Jean-Francois Dayen

Light-triggered self-construction of supramolecular organic nanowires as metallic interconnects

The construction of soft and processable organic material able to display metallic conduction properties-a large density of freely moving charges-is a major challenge for electronics. Films of doped conjugated polymers are widely used as semiconductor devices, but metallic-type transport in the bulk of such materials remains extremely rare. On the other hand, single-walled carbon nanotubes can exhibit remarkably low contact resistances with related large currents, but are intrinsically very difficult to isolate and process. Here, we describe the self-assembly of supramolecular organic nanowires between two metallic electrodes, from a solution of triarylamine derivative, under the simultaneous action of light and electric field triggers. They exhibit a combination of large conductivity values (>5 × 10(3) S m(-1)) and a low interface resistance (<2 × 10(-4) Ω m). Moreover, the resistance of nanowires in series with metal interfaces systematically decreases when the temperature is lowered to 1.5 K, revealing an intrinsic metallic behaviour.

Conductivity in organic semiconductors hybridized with the vacuum field.

Much effort over the past decades has been focused on improving carrier mobility in organic thin-film transistors by optimizing the organization of the material or the device architecture. Here we take a different path to solving this problem, by injecting carriers into states that are hybridized to the vacuum electromagnetic field. To test this idea, organic semiconductors were strongly coupled to plasmonic modes to form coherent states that can extend over as many as 10(5) molecules and should thereby favour conductivity. Experiments show that indeed the current does increase by an order of magnitude at resonance in the coupled state, reflecting mostly a change in field-effect mobility. A theoretical quantum model confirms the delocalization of the wavefunctions of the hybridized states and its effect on the conductivity. Our findings illustrate the potential of engineering the vacuum electromagnetic environment to modify and to improve properties of materials.

Spin transition in arrays of gold nanoparticles and spin crossover molecules.

We investigate if the functionality of spin crossover molecules is preserved when they are assembled into an interfacial device structure. Specifically, we prepare and investigate gold nanoparticle arrays, into which room-temperature spin crossover molecules are introduced, more precisely, [Fe(AcS-BPP)2](ClO4)2, where AcS-BPP = (S)-(4-{[2,6-(dipyrazol-1-yl)pyrid-4-yl]ethynyl}phenyl)ethanethioate (in short, Fe(S-BPP)2). We combine three complementary experiments to characterize the molecule-nanoparticle structure in detail. Temperature-dependent Raman measurements provide direct evidence for a (partial) spin transition in the Fe(S-BPP)2-based arrays. This transition is qualitatively confirmed by magnetization measurements. Finally, charge transport measurements on the Fe(S-BPP)2-gold nanoparticle devices reveal a minimum in device resistance versus temperature, R(T), curves around 260-290 K. This is in contrast to similar networks containing passive molecules only that show monotonically decreasing R(T) characteristics. Backed by density functional theory calculations on single molecular conductance values for both spin states, we propose to relate the resistance minimum in R(T) to a spin transition under the hypothesis that (1) the molecular resistance of the high spin state is larger than that of the low spin state and (2) transport in the array is governed by a percolation model.

Side‐Gated Transport in Focused‐Ion‐Beam‐Fabricated Multilayered Graphene Nanoribbons

In this Letter, we present the patterning, exfoliation and micromanipulation of thin graphitic discs which are subsequently connected and patterned into sub-100nm wide ribbons with a resist-free process using Focused Ion Beam (FIB) lithography and deposition. The electronic transport properties of the double side-gated nanoribbons are then investigated down to 40 K and interpreted with a simple model of 1D array of tunnelling junctions.

