transmission electron spectroscopy (AC-HRTEM) of a metal cluster surrounded by amorphous carbon inside a carbon nanotube serving as a nanoreactor and apply this method for synthesis of nickel EMFs. The use of AC-HRTEM makes it possible not only to synthesize new, previously unattainable nanoobjects but also to study in situ the mechanism of structural transformations. Molecular dynamics simulations using the state-of-the-art approach for modeling the effect of electron irradiation are performed to rationalize the experimental observations and to link the observed processes with conditions of bulk EMF synthesis., A.S.S., I.V.L., A.A.K., and A.M.P. acknowledge the Russian Foundation of Basic Research (14-02-00739-a). I.V.L. acknowledges the financial support from Grupos Consolidados UPV/EHU del Gobierno Vasco (IT578-13) and EU-H2020 project “MOSTOPHOS” (no. 646259). A.N.K., T.W.C., and R.L.M. acknowledge the ERC and EPSRC for financial support, and the Nanoscale & Microscale Research Centre (nmRC). T.Z., J.B., and U.K. gratefully acknowledge the funding by the DFG (German Research Foundation) and the Ministry of Science, Research and the Arts (MWK) of Baden Wuerttemberg in the framework of the SALVE (Sub Angstrom Low-Voltage Electron Microscopy) project.

We demonstrate milling of partial antenna gaps and narrow conducting bridges with nanometer precision using a helium ion beam microscope. Single particle spectroscopy shows large shifts in the plasmonic mode spectrum of the milled antennas, associated with the transition from capacitive to conductive gap loading. A conducting bridge of nanometer height is found sufficient to shift the antenna from the capacitive to the conductive coupling regime, in agreement with circuit theory. Picosecond pump-probe spectroscopy reveals an enhanced nonlinear response for partially milled antennas, reaching an optimum value for an intermediate bridge height. Our results show that manipulation of the antenna load can be used to increase the nonlinear response of plasmonic antennas. © 2013 American Chemical Society., This work was supported by EPSRC through grant EP/J011797/1; O.M. acknowledges support through an EPSRC fellowship EP/J016918/1.

Graphene is used as the thinnest possible spacer between gold nanoparticles and a gold substrate. This creates a robust, repeatable, and stable subnanometer gap for massive plasmonic field enhancements. White light spectroscopy of single 80 nm gold nanoparticles reveals plasmonic coupling between the particle and its image within the gold substrate. While for a single graphene layer, spectral doublets from coupled dimer modes are observed shifted into the near-infrared, these disappear for increasing numbers of layers. These doublets arise from charger-transfer-sensitive gap plasmons, allowing optical measurement to access out-of-plane conductivity in such layered systems. Gating the graphene can thus directly produce plasmon tuning. © 2013 American Chemical Society., We gratefully acknowledge support from U.K. EPSRC Grants EP/G060649/1, EP/G037221/1, EP/H007024/1, EP/G042357/1, EP/K01711X/1, EP/K017144/1, from ERC Grants LINASS 320503 and NANOPOTS, from Nokia Research Centre, and from a Royal Society Wolfson Research Merit Award, EU Grants RODIN, GENIUS, CareRAMM, Graphene Flagship (contract no. CNECT-ICT-604391), Project FIS2010-19609-C02-01 of the Spanish Ministry of Science and Education and project IT756-13 of the Basque Government for groups in the UPV/EHU. J.M. acknowledges support from the Winton Programme of the Physics of Sustainability.

