Unconventional magnetoresistance and resistivity scaling in amorphous CoSi thin films.

The resistivity scaling of Cu electrical interconnects represents a critical challenge in Si CMOS technology. As interconnect dimensions reach below 10 nm, Cu resistivity increases significantly due to surface scattering. Topological materials have been considered for application in ultra-scaled interconnects (below 5 nm), due to their topologically protected surface states that have reduced electron scattering. Recent theoretical work on the topological chiral semimetal CoSi suggests that this material could offer lower resistivity than Cu at dimensions smaller than 10 nm. Here we investigate the scaling trend of textured and amorphous CoSi thin films, deposited by molecular beam epitaxy in a thickness range between 2 and 82.5 nm. Contrary to predictions of standard resistivity models, we report here a reduction in resistivity for thin amorphous CoSi films, which is instead consistent with surface-dominated transport. Moreover, magnetotransport measurements reveal significant enhancement of the magnetoresistance in scaled films, highlighting the complex transport mechanisms present in these highly disordered films at thicknesses of a few nanometers.

Intrinsic negative magnetoresistance from the chiral anomaly of multifold fermions.

The chiral anomaly - a hallmark of chiral spin-1/2 Weyl fermions - is an imbalance between left- and right-moving particles that underpins phenomena such as particle decay and negative longitudinal magnetoresistance in Weyl semimetals. The discovery that chiral crystals can host higher-spin generalizations of Weyl quasiparticles without high-energy counterparts, known as multifold fermions, raises the fundamental question of whether the chiral anomaly is a more general phenomenon. Answering this question requires materials with chiral quasiparticles within a sizable energy window around the Fermi level that are unaffected by extrinsic effects such as current jetting. Here, we report the chiral anomaly of multifold fermions in CoSi, which features multifold bands within ~0.85 eV of the Fermi level. By excluding current jetting through the squeezing test, we measure an intrinsic, longitudinal negative magnetoresistance. We develop a semiclassical theory to show that the negative magnetoresistance originates in the chiral anomaly, despite a sizable and detrimental orbital magnetic moment contribution. A concomitant non-linear Hall effect supports the multifold-fermion origin of the magnetotransport. Our work confirms the chiral anomaly of higher-spin generalizations of Weyl fermions, currently inaccessible outside solid-state platforms.

Highly reproducible and CMOS-compatible VO2-based oscillators for brain-inspired computing.

With remarkable electrical and optical switching properties induced at low power and near room temperature (68 °C), vanadium dioxide (VO2) has sparked rising interest in unconventional computing among the phase-change materials research community. The scalability and the potential to compute beyond the von Neumann model make VO2 especially appealing for implementation in oscillating neural networks for artificial intelligence applications, to solve constraint satisfaction problems, and for pattern recognition. Its integration into large networks of oscillators on a Silicon platform still poses challenges associated with the stabilization in the correct oxidation state and the ability to fabricate a structure with predictable electrical behavior showing very low variability. In this work, the role played by the different annealing parameters applied by three methods (slow thermal annealing, flash annealing, and rapid thermal annealing), following the vanadium oxide atomic layer deposition, on the formation of VO2 grains is studied and an optimal substrate stack configuration that minimizes variability between devices is proposed. Material and electrical characterizations are performed on the different films and a step-by-step recipe to build reproducible VO2-based oscillators is presented, which is argued to be made possible thanks to the introduction of a hafnium oxide (HfO2) layer between the silicon substrate and the vanadium oxide layer. Up to seven nearly identical VO2-based devices are contacted simultaneously to create a network of oscillators, paving the way for large-scale implementation of VO2 oscillating neural networks.

Magnetoresistive-coupled transistor using the Weyl semimetal NbP.

Semiconductor transistors operate by modulating the charge carrier concentration of a channel material through an electric field coupled by a capacitor. This mechanism is constrained by the fundamental transport physics and material properties of such devices-attenuation of the electric field, and limited mobility and charge carrier density in semiconductor channels. In this work, we demonstrate a new type of transistor that operates through a different mechanism. The channel material is a Weyl semimetal, NbP, whose resistivity is modulated via a magnetic field generated by an integrated superconductor. Due to the exceptionally large electron mobility of this material, which reaches over 1,000,000 cm2/Vs, and the strong magnetoresistive coupling, the transistor can generate significant transconductance amplification at nanowatt levels of power. This type of device can enable new low-power amplifiers, suitable for qubit readout operation in quantum computers.

