arXiv subjects

S. Boukari

Publications and source records attributed to S. Boukari.

9 recordsLinked to original sources

arXiv2026

A low-tech solution to process entire metal/molecule heterostructure stacks into vertical nanopillar electronic devices

Quantum technologies aim to assemble devices whose operation is controlled by the quantum state of individual atoms. Achieving this level of control in a practical, scalable design remains, however, a major obstacle to mass societal adoption. By working at the level of interatomic bonding, molecular engineering has enabled exquisite control over the electronic properties of individual atoms and their interactions with neighboring atoms. This positions molecular electronics as a potentially disruptive quantum technology, but serious technological challenges have prevented it from being included in technical road maps. The main obstacle is that conventional, mass scalable nanodevice technologies utilize resists and solvents that can degrade molecules. Some approaches involve exposing junction interfaces to contaminants (e.g. air, resist etc...), which can be particularly problematic for spintronics. In this technical paper, we present our decade-long work into building a nanotechnological chain that can process entire metal/molecule heterostructures into vertical nanopillars electronic devices. We discuss the advantages and pitfalls of the various iterations of this process that were implemented. We also discuss outlooks for this unique technology.

cond-mat.mes-hall↗

arXiv2019

Magnetoresistance and spintronic anisotropy induced by spin excitations along molecular spin chains

Electrically manipulating the quantum properties of nano-objects, such as atoms or molecules, is typically done using scanning tunnelling microscopes and lateral junctions. The resulting nanotransport path is well established in these model devices. Societal applications require transposing this knowledge to nano-objects embedded within vertical solid-state junctions, which can advantageously harness spintronics to address these quantum properties thanks to ferromagnetic electrodes and high-quality interfaces. The challenge here is to ascertain the device's effective, buried nanotransport path, and to electrically involve these nano-objects in this path by shrinking the device area from the macro- to the nano-scale while maintaining high structural/chemical quality across the heterostructure. We've developed a low-tech, resist- and solvent-free technological process that can craft nanopillar devices from entire in-situ grown heterostructures, and use it to study magnetotransport between two Fe and Co ferromagnetic electrodes across a functional magnetic CoPc molecular layer. We observe how spin-flip transport across CoPc molecular spin chains promotes a specific magnetoresistance effect, and alters the nanojunction's magnetism through spintronic anisotropy. In the process, we identify three magnetic units along the effective nanotransport path thanks to a macrospin model of magnetotransport. Our work elegantly connects the until now loosely associated concepts of spin-flip spectroscopy, magnetic exchange bias and magnetotransport due to molecular spin chains, within a solid-state device. We notably measure a 5.9meV energy threshold for magnetic decoupling between the Fe layer's buried atoms and those in contact with the CoPc layer forming the so-called 'spinterface'. This provides a first insight into the experimental energetics of this promising low-power information encoding unit.

cond-mat.mes-hall↗

arXiv2019

Hole transport across MgO-based magnetic tunnel junctions with high resistance-area product due to oxygen vacancies

The quantum mechanical tunnelling process conserves the quantum properties of the particle considered. As applied to solid-state tunnelling (SST), this physical law was verified, within the field of spintronics, regarding the electron spin in early experiments across Ge tunnel barriers, and in the 90s across Al2O3 barriers. The conservation of the quantum parameter of orbital occupancy, as grouped into electronic symmetries, was observed in the '00s across MgO barriers, followed by SrTiO3 (STO). Barrier defects, such as oxygen vacancies, partly conserve this electronic symmetry. In the solid-state, an additional subtlety is the sign of the charge carrier: are holes or electrons involved in transport? We demonstrate that SST across MgO magnetic tunnel junctions (MTJs) with a large resistance-area (RA) product involves holes by examining how shifting the MTJ's Fermi level alters the ensuing barrier heights defined by the barrier's oxygen vacancies. In the process, we consolidate the description of tunnel barrier heights induced by specific oxygen-vacancy induced localized states. Our work opens prospects to understand the concurrent observation of high TMR and spin transfer torque across MgO-based nanopillars.

cond-mat.mes-hall↗

arXiv2018

Spin-driven electrical power generation at room temperature

To mitigate climate change, our global society is harnessing direct (solar irradiation) and indirect (wind/water flow) sources of renewable electrical power generation. Emerging direct sources include current-producing thermal gradients in thermoelectric materials, while quantum physics-driven processes to convert quantum information into energy have been demonstrated at very low temperatures. The magnetic state of matter, assembled by ordering the electron's quantum spin property, represents a sizeable source of built-in energy. We propose to create a direct source of electrical power at room temperature (RT) by utilizing magnetic energy to harvest thermal fluctuations on paramagnetic (PM) centers. Our spin engine rectifies current fluctuations across the PM centers' spin states according to the electron spin by utilizing so-called 'spinterfaces' with high spin polarization. As a rare experimental event, we demonstrate how this path can generate 0.1nW at room temperature across a 20 micron-wide spintronic device called the magnetic tunnel junction, assembled using commonplace Co, C and MgO materials. The presence of this path in our experiment, which also generates very high spintronic performance, is confirmed by analytical and ab-initio calculations. Device downscaling, and the ability for other materials systems than the spinterface to select a transport spin channel at RT widens opportunities for routine device reproduction. The challenging control over PM centers within the tunnel barrier's nanotransport path may be addressed using oxide- and organic-based nanojunctions. At present densities in MRAM products, this spin engine could lead to 'always-on' areal power densities well beyond that generated by solar irradiation on earth. Further developing this concept can fundamentally alter our energy-driven society's global economic, social and geopolitical constructs.

