Odd Nonlinear Conductivity under Spatial Inversion in Chiral Tellurium.

Electrical transport in noncentrosymmetric materials departs from the well-established phenomenological Ohm's law. Instead of a linear relation between current and electric field, a nonlinear conductivity emerges along specific crystallographic directions. This nonlinear transport is fundamentally related to the lack of spatial inversion symmetry. However, the experimental implications of an inversion symmetry operation on the nonlinear conductivity remain to be explored. Here, we report on a large, nonlinear conductivity in chiral tellurium. By measuring samples with opposite handedness, we demonstrate that the nonlinear transport is odd under spatial inversion. Furthermore, by applying an electrostatic gate, we modulate the nonlinear output by a factor of 300, reaching the highest reported value excluding engineered heterostructures. Our results establish chiral tellurium as an ideal compound not just to study the fundamental interplay between crystal structure, symmetry operations and nonlinear transport; but also to develop wireless rectifiers and energy-harvesting chiral devices.

Gate-tuneable and chirality-dependent charge-to-spin conversion in tellurium nanowires.

Chiral materials are an ideal playground for exploring the relation between symmetry, relativistic effects and electronic transport. For instance, chiral organic molecules have been intensively studied to electrically generate spin-polarized currents in the last decade, but their poor electronic conductivity limits their potential for applications. Conversely, chiral inorganic materials such as tellurium have excellent electrical conductivity, but their potential for enabling the electrical control of spin polarization in devices remains unclear. Here, we demonstrate the all-electrical generation, manipulation and detection of spin polarization in chiral single-crystalline tellurium nanowires. By recording a large (up to 7%) and chirality-dependent unidirectional magnetoresistance, we show that the orientation of the electrically generated spin polarization is determined by the nanowire handedness and uniquely follows the current direction, while its magnitude can be manipulated by an electrostatic gate. Our results pave the way for the development of magnet-free chirality-based spintronic devices.

All-Electrical Spin-to-Charge Conversion in Sputtered BixSe1-x.

One of the major obstacles to realizing spintronic devices such as MESO logic devices is the small signal magnitude used for magnetization readout, making it important to find materials with high spin-to-charge conversion efficiency. Although intermixing at the junction of two materials is a widely occurring phenomenon, its influence on material characterization and the estimation of spin-to-charge conversion efficiencies are easily neglected or underestimated. Here, we demonstrate all-electrical spin-to-charge conversion in BixSe1-x nanodevices and show how the conversion efficiency can be overestimated by tens of times depending on the adjacent metal used as a contact. We attribute this to the intermixing-induced compositional change and the properties of a polycrystal that lead to drastic changes in resistivity and spin Hall angle. Strategies to improve the spin-to-charge conversion signal in similar structures for functional devices are discussed.

Doping of Carbon Nanotubes with Encapsulated Phosphorus Chains.

Single-walled carbon nanotubes (SWCNTs) are a perfect host for the formation of one-dimensional phosphorus structures and to obtain hybrid materials with a large P-C ratio. This work presents a procedure for high-yield phosphorus filling of commercial Tuball SWCNTs and efficient removal of phosphorus deposits from the external nanotube surface. We probed white and red phosphorus as precursors, varied the synthesis temperature and the ampoule shape, and tested three solvents for sample purification. High-resolution transmission electron microscopy and Raman spectroscopy indicated crystallization of interior phosphorus in a form resembling fibrous red phosphorus. An aqueous sodium hydroxide solution allowed removing the majority of external phosphorus particles. Thermogravimetric analysis of the product determined ∼23 wt % (∼10 atom %) of phosphorus, and the X-ray photoelectron spectroscopy (XPS) data showed that ca. 80% of it is in the form of elemental phosphorus. Externally purified SWCNTs filled with phosphorus were used to study the interaction between the components. Raman spectroscopy and core-level XPS revealed p-type SWCNT doping. Valence-band XPS data and density functional theory calculations confirmed the transfer of the SWCNT electron density to the encapsulated phosphorus.

Strong Interfacial Exchange Field in a Heavy Metal/Ferromagnetic Insulator System Determined by Spin Hall Magnetoresistance.

Spin-dependent transport at heavy metal/magnetic insulator interfaces is at the origin of many phenomena at the forefront of spintronics research. A proper quantification of the different interfacial spin conductances is crucial for many applications. Here, we report the first measurement of the spin Hall magnetoresistance (SMR) of Pt on a purely ferromagnetic insulator (EuS). We perform SMR measurements in a wide range of temperatures and fit the results by using a microscopic model. From this fitting procedure, we obtain the temperature dependence of the spin conductances (Gs, Gr, and Gi), disentangling the contribution of field-like torque (Gi), damping-like torque (Gr), and spin-flip scattering (Gs). An interfacial exchange field of the order of 1 meV acting upon the conduction electrons of Pt can be estimated from Gi, which is at least three times larger than Gr below the Curie temperature. Our work provides an easy method to quantify this interfacial spin-splitting field, which plays a key role in emerging fields such as superconducting spintronics and caloritronics as well as topological quantum computation.