Full thermoelectric characterization of a single molecule.

Molecules are predicted to be chemically tunable towards high thermoelectric efficiencies and they could outperform existing materials in the field of energy conversion. However, their capabilities at the more technologically relevant temperature of 300 K are yet to be demonstrated. A possible reason could be the lack of a comprehensive technique able to measure the thermal and (thermo)electrical properties, including the role of phonon conduction. Here, by combining the break junction technique with a suspended heat-flux sensor, we measured the total thermal and electrical conductance of a single molecule, at room temperature, together with its Seebeck coefficient. We used this method to extract the figure of merit zT of a tailor-made oligo(phenyleneethynylene)-9,10-anthracenyl molecule with dihydrobenzo[b]thiophene anchoring groups (DHBT-OPE3-An), bridged between gold electrodes. The result is in excellent agreement with predictions from density functional theory and molecular dynamics. This work represents the first measurement, within the same setup, of experimental zT of a single molecule at room temperature and opens new opportunities for the screening of several possible molecules in the light of future thermoelectric applications. The protocol is verified using SAc-OPE3, for which individual measurements for its transport properties exist in the literature.

Disorder-Induced Magnetotransport Anomalies in Amorphous and Textured Co1-xSix Semimetal Thin Films.

In recent times the chiral semimetal cobalt monosilicide (CoSi) has emerged as a prototypical, nearly ideal topological conductor hosting giant, topologically protected Fermi arcs. Exotic topological quantum properties have already been identified in CoSi bulk single crystals. However, CoSi is also known for being prone to intrinsic disorder and inhomogeneities, which, despite topological protection, risk jeopardizing its topological transport features. Alternatively, topology may be stabilized by disorder, suggesting the tantalizing possibility of an amorphous variant of a topological metal, yet to be discovered. In this respect, understanding how microstructure and stoichiometry affect magnetotransport properties is of pivotal importance, particularly in case of low-dimensional CoSi thin films and devices. Here we comprehensively investigate the magnetotransport and magnetic properties of ≈25 nm Co1-xSix thin films grown on a MgO substrate with controlled film microstructure (amorphous vs textured) and chemical composition (0.40 < x < 0.60). The resistivity of Co1-xSix thin films is nearly insensitive to the film microstructure and displays a progressive evolution from metallic-like (dρxx/dT > 0) to semiconducting-like (dρxx/dT < 0) regimes of conduction upon increasing the silicon content. A variety of anomalies in the magnetotransport properties, comprising for instance signatures consistent with quantum localization and electron-electron interactions, anomalous Hall and Kondo effects, and the occurrence of magnetic exchange interactions, are attributable to the prominent influence of intrinsic structural and chemical disorder. Our systematic survey brings to attention the complexity and the challenges involved in the prospective exploitation of the topological chiral semimetal CoSi in nanoscale thin films and devices.

Molecular electronic refrigeration against parallel phonon heat leakage channels.

Due to their structured density of states, molecular junctions provide rich resources to filter and control the flow of electrons and phonons. Here we compute the out of equilibrium current-voltage characteristics and dissipated heat of some recently synthesized oligophenylenes (OPE3) using the Density Functional based Tight-Binding (DFTB) method within Non-Equilibrium Green's Function Theory (NEGF). We analyze the Peltier cooling power for these molecular junctions as function of a bias voltage and investigate the parameters that lead to optimal cooling performance. In order to quantify the attainable temperature reduction, an electro-thermal circuit model is presented, in which the key electronic and thermal transport parameters enter. Overall, our results demonstrate that the studied OPE3 devices are compatible with temperature reductions of several K. Based on the results, some strategies to enable high performance devices for cooling applications are briefly discussed.

Thermal Simulation and Experimental Analysis of Optically Pumped InP-on-Si Micro- and Nanocavity Lasers.

