Experimental signatures of the mixed axial-gravitational anomaly in the Weyl semimetal NbP.

The conservation laws, such as those of charge, energy and momentum, have a central role in physics. In some special cases, classical conservation laws are broken at the quantum level by quantum fluctuations, in which case the theory is said to have quantum anomalies. One of the most prominent examples is the chiral anomaly, which involves massless chiral fermions. These particles have their spin, or internal angular momentum, aligned either parallel or antiparallel with their linear momentum, labelled as left and right chirality, respectively. In three spatial dimensions, the chiral anomaly is the breakdown (as a result of externally applied parallel electric and magnetic fields) of the classical conservation law that dictates that the number of massless fermions of each chirality are separately conserved. The current that measures the difference between left- and right-handed particles is called the axial current and is not conserved at the quantum level. In addition, an underlying curved space-time provides a distinct contribution to a chiral imbalance, an effect known as the mixed axial-gravitational anomaly, but this anomaly has yet to be confirmed experimentally. However, the presence of a mixed gauge-gravitational anomaly has recently been tied to thermoelectrical transport in a magnetic field, even in flat space-time, suggesting that such types of mixed anomaly could be experimentally probed in condensed matter systems known as Weyl semimetals. Here, using a temperature gradient, we observe experimentally a positive magneto-thermoelectric conductance in the Weyl semimetal niobium phosphide (NbP) for collinear temperature gradients and magnetic fields that vanishes in the ultra-quantum limit, when only a single Landau level is occupied. This observation is consistent with the presence of a mixed axial-gravitational anomaly, providing clear evidence for a theoretical concept that has so far eluded experimental detection.

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.

Nanoelectrical analysis of single molecules and atomic-scale materials at the solid/liquid interface.

Evaluating the built-in functionality of nanomaterials under practical conditions is central for their proposed integration as active components in next-generation electronics. Low-dimensional materials from single atoms to molecules have been consistently resolved and manipulated under ultrahigh vacuum at low temperatures. At room temperature, atomic-scale imaging has also been performed by probing materials at the solid/liquid interface. We exploit this electrical interface to develop a robust electronic decoupling platform that provides precise information on molecular energy levels recorded using in situ scanning tunnelling microscopy/spectroscopy with high spatial and energy resolution in a high-density liquid environment. Our experimental findings, supported by ab initio electronic structure calculations and atomic-scale molecular dynamics simulations, reveal direct mapping of single-molecule structure and resonance states at the solid/liquid interface. We further extend this approach to resolve the electronic structure of graphene monolayers at atomic length scales under standard room-temperature operating conditions.

ß-Relaxation of PMMA: Tip Size and Stress Effects in Friction Force Microscopy.

The kinetic signature of the ß-relaxation of poly(methyl methacrylate) (PMMA) is investigated by friction force microscopy. The variation in friction force was measured as a function of scan velocity, temperature (300 K-410 K), and applied load using both sharp and blunt probe tips. The friction data show distinct maxima, which can be ascribed to the ß-relaxation of PMMA. The contact area was varied over the ranges of approximately 20 to 70 nm(2) and 12,000 to 43,000 nm(2) through the use of probe tips with radii of approximately 15, 18, 1350, and 2650 nm. Kinetic analysis shows that the apparent activation energy of the ß-relaxation decreases with the tip radius. Accompanying finite element simulations indicate that for the sharp tips a substantial subvolume of the polymer underneath the tip exceeds the yield stress of PMMA. This suggests that for small contact sizes and high stresses the activation barrier of the ß-process decreases through the activation of the α-process by material yielding.

Frictional dissipation in a polymer bilayer system.

Sliding friction between a silicon tip and a polymer bilayer system consisting of a polystyrene (PS) film covered with a few-nanometers-thick capping layer of hard plasma polymer is studied using friction force microscopy. The system was chosen to enable subsurface dissipation channels to be distinguished from surface friction. Frictional energy dissipation in the underlayer can be identified through the kinetics of the polymer relaxation modes that we measured using nanoscale friction experiments as a function of sample temperature, scanning velocity, and applied load. We found a strong nonlinear increase in friction as a function of applied load around the glass-transition temperature of the PS underlayer. This behavior is a clear signature of frictional dissipation occurring in the volume of the polystyrene layer, well below the surface of the sample. The time-temperature kinetics associated with frictional energy dissipation into the PS was found to be in agreement with the known material properties of PS. Moreover, the data was found to support the hypothesis that the observed friction can be understood as the sum of friction resulting from the relaxation process in the polymer underlayer induced by stress due to the sliding of the tip and a second term associated with dissipation due to sliding friction on the capping layer.