Large Multidirectional Spin-to-Charge Conversion in Low-Symmetry Semimetal MoTe2 at Room Temperature.

Efficient and versatile spin-to-charge current conversion is crucial for the development of spintronic applications, which strongly rely on the ability to electrically generate and detect spin currents. In this context, the spin Hall effect has been widely studied in heavy metals with strong spin-orbit coupling. While the high crystal symmetry in these materials limits the conversion to the orthogonal configuration, unusual configurations are expected in low-symmetry transition-metal dichalcogenide semimetals, which could add flexibility to the electrical injection and detection of pure spin currents. Here, we report the observation of spin-to-charge conversion in MoTe2 flakes, which are stacked in graphene lateral spin valves. We detect two distinct contributions arising from the conversion of two different spin orientations. In addition to the conventional conversion where the spin polarization is orthogonal to the charge current, we also detect a conversion where the spin polarization and the charge current are parallel. Both contributions, which could arise either from bulk spin Hall effect or surface Edelstein effect, show large efficiencies comparable to the best spin Hall metals and topological insulators. Our finding enables the simultaneous conversion of spin currents with any in-plane spin polarization in one single experimental configuration.

Colloidal branched CdSe/CdS 'nanospiders' with 2D/1D heterostructure.

In this paper we report the synthesis of colloidal CdSe/CdS core-shell heteronanoplatelets with epitaxially grown wurtzite (WZ) 1D CdS branches or legs by using cadmium diethyldithiocarbamate as a single-source precursor. The growth of WZ branches was achieved by exploiting zinc blende-wurtzite polytypism of cadmium chalcogenides induced by oleylamine. Synthesized 'nanospiders' exhibit enhanced absorption in the UV-blue region and narrow and relatively intense red photoluminescence depending on the amount of CdS in the heteronanostructure.

Remote Magnetomechanical Nanoactuation.

A novel approach to nanoactuation that relies on magnetomechanics instead of the conventional electromechanics utilized in micro and nanoactuated mechanical systems is devised and demonstrated. Namely, nanoactuated magnetomechanical devices that can change shape on command using a remote magnetic external stimulus, with a control at the subnanometer scale are designed and fabricated. In contrast to micro and nanoactuated electromechanical systems, nanoactuated magnetomechanical remote activation does not require physical contacts. Remote activation and control have a tremendous potential in bringing vast technological capabilities to more diverse environments, such as liquids or even inside living organisms, opening a clear path to applications in biotechnology and the emerging field of nanorobotics.

Chiral templating of self-assembling nanostructures by circularly polarized light.

The high optical and chemical activity of nanoparticles (NPs) signifies the possibility of converting the spin angular momenta of photons into structural changes in matter. Here, we demonstrate that illumination of dispersions of racemic CdTe NPs with right- (left-)handed circularly polarized light (CPL) induces the formation of right- (left-)handed twisted nanoribbons with an enantiomeric excess exceeding 30%, which is ∼10 times higher than that of typical CPL-induced reactions. Linearly polarized light or dark conditions led instead to straight nanoribbons. CPL 'templating' of NP assemblies is based on the enantio-selective photoactivation of chiral NPs and clusters, followed by their photooxidation and self-assembly into nanoribbons with specific helicity as a result of chirality-sensitive interactions between the NPs. The ability of NPs to retain the polarization information of incident photons should open pathways for the synthesis of chiral photonic materials and allow a better understanding of the origins of biomolecular homochirality.

Virus-Templated Near-Amorphous Iron Oxide Nanotubes.

We present a simple synthesis of iron oxide nanotubes, grown under very mild conditions from a solution containing Fe(II) and Fe(III), on rod-shaped tobacco mosaic virus templates. Their well-defined shape and surface chemistry suggest that these robust bionanoparticles are a versatile platform for synthesis of small, thin mineral tubes, which was achieved efficiently. Various characterization tools were used to explore the iron oxide in detail: Electron microscopy (SEM, TEM), magnetometry (SQUID-VSM), diffraction (XRD, TEM-SAED), electron spectroscopies (EELS, EDX, XPS), and X-ray absorption (XANES with EXAFS analysis). They allowed determination of the structure, crystallinity, magnetic properties, and composition of the tubes. The protein surface of the viral templates was crucial to nucleate iron oxide, exhibiting analogies to biomineralization in natural compartments such as ferritin cages.