We report the light-induced formation of conductive links across nanometer-wide insulating gaps. These are realized by incorporating spacers of molecules or 2D monolayers inside a gold plasmonic nanoparticle-on-mirror (NPoM) geometry. Laser irradiation of individual NPoMs controllably reshapes and tunes the plasmonic system, in some cases forming conductive bridges between particle and substrate, which shorts the nanometer-wide plasmonic gaps geometrically and electronically. Dark-field spectroscopy monitors the bridge formation in situ, revealing strong plasmonic mode mixing dominated by clear anticrossings. Finite difference time domain simulations confirm this spectral evolution, which gives insights into the metal filament formation. A simple analytic cavity model describes the observed plasmonic mode hybridization between tightly confined plasmonic cavity modes and a radiative antenna mode sustained in the NPoM. Our results show how optics can reveal the properties of electrical transport across well-defined metallic nanogaps to study and develop technologies such as resistive memory devices (memristors)., We gratefully acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EPSRC NanoDTC EP/L015978/1 and ERC grant LINASS 320503. J.M. and F.B. acknowledge support from the Winton Programme of the Physics of Sustainability. J.A. acknowledges financial support from Project FIS2013- 41184-P from MINECO and IT756-13 from the Basque Government consolidated groups.

This is an open access article published under a Creative Commons Attribution (CC-BY) License.-- et al., Gold nanoparticles are separated above a planar gold film by 1.1 nm thick self-assembled molecular monolayers of different conductivities. Incremental replacement of the nonconductive molecules with a chemically equivalent conductive version differing by only one atom produces a strong 50 nm blue-shift of the coupled plasmon. With modeling this gives a conductance of 0.17G0 per biphenyl-4,4′-dithiol molecule and a total conductance across the plasmonic junction of 30G0. Our approach provides a reliable tool quantifying the number of molecules in each plasmonic hotspot, here, We acknowledge financial support from EPSRC grant EP/G060649/1, EP/I012060/1, EP/L027151/1, EP/K028510/1, ERC grant LINASS 320503. F.B. acknowledges support from the Winton Programme for the Physics of Sustainability. C.T. and J.A. acknowledge financial support from Project FIS2013-41184-P from MINECO, ETORTEK 2014-15 of the Basque Department of Industry and IT756-13 from the Basque consolidated groups.

Responsive hybrid nanomaterials with well-defined properties are of significant interest for the development of biosensors with additional applications in tissue engineering and drug delivery. Here, we present a detailed characterization using UV-vis spectroscopy and small angle X-ray scattering of a hybrid material comprised of polypeptide-decorated gold nanoparticles with highly controllable assembly properties. The assembly is triggered by a folding-dependent bridging of the particles mediated by the heteroassociation of immobilized helix-loop-helix polypeptides and a complementary nonlinear polypeptide present in solution. The polypeptides are de novo designed to associate and fold into a heterotrimeric complex comprised of two disulfide-linked four-helix bundles. The particles form structured assemblies with a highly defined interparticle gap (4.8 ± 0.4 nm) that correlates to the size of the folded polypeptides. Transitions in particle aggregation dynamics, mass-fractal dimensions and ordering, as a function of particle size and the concentration of the bridging polypeptide, are observed; these have significant effects on the optical properties of the assemblies. The assembly and ordering of the particles are highly complex processes that are affected by a large number of variables including the number of polypeptides bridging the particles and the particle mobility within the aggregates. A fundamental understanding of these processes is of paramount interest for the development of novel hybrid nanomaterials with tunable structural and optical properties and for the optimization of nanoparticle-based colorimetric biodetection strategies. © 2011 American Chemical Society., Financial support from the Knut and Alice Wallenberg Foundation (KAW) for D.A., the EPSRC and ERC Grant “Naturale” for M.M.S., the Swedish Research Council (VR), and the Swedish Foundation for Strategic Research (SSF) is gratefully acknowledged. B.S. acknowledges the “Ramón y Cajal” program from “Ministerio de Ciencia e Innovación” of Spain for financial support. We thank the Australian synchrotron for synchrotron time on the SAXS beamline (Grant AS093/SAXS1875) and the extensive support of the beamline scientists (Dr. Hawley and Dr. Mudie) without whom this research could not have been performed. We thank Dr. Nicholas Schaeffer and Dr. Aaron Eberle for discussions and input.