cond-mat.mes-hall↗

arXiv2017

Cu metal / Mn phthalocyanine organic spinterfaces atop Co with high spin polarization at room temperature

The organic spinterface describes the spin-polarized properties that develop, due to charge transfer, at the interface between a ferromagnetic metal (FM) and the molecules of an organic semiconductor. Yet, if the latter is also magnetic (e.g. molecular spin chains), the interfacial magnetic coupling can generate complexity within magnetotransport experiments. Also, assembling this interface may degrade the properties of its constituents (e.g. spin crossover or non-sublimable molecules). To circumvent these issues, one can separate the molecular and FM films using a less reactive nonmagnetic metal (NM). Spin-resolved photoemission spectroscopy measurements on the prototypical system Co(001)//Cu/Mnphthalocyanine (MnPc) reveal that the Cu/MnPc spinterface atop ferromagnetic Co is highly spin-polarized at room temperature, up to Cu spacer thicknesses of at least 10 monolayers. Ab-initio theory describes a spin polarization of the topmost Cu layer after molecular hybridization that can be accompanied by magnetic hardening effects. This spinterface's unexpected robustness paves the way for 1) integrating electronically fragile molecules within organic spinterfaces, and 2) manipulating molecular spin chains using the well-documented spin transfer torque properties of the FM/NM bilayer.

cond-mat.mtrl-sci↗

arXiv2014

Efficient, high-density, carbon-based spinterfaces

The research field of spintronics has sought, over the past 25 years and through several materials science tracks, a source of highly spin-polarized current at room temperature. Organic spinterfaces, which consist in an interface between a ferromagnetic metal and a molecule, represent the most promising track as demonstrated for a handful of interface candidates. How general is this effect? We deploy topographical and spectroscopic techniques to show that a strongly spin-polarized interface arises already between ferromagnetic cobalt and mere carbon atoms. Scanning tunneling microscopy and spectroscopy show how a dense semiconducting carbon film with a low band gap of about 0.4 eV is formed atop the metallic interface. Spin-resolved photoemission spectroscopy reveals a high degree of spin polarization at room temperature of carbon-induced interface states at the Fermi energy. From both our previous study of cobalt/phthalocyanine spinterfaces and present x-ray photoemission spectroscopy studies of the cobalt/carbon interface, we infer that these highly spin-polarized interface states arise mainly from sp2-bonded carbon atoms. We thus demonstrate the molecule-agnostic, generic nature of the spinterface formation.

cond-mat.mtrl-sci↗

arXiv2012

Direct observation of a highly spin-polarized organic spinterface at room temperature

The design of large-scale electronic circuits that are entirely spintronics-driven requires a current source that is highly spin-polarised at and beyond room temperature, cheap to build, efficient at the nanoscale and straightforward to integrate with semiconductors. Yet despite research within several subfields spanning nearly two decades, this key building block is still lacking. We experimentally and theoretically show how the interface between Co and phthalocyanine molecules constitutes a promising candidate. Spin-polarised direct and inverse photoemission experiments reveal a high degree of spin polarisation at room temperature at this interface. We measured a magnetic moment on the molecules's nitrogen pi orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanims in each spin channel. We propose, through this example, a recipe to engineer simple organic-inorganic interfaces with remarkable spintronic properties that can endure well above room temperature.

cond-mat.mtrl-sci↗

arXiv2010

Control of defect-mediated tunneling barrier heights in ultrathin MgO films

The impact of oxygen vacancies on local tunneling properties across rf-sputtered MgO thin films was investigated by optical absorption spectroscopy and conducting atomic force microscopy. Adding O$_2$ to the Ar plasma during MgO growth alters the oxygen defect populations, leading to improved local tunneling characteristics such as a lower density of current hotspots and a lower tunnel current amplitude. We discuss a defect-based potential landscape across ultrathin MgO barriers.

cond-mat.mtrl-sci↗

arXiv2009

Study of molecular spin-crossover complex Fe(phen)2(NCS)2 thin films

We report on the growth by evaporation under high vacuum of high-quality thin films of Fe(phen)2(NCS)2 (phen=1,10-phenanthroline) that maintain the expected electronic structure down to a thickness of 10 nm and that exhibit a temperature-driven spin transition. We have investigated the current-voltage characteristics of a device based on such films. From the space charge-limited current regime, we deduce a mobility of 6.5x10-6 cm2/V?s that is similar to the low-range mobility measured on the widely studied tris(8-hydroxyquinoline)aluminium organic semiconductor. This work paves the way for multifunctional molecular devices based on spin-crossover complexes.

cond-mat.mtrl-sci↗