There is a general trend of downscaling laser cavities, but with high integration and energy densities of nanocavity lasers, significant thermal issues affect their operation. The complexity of geometrical parameters and the various materials involved hinder the extraction of clear design guidelines and operation strategies. Here, we present a systematic thermal analysis of InP-on-Si micro- and nanocavity lasers based on steady-state and transient thermal simulations and experimental analysis. In particular, we investigate the use of metal cavities for improving the thermal properties of InP-on-Si micro- and nanocavity lasers. Heating of lasers is studied by using Raman thermometry and the results agree well with simulation results, both revealing a temperature reduction of hundreds of kelvins for the metal-clad cavity. Transient simulations are carried out to improve our understanding of the dynamic temperature variation under pulsed and continuous wave pumping conditions. The results show that the presence of a metal cladding not only increases the overall efficiency in heat dissipation but also causes a much faster temperature response. Together with optical experimental results under pulsed pumping, we conclude that a pulse width of 10 ns and a repetition rate of 100 kHz is the optimal pumping condition for a 2 µm wide square cavity.

Waveguide coupled III-V photodiodes monolithically integrated on Si.

The seamless integration of III-V nanostructures on silicon is a long-standing goal and an important step towards integrated optical links. In the present work, we demonstrate scaled and waveguide coupled III-V photodiodes monolithically integrated on Si, implemented as InP/In0.5Ga0.5As/InP p-i-n heterostructures. The waveguide coupled devices show a dark current down to 0.048 A/cm2 at -1 V and a responsivity up to 0.2 A/W at -2 V. Using grating couplers centered around 1320 nm, we demonstrate high-speed detection with a cutoff frequency f3dB exceeding 70 GHz and data reception at 50 GBd with OOK and 4PAM. When operated in forward bias as a light emitting diode, the devices emit light centered at 1550 nm. Furthermore, we also investigate the self-heating of the devices using scanning thermal microscopy and find a temperature increase of only ~15 K during the device operation as emitter, in accordance with thermal simulation results.

Sondheimer oscillations as a probe of non-ohmic flow in WP2 crystals.

As conductors in electronic applications shrink, microscopic conduction processes lead to strong deviations from Ohm's law. Depending on the length scales of momentum conserving (lMC) and relaxing (lMR) electron scattering, and the device size (d), current flows may shift from ohmic to ballistic to hydrodynamic regimes. So far, an in situ methodology to obtain these parameters within a micro/nanodevice is critically lacking. In this context, we exploit Sondheimer oscillations, semi-classical magnetoresistance oscillations due to helical electronic motion, as a method to obtain lMR even when lMR ≫ d. We extract lMR from the Sondheimer amplitude in WP2, at temperatures up to T ~ 40 K, a range most relevant for hydrodynamic transport phenomena. Our data on µm-sized devices are in excellent agreement with experimental reports of the bulk lMR and confirm that WP2 can be microfabricated without degradation. These results conclusively establish Sondheimer oscillations as a quantitative probe of lMR in micro-devices.

Coupled VO2 Oscillators Circuit as Analog First Layer Filter in Convolutional Neural Networks.

In this work we present an in-memory computing platform based on coupled VO2 oscillators fabricated in a crossbar configuration on silicon. Compared to existing platforms, the crossbar configuration promises significant improvements in terms of area density and oscillation frequency. Further, the crossbar devices exhibit low variability and extended reliability, hence, enabling experiments on 4-coupled oscillator. We demonstrate the neuromorphic computing capabilities using the phase relation of the oscillators. As an application, we propose to replace digital filtering operation in a convolutional neural network with oscillating circuits. The concept is tested with a VGG13 architecture on the MNIST dataset, achieving performances of 95% in the recognition task.

Correction: Electronic conductance and thermopower of single-molecule junctions of oligo(phenyleneethynylene) derivatives.

Correction for 'Electronic conductance and thermopower of single-molecule junctions of oligo(phenyleneethynylene) derivatives' by Hervé Dekkiche et al., Nanoscale, 2020, 12, 18908-18917, DOI: 10.1039/D0NR04413J.

Ultra-stable dry cryostat for variable temperature break junction.