Tuning the light emission from GaAs nanowires over 290 meV with uniaxial strain.

Strain engineering has been used to increase the charge carrier mobility of complementary metal-oxide-semiconductor transistors as well as to boost and tune the performance of optoelectronic devices, enabling wavelength tuning, polarization selectivity and suppression of temperature drifts. Semiconducting nanowires benefit from enhanced mechanical properties, such as increased yield strength, that turn out to be beneficial to amplify strain effects. Here we use photoluminescence (PL) to study the effect of uniaxial stress on the electronic properties of GaAs/Al0.3Ga0.7As/GaAs core/shell nanowires. Both compressive and tensile mechanical stress were applied continuously and reversibly to the nanowire, resulting in a remarkable decrease of the bandgap of up to 296 meV at 3.5% of strain. Raman spectra were measured and analyzed to determine the axial strain in the nanowire and the Poisson ratio in the <111> direction. In both PL and Raman spectra, we observe fingerprints of symmetry breaking due to anisotropic deformation of the nanowire. The shifts observed in the PL and Raman spectra are well described by bulk deformation potentials for band structure and phonon energies. The fact that exceptionally high elastic strain can be applied to semiconducting nanowires makes them ideally suited for novel device applications that require a tuning of the band structure over a broad range.

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.

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.

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.

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.

Bonding and electronic transport properties of fullerene and fullerene derivatives in break-junction geometries.

Fullerenes are considered anchoring groups for molecular electronics due to a large contact area and their affinity for noble metals. The conductances of fullerene-terminated molecules, however, are found to be even lower than for thiol termination. The effects of weak molecule-metal coupling and symmetry breaking are studied by transport measurements of C(60) and functionalized C(60). The results demonstrate highy efficient contacts between Au and C(60), despite of deposition from solution.

Thermal transport into graphene through nanoscopic contacts.

Superior thermal conductivity of graphene is frequently reported and used to justify its technical relevance for ultimately scaled devices. However, this extraordinary property is size dependent, and understanding of graphene's thermal properties in the quasiballistic thermal transport regime is lacking. To overcome this limitation, we directly probe local heat transfer into graphene by high-resolution scanning thermal microscopy on amorphous silicon oxide (SiO2) and crystalline silicon carbide (SiC). We quantify thickness-dependent thermal resistance modulations at sub-10-nm lateral resolution and thermal sensitivity for the individual atomic layers. On SiO2, we observe a decrease of thermal resistance with increasing number of graphene layers. We attribute this trend to the spreading of heat using the thickness dependence of graphene's thermal conductivity. On SiC, the heated tip-sample contact is scaled below the phonon mean free path of both the graphene and its supporting substrate. Consistently, we find the thermal interface resistances of the graphene top and bottom contacts dominating thermal transport.

Nanoscale origin of defects at metal/molecule engineered interfaces.

The control and repair of defects at metal/molecule interfaces is central to the realization of molecular electronic circuits with reproducible performance. The fundamental mechanism governing defect (pore) evolution on mica-supported metal surfaces, its propagation in self-assembled molecular layers, and its implications for molecular junction devices are discussed. Pore eradication by replacing mica with halide platforms coupled with elevated substrate temperature during metal deposition yields exceptionally ultraflat metal landscapes. In situ scanning tunneling microscopy further substantiates molecular locking at defect sites and upon defect healing; the emergence of a closely packed 2-D molecular architecture is demonstrated with nanometer-scale spatial resolution in liquids.

Quantitative thermometry of nanoscale hot spots.

A method is described to quantify thermal conductance and temperature distributions with nanoscale resolution using scanning thermal microscopy. In the first step, the thermal resistance of the tip-surface contact is measured for each point of a surface. In the second step, the local temperature is determined from the difference between the measured heat flux for heat sources switched on and off. The method is demonstrated using self-heating of silicon nanowires. While a homogeneous nanowire shows a bell-shaped temperature profile, a nanowire diode exhibits a hot spot centered near the junction between two doped segments.

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.