Structural peculiarities of single crystal diamond needles of nanometer thickness.

Diamond is attractive for various applications due to its unique mechanical and optical properties. In particular, single crystal diamond needles with high aspect ratios and sharp apexes of nanometer size are demanded for different types of optical sensors including optically sensing tip probes for scanning microscopy. This paper reports on electron microscopy and Raman spectroscopy characterization of the diamond needles having geometrically perfect pyramidal shapes with rectangular atomically flat bases with (001) crystallography orientation, 2-200 nm sharp apexes, and with lengths from about 10-160 µm. The needles were produced by selective oxidation of (001) textured polycrystalline diamond films grown by chemical vapor deposition. Here we study the types and distribution of defects inside and on the surface of the single crystal diamond needles. We show that sp3 type point defects are incorporated into the volume of the diamond crystal during growth, while the surface of the lateral facets is enriched by multiple extended defects. Nitrogen addition to the reaction mixture results in increase of the growth rate on {001} facets correlated with the rise in the concentration of sp3 type defects.

Temperature dependent radiative and non-radiative recombination dynamics in CdSe-CdTe and CdTe-CdSe type II hetero nanoplatelets.

We investigate the temperature-dependent decay kinetics of type II CdSe-CdTe and CdTe-CdSe core-lateral shell nanoplatelets. From a kinetic analysis of the photoluminescence (PL) decay and a measurement of the temperature dependent quantum yield we deduce the temperature dependence of the non-radiative and radiative lifetimes of hetero nanoplates. In line with the predictions of the giant oscillator strength effect in 2D we observe a strong increase of the radiative lifetime with temperature. This is attributed to an increase of the homogeneous transition linewidth with temperature. Comparing core only and hetero platelets we observe a significant prolongation of the radiative lifetime in type II platelets by two orders in magnitude while the quantum yield is barely affected. In a careful analysis of the PL decay transients we compare different recombination models, including electron hole pairs and exciton decay, being relevant for the applicability of those structures in photonic applications like solar cells or lasers. We conclude that the observed biexponential PL decay behavior in hetero platelets is predominately due to spatially indirect excitons being present at the hetero junction and not ionized e-h pair recombination.

Weak Delocalization in Graphene on a Ferromagnetic Insulating Film.

Graphene has been predicted to develop a magnetic moment by proximity effect when placed on a ferromagnetic film, a promise that could open exciting possibilities in the fields of spintronics and magnetic data recording. In this work, the interplay between the magnetoresistance of graphene and the magnetization of an underlying ferromagnetic insulating film is studied in detail. A clear correlation between both magnitudes is observed but through a careful modeling of the magnetization and the weak localization measurements, that such correspondence can be explained by the effects of the magnetic stray fields arising from the ferromagnetic insulator is found. The results emphasize the complexity arising at the interface between magnetic and 2D materials.

Resonant antenna probes for tip-enhanced infrared near-field microscopy.

We report the development of infrared-resonant antenna probes for tip-enhanced optical microscopy. We employ focused-ion-beam machining to fabricate high-aspect ratio gold cones, which replace the standard tip of a commercial Si-based atomic force microscopy cantilever. Calculations show large field enhancements at the tip apex due to geometrical antenna resonances in the cones, which can be precisely tuned throughout a broad spectral range from visible to terahertz frequencies by adjusting the cone length. Spectroscopic analysis of these probes by electron energy loss spectroscopy, Fourier transform infrared spectroscopy, and Fourier transform infrared near-field spectroscopy corroborates their functionality as resonant antennas and verifies the broad tunability. By employing the novel probes in a scattering-type near-field microscope and imaging a single tobacco mosaic virus (TMV), we experimentally demonstrate high-performance mid-infrared nanoimaging of molecular absorption. Our probes offer excellent perspectives for optical nanoimaging and nanospectroscopy, pushing the detection and resolution limits in many applications, including nanoscale infrared mapping of organic, molecular, and biological materials, nanocomposites, or nanodevices.

Toward sub-second solution exchange dynamics in flow reactors for liquid-phase transmission electron microscopy.

