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Pascal Gehring

Publications and source records attributed to Pascal Gehring.

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Direct Mapping of Local Seebeck Coefficient in 2D Material Nanostructures via Scanning Thermal Gate Microscopy

Local variations in the Seebeck coefficient in low-dimensional materials-based nanostructures and devices play a major role in their thermoelectric performance. Unfortunately, currently most thermoelectric measurements probe the aggregate characteristics of the device as a whole, failing to observe the effects of the local variations and internal structure. Such variations can be caused by local defects, geometry, electrical contacts or interfaces and often substantially influence thermoelectric properties, most profoundly in two-dimensional (2D) materials. Here, we use Scanning Thermal Gate Microscopy (STGM), a non-invasive method not requiring an electrical contact between the nanoscale tip and the probed sample, to obtain nanoscale resolution 2D maps of the thermovoltage in graphene samples. We investigate a junction formed between single-layer and bilayer graphene and identify the impact of internal strain and Fermi level pinning by the contacts using a deconvolution method to directly map the local Seebeck coefficient. The new approach paves the way for an in-depth understanding of thermoelectric behaviour and phenomena in 2D materials nanostructures and devices.

cond-mat.mes-hall

Single-Material Graphene Thermocouples

On-chip temperature sensing on a micro- to nanometer scale is becoming more desirable as the complexity of nanodevices and size requirements increase and with it the challenges in thermal probing and management. This highlights the need for scalable and reliable temperature sensors which have the potential to be incorporated into current and future device structures. Here, we show that U-shaped graphene stripes consisting of one wide and one narrow leg form a single material thermocouple that can function as a self-powering temperature sensor. We find that the graphene thermocouples increase in sensitivity with a decrease in leg width, due to a change in the Seebeck coefficient, which is in agreement with our previous findings and report a maximum sensitivity of $ΔS \approx$ 39 $\mathrmμ$V/K.

physics.app-ph

A Mechanically Tunable Quantum Dot in a Graphene Break Junction

Graphene quantum dots (QDs) are intensively studied as platforms for the next generation of quantum electronic devices. Fine tuning of the transport properties in monolayer graphene QDs, in particular with respect to the independent modulation of the tunnel barrier transparencies, remains challenging and is typically addressed using electrostatic gating. We investigate charge transport in back-gated graphene mechanical break junctions and reveal Coulomb blockade physics characteristic of a single, high-quality QD when a nanogap is opened in a graphene constriction. By mechanically controlling the distance across the newly-formed graphene nanogap, we achieve reversible tunability of the tunnel coupling to the drain electrode by five orders of magnitude, while keeping the source-QD tunnel coupling constant. These findings indicate that the tunnel coupling asymmetry can be significantly modulated with a mechanical tuning knob and has important implications for the development of future graphene-based devices, including energy converters and quantum calorimeters.

cond-mat.mes-hall

Efficient heating of single-molecule junctions for thermoelectric studies at cryogenic temperatures

The energy dependent thermoelectric response of a single molecule contains valuable information about its transmission function and its excited states. However, measuring it requires devices that can efficiently heat up one side of the molecule while being able to tune its electrochemical potential over a wide energy range. Furthermore, to increase junction stability devices need to operate at cryogenic temperatures. In this work we report on a new device architecture to study the thermoelectric properties and the conductance of single molecules simultaneously over a wide energy range. We employ a sample heater in direct contact with the metallic electrodes contacting the single molecule which allows us to apply temperature biases up to $ΔT = 60$K with minimal heating of the molecular junction. This makes these devices compatible with base temperatures $T_\mathrm{bath} <2$K and enables studies in the linear ($ΔT \ll T_\mathrm{molecule}$) and non-linear ($ΔT \gg T_\mathrm{molecule}$) thermoelectric transport regimes.

cond-mat.mes-hall

Tunneling spectroscopy of localized states of $\mathrm{WS}_2$ barriers in vertical van der Waals heterostructures