We present the design of a variable temperature setup that uses a pulse tube cryocooler to perform break-junction experiments at variable temperatures ranging from 12 K to room temperature. The use of pulse tube coolers is advantageous because they are easy to use, can be highly automatized, and used to avoid wastage of cryogenic fluids. This is the reason why dry cryostats are conquering more and more fields in cryogenic physics. However, the main drawback is the level of vibration that can be up to several micrometers at the cold-head. The vibrations make the operation of scanning probe-based microscopes challenging. We implemented vibration-damping techniques that allow obtaining a vibration level of 12 pm between the tip and sample. With these adaptations, we show the possibility to perform break junction measurements in a cryogenic environment and keep in place atomic chains of a few nanometers between the two electrodes.

Spatially resolved thermoelectric effects in operando semiconductor-metal nanowire heterostructures.

The thermoelectric properties of a nanoscale germanium segment connected by aluminium nanowires are studied using scanning thermal microscopy. The germanium segment of 168 nm length features atomically sharp interfaces to the aluminium wires and is surrounded by an Al2O3 shell. The temperature distribution along the self-heated nanowire is measured as a function of the applied electrical current, for both Joule and Peltier effects. An analysis is developed that is able to extract the thermal and thermoelectric properties including thermal conductivity, the thermal boundary resistance to the substrate and the Peltier coefficient from a single measurement. Our investigations demonstrate the potential of quantitative measurements of temperature around self-heated devices and structures down to the scattering length of heat carriers.

Electronic conductance and thermopower of single-molecule junctions of oligo(phenyleneethynylene) derivatives.

We report the synthesis and the single-molecule transport properties of three new oligo(phenyleneethynylene) (OPE3) derivatives possessing terminal dihydrobenzo[b]thiophene (DHBT) anchoring groups and various core substituents (phenylene, 2,5-dimethoxyphenylene and 9,10-anthracenyl). Their electronic conductance and their Seebeck coefficient have been determined using scanning tunneling microscopy-based break junction (STM-BJ) experiments between gold electrodes. The transport properties of the molecular junctions have been modelled using DFT-based computational methods which reveal a specific binding of the sulfur atom of the DHBT anchor to the electrodes. The experimentally determined Seebeck coefficient varies between -7.9 and -11.4 µV K-1 in the series and the negative sign is consistent with charge transport through the LUMO levels of the molecules.

Author Correction: Topological matter: Shrewd detectives find a dissipation channel.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Thermal Transport through Single-Molecule Junctions.

Molecular junctions exhibit a rich and tunable set of thermal transport phenomena. However, the predicted high thermoelectric efficiencies, phonon quantum interference effects, rectification, and nonlinear heat transport properties of organic molecules are yet to be verified because suitable experimental techniques have been missing. Here, by combining the break junction technique with suspended heat-flux sensors with picowatt per Kelvin sensitivity, we measured the thermal and electrical conductance of single organic molecules at room temperature simultaneously. We used this method to study the thermal transport properties of two model systems, namely, dithiol-oligo(phenylene ethynylene) and octane dithiol junctions with gold electrodes. In agreement with our density functional theory and phase-coherent transport calculations, we show that heat transport across these systems is governed by the phonon mismatch between the molecules and the metallic electrodes. This work represents the first measurement of thermal transport through single molecules and opens new opportunities for studying heat management at the nanoscale level.

Combined scanning probe electronic and thermal characterization of an indium arsenide nanowire.

As electronic devices are downsized, physical processes at the interface to electrodes may dominate and limit device performance. A crucial step towards device optimization is being able to separate such contact effects from intrinsic device properties. Likewise, an increased local temperature due to Joule heating at contacts and the formation of hot spots may put limits on device integration. Therefore, being able to observe profiles of both electronic and thermal device properties at the nanoscale is important. Here, we show measurements by scanning thermal and Kelvin probe force microscopy of the same 60 nm diameter indium arsenide nanowire in operation. The observed temperature along the wire is substantially elevated near the contacts and deviates from the bell-shaped temperature profile one would expect from homogeneous heating. Voltage profiles acquired by Kelvin probe force microscopy not only allow us to determine the electrical nanowire conductivity, but also to identify and quantify sizable and non-linear contact resistances at the buried nanowire-electrode interfaces. Complementing these data with thermal measurements, we obtain a device model further permitting separate extraction of the local thermal nanowire and interface conductivities.