Liquid-phase transmission electron microscopy is a burgeoning experimental technique for monitoring nanoscale dynamics in a liquid environment, increasingly employing microfluidic reactors to control the composition of the sample solution. Current challenges comprise fast mass transport dynamics inside the central nanochannel of the liquid cell, typically flow cells, and reliable fixation of the specimen in the limited imaging area. In this work, we present a liquid cell concept - the diffusion cell - that satisfies these seemingly contradictory requirements by providing additional on-chip bypasses to allow high convective transport around the nanochannel in which diffusive transport predominates. Diffusion cell prototypes are developed using numerical mass transport models and fabricated on the basis of existing two-chip setups. Important hydrodynamic parameters, i.e., the total flow resistance, the flow velocity in the imaging area, and the time constants of mixing, are improved by 2-3 orders of magnitude compared to existing setups. The solution replacement dynamics achieved within seconds already match the mixing timescales of many ex-situ scenarios, and further improvements are possible. Diffusion cells can be easily integrated into existing liquid-phase transmission electron microscopy workflows, provide correlation of results with ex-situ experiments, and can create additional research directions addressing fast nanoscale processes.

Voltage-based magnetization switching and reading in magnetoelectric spin-orbit nanodevices.

As CMOS technologies face challenges in dimensional and voltage scaling, the demand for novel logic devices has never been greater, with spin-based devices offering scaling potential, at the cost of significantly high switching energies. Alternatively, magnetoelectric materials are predicted to enable low-power magnetization control, a solution with limited device-level results. Here, we demonstrate voltage-based magnetization switching and reading in nanodevices at room temperature, enabled by exchange coupling between multiferroic BiFeO3 and ferromagnetic CoFe, for writing, and spin-to-charge current conversion between CoFe and Pt, for reading. We show that, upon the electrical switching of the BiFeO3, the magnetization of the CoFe can be reversed, giving rise to different voltage outputs. Through additional microscopy techniques, magnetization reversal is linked with the polarization state and antiferromagnetic cycloid propagation direction in the BiFeO3. This study constitutes the building block for magnetoelectric spin-orbit logic, opening a new avenue for low-power beyond-CMOS technologies.

CdSe-CdS nanoheteroplatelets with efficient photoexcitation of central CdSe region through epitaxially grown CdS wings.

We synthesized a new type of optically active semiconductor nanoheterostructure based on CdSe nanoplatelets with epitaxially grown CdS flat branches or wings. CdS branches work as efficient photonic antenna in the blue spectral region, enhancing the excitation of CdSe band edge emission. The formation of CdSe-CdS nanoheteroplatelets instead of CdSe/CdS core-shell nanoplatelets was achieved using short-chain Cd ethylhexanoate and sulfur in octadecene as precursors for CdS overgrowth in the presence of acetate salt.

The condensation of water on adsorbed viruses.

The wetting and dewetting behavior of biological nanostructures and to a greater degree single molecules is not well-known even though their contact with water is the basis for all biology. Here, we show that environmental electron microscopy (EM) can be applied as a means of imaging the condensation of water onto viruses. We captured the formation of submicrometer water droplets and filaments on single viral particles by environmental EM and by environmental transmission EM. The condensate structures are compatible with capillary condensation between adsorbed virus particles and with known droplet shapes on patterned surfaces. Our results confirm that such droplets exist down to <50 nm. The viruses preserved their shape after a condensation/evaporation cycle as expected from their stability in air and water. Moreover we developed procedures that overcome problems of beam damage and of resolving structures with a low atomic number.

Synthesis of triazole-linked oligonucleotides with high affinity to DNA complements and an analysis of their compatibility with biosystems.

New oligonucleotide analogues with triazole internucleotide linkages were synthesized, and their hybridization properties were studied. The analogues demonstrated DNA binding affinities similar to those of unmodified oligonucleotides. The modification was shown to protect the oligonucleotides from nuclease hydrolysis. The modified oligonucleotides were tested as PCR primers. Modifications remote from the 3'-terminus were tolerated by polymerases. Our results suggest that these new oligonucleotide analogues are among the most promising triazole DNA mimics characterized to date.

The mechanism of {113} defect formation in silicon: clustering of interstitial-vacancy pairs studied by in situ high-resolution electron microscope irradiation.

We report the direct visualization of point defect clustering in {113} planes of silicon crystal using a transmission electron microscope, which was supported by structural modeling and high-resolution electron microscope image simulations. In the initial stage an accumulation of nonbonded interstitial-vacancy (I-V) pairs stacked at a distance of 7.68 Å along neighboring atomic chains located on the {113} plane takes place. Further broadening of the {113} defect across its plane is due to the formation of planar fourfold coordinated defects (FFCDs) perpendicular to chains accumulating I-V pairs. Closely packed FFCDs create a sequence of eightfold rings in the {113} plane, providing sites for additional interstitials. As a result, the perfect interstitial chains are built on the {113} plane to create an equilibrium structure. Self-ordering of point defects driven by their nonisotropic strain fields is assumed to be the main force for point defect clustering in the {113} plane under the existence of an energy barrier for their recombination.