In transition metal dichalcogenides, defects have been found to play an important role, affecting doping, spin-valley relaxation dynamics, and assisting in proximity effects of spin-orbit coupling. Here, we study localized states in $\mathrm{WS}_2$ and how they affect tunneling through van der Waals heterostructures of h-BN/graphene/$\mathrm{WS}_2$/metal. The obtained conductance maps as a function of bias and gate voltage reveal single-electron transistor behavior (Coulomb blockade) with a rich set of transport features including excited states and negative differential resistance regimes. Applying a perpendicular magnetic field, we observe a shift in the energies of the quantum levels and information about the orbital magnetic moment of the localized states is extracted.

cond-mat.mes-hall

The role of metallic leads and electronic degeneracies in thermoelectric power generation in quantum dots

The power factor of a thermoelectric device is a measure of the heat-to-energy conversion efficiency in nanoscopic devices. Yet, even as interest in low-dimensional thermoelectric materials has increased, experimental research on what influences the power factor in these systems is scarce. Here, we present a detailed thermoelectric study of graphene quantum dot devices. We show that spin-degeneracy of the quantum dot states has a significant impact on the zero-bias conductance of the device and leads to an increase of the power factor. Conversely, we demonstrate that non-ideal heat exchange within the leads can suppress the power factor near the charge degeneracy point and non-trivially influences its temperature dependence.

cond-mat.mes-hall

Ground-state spin blockade in a single-molecule junction

It is known that the quantum-mechanical ground state of a nano-scale junction has a significant impact on its electrical transport properties. This becomes particularly important in transistors consisting of a single molecule. Due to strong electron-electron interactions and the possibility to access ground states with high spins, these systems are eligible hosts of a current-blockade phenomenon called ground-state spin blockade. This effect arises from the inability of a charge carrier to account for the spin difference required to enter the junction, as that process would violate the spin selection rules. Here, we present a direct experimental demonstration of ground-state spin blockade in a high-spin single-molecule transistor. The measured transport characteristics of this device exhibit a complete suppression of resonant transport due to a ground-state spin difference of 3/2 between subsequent charge states. Strikingly, the blockade can be reversibly lifted by driving the system through a magnetic ground-state transition in one charge state, using the tunability offered by both magnetic and electric fields.

cond-mat.mes-hall

Geometrically Enhanced Thermoelectric Effects in Graphene Nanoconstrictions

The influence of nanostructuring and quantum confinement on the thermoelectric properties of materials has been extensively studied. While this has made possible multiple breakthroughs in the achievable figure of merit, classical confinement, and its effect on the local Seebeck coefficient has mostly been neglected, as has the Peltier effect in general due to the complexity of measuring small temperature gradients locally. Here we report that reducing the width of a graphene channel to 100 nm changes the Seebeck coefficient by orders of magnitude. Using a scanning thermal microscope allows us to probe the local temperature of electrically contacted graphene two-terminal devices or to locally heat the sample. We show that constrictions in mono- and bilayer graphene facilitate a spatially correlated gradient in the Seebeck and Peltier coefficient, as evidenced by the pronounced thermovoltage $V_{th}$ and heating/cooling response $ΔT_{Peltier}$, respectively. This geometry dependent effect, which has not been reported previously in 2D materials, has important implications for measurements of patterned nanostructures in graphene and points to novel solutions for effective thermal management in electronic graphene devices or concepts for single material thermocouples.

cond-mat.mes-hall

Mechanically Controlled Quantum Interference in Graphene Break Junctions

The ability to detect and distinguish quantum interference signatures is important for both fundamental research and for the realization of devices including electron resonators, interferometers and interference-based spin filters. Consistent with the principles of subwavelength optics, the wave nature of electrons can give rise to various types of interference effects, such as Fabry-Pérot resonances, Fano resonances and the Aharonov-Bohm effect. Quantum-interference conductance oscillations have indeed been predicted for multiwall carbon nanotube shuttles and telescopes, and arise from atomic-scale displacements between the inner and outer tubes. Previous theoretical work on graphene bilayers indicates that these systems may display similar interference features as a function of the relative position of the two sheets. Experimental verification is, however, still lacking. Graphene nanoconstrictions represent an ideal model system to study quantum transport phenomena due to the electronic coherence and the transverse confinement of the carriers. Here, we demonstrate the fabrication of bowtie-shaped nanoconstrictions with mechanically controlled break junctions (MCBJs) made from a single layer of graphene. We find that their electrical conductance displays pronounced oscillations at room temperature, with amplitudes that modulate over an order of magnitude as a function of sub-nanometer displacements. Surprisingly, the oscillations exhibit a period larger than the graphene lattice constant. Charge-transport calculations show that the periodicity originates from a combination of quantum-interference and lattice-commensuration effects of two graphene layers that slide across each other. Our results provide direct experimental observation of Fabry-Pérot-like interference of electron waves that are partially reflected/transmitted at the edges of the graphene bilayer overlap region.