Nanoplatelets Bridging a Nanotrench: A New Architecture for Photodetectors with Increased Sensitivity

Interparticle charge hopping severely limits the integration of colloidal nanocrystals films for optoelectronic device applications. We propose here to overcome this problem by using high aspect ratio interconnects made of wide electrodes separated by a few tens of namometers, a distance matching the size of a single nanoplatelet. The semiconducting CdSe/CdS nanoplatelet coupling with such electrodes allows an efficient electron-hole pair dissociation despite the large binding energy of the exciton, resulting in optimal photoconductance responsivity. We report the highest responsivity obtained so far for CdSe colloidal material with values reaching kA·W(-1), corresponding to eight decades of enhancement compared to usual micrometer-scaled architectures. In addition, a decrease of 1 order of magnitude of the current noise is observed, revealing the reduced influence of the surface traps on transport. The nanotrench geometry provides top access to ion gel electrolyte gating, allowing for a photoresponsive transistor with 10(4) on/off ratio. A simple analytical model reproduces the device behavior and underlines the key parameters related to its performance.

Enhancing the Molecular Signature in Molecule-Nanoparticle Networks Via Inelastic Cotunneling

Charge transport in networks of nanoparticles linked by molecular spacers is investigated. Remarkably, in the regime where cotunneling dominates, the molecular signature of a device is strongly enhanced. We demonstrate that the resistance ratio of identical networks with different molecular spacers increases dramatically, from an initial value of 50 up to 10(5) , upon entering the cotunneling regime. Our work shows that intrinsic molecular properties can be amplified through nanoscale engineering.

Nanotrench for nano and microparticle electrical interconnects

We present a simple and versatile patterning procedure for the reliable and reproducible fabrication of high aspect ratio (10(4)) electrical interconnects that have separation distances down to 20 nm and lengths of several hundreds of microns. The process uses standard optical lithography techniques and allows parallel processing of many junctions, making it easily scalable and industrially relevant. We demonstrate the suitability of these nanotrenches as electrical interconnects for addressing micro and nanoparticles by realizing several circuits with integrated species. Furthermore, low impedance metal-metal low contacts are shown to be obtained when trapping a single metal-coated microsphere in the gap, emphasizing the intrinsic good electrical conductivity of the interconnects, even though a wet process is used. Highly resistive magnetite-based nanoparticles networks also demonstrate the advantage of the high aspect ratio of the nanotrenches for providing access to electrical properties of highly resistive materials, with leakage current levels below 1 pA.

Voltage-controlled inversion of tunnel magnetoresistance in epitaxial nickel/graphene/MgO/cobalt junctions

We report on the fabrication and characterization of vertical spin-valve structures using a thick epitaxial MgO barrier as spacer layer and a graphene-passivated Ni film as bottom ferromagnetic electrode. The devices show robust and scalable tunnel magnetoresistance, with several changes of sign upon varying the applied bias voltage. These findings are explained by a model of phonon-assisted transport mechanisms that relies on the peculiarity of the band structure and spin density of states at the hybrid graphene|Ni interface.

Electronic transport of silicon nanowires grown in porous Al2O3 membrane

Electronic transport properties of silicon nanowires grown by chemical vapor deposition, embedded in an insulating alumina nanoporous membrane are studied. Transport measurements were performed from 300to4.2K, which revealed a scaling law of the conductance as a function of the temperature and the dc bias voltage, which the authors interpreted as a Coulomb blockade manifestation. Magnetoconductive measurements at low temperature revealed a positive magnetoconductance which can be well fitted by quasi-one-dimensional (quasi-1D) weak localization theory. These results seem to indicate that electron-electron interactions and quasi-1D effect predominate on the electronic transport properties of these systems.

Anisotropic magnetothermopower : Contribution of interband relaxation

Spin injection in metallic normal/ferromagnetic junctions is investigated taking into account interband relaxation and the consequences in terms of thermoelectric power. On the basis of a generalized two-channel model, it is shown that there is an interface resistance and thermoelectric power contribution due to anisotropic scattering, besides spin accumulation and giant magnetoresistance. The corresponding expression of the thermoelectric power is derived and compared with the expression accounting for the thermoelectric power produced by the giant magnetoresistance. Measurements of anisotropic magnetothermoelectric power are presented in electrodeposited Ni nanowires contacted with Ni, Au, and Cu. It is shown that a thermoelectric power is generated at the interfaces of the nanowire and that the experimental results strongly support the model.