cond-mat.mes-hall

Massively parallel fabrication of crack-defined gold break junctions featuring sub-3 nm gaps for molecular devices

Break junctions provide tip-shaped contact electrodes that are fundamental components of nano and molecular electronics. However, the fabrication of break junctions remains notoriously time-consuming and difficult to parallelize. Here we demonstrate true parallel fabrication of gold break junctions featuring sub-3 nm gaps on the wafer-scale, by relying on a novel self-breaking mechanism based on controlled crack formation in notched bridge structures. We achieve fabrication densities as high as 7 million junctions per cm$^{2}$, with fabrication yields of around 7% for obtaining crack-defined break junctions with sub-3 nm gaps of fixed gap width that exhibit electron tunneling. We also form molecular junctions using dithiol-terminated oligo(phenylene ethynylene) (OPE3) to demonstrate the feasibility of our approach for electrical probing of molecules down to liquid helium temperatures. Our technology opens a whole new range of experimental opportunities for nano and molecular electronics applications, by enabling very large-scale fabrication of solid-state break junctions.

physics.app-ph

Field-Effect Control of Graphene-Fullerene Thermoelectric Nanodevices

Although it was demonstrated that discrete molecular levels determine the sign and magnitude of the thermoelectric effect in single-molecule junctions, full electrostatic control of these levels has not been achieved to date. Here, we show that graphene nanogaps combined with gold microheaters serve as a testbed for studying single-molecule thermoelectricity. Reduced screening of the gate electric field compared to conventional metal electrodes allows control of the position of the dominant transport orbital by hundreds of meV. We find that the power factor of graphene-fullerene junctions can be tuned over several orders of magnitude to a value close to the theoretical limit of an isolated Breit-Wigner resonance. Furthermore, our data suggest that the power factor of an isolated level is only given by the tunnel coupling to the leads and temperature. These results open up new avenues for exploring thermoelectricity and charge transport in individual molecules and highlight the importance of level alignment and coupling to the electrodes for optimum energy conversion in organic thermoelectric materials.

cond-mat.mes-hall

Scaling limits of graphene nanoelectrodes

Graphene is an ideal material for fabricating atomically thin nanometre spaced electrodes. Recently, carbon-based nanoelectrodes have been employed to create single-molecule transistors and phase change memory devices. In spite of the significant recent interest in their use in a range of nanoscale devices from phase change memories to molecular electronics, the operating and scaling limits of these electrodes are completely unknown. In this paper, we report on our observations of consistent voltage driven resistance switching in sub-5 nm graphene nanogaps. We find that we are able to reversibly cycle between a low and a high resistance state using feedback-controlled voltage ramps.We attribute this unexplained switching in the gap to the formation and breakdown of carbon filaments.By increasing the gap, we find that such intrinsic resistance switching of graphene nanogaps imposes a scaling limit of 10 nm (approx.) on the gap-size for devices with operating voltages of 1 to 2 volts.

cond-mat.mes-hall

Quantum Interference in Graphene Nanoconstrictions

We report quantum interference effects in the electrical conductance of chemical vapor deposited graphene nanoconstrictions fabricated using feedback controlled electroburning. The observed multimode Fabry-Perot interferences can be attributed to reflections at potential steps inside the channel. Sharp antiresonance features with a Fano line shape are observed. Theoretical modeling reveals that these Fano resonances are due to localized states inside the constriction, which couple to the delocalized states that also give rise to the Fabry-Perot interference patterns. This study provides new insight into the interplay between two fundamental forms of quantum interference in graphene nanoconstrictions.

cond-mat.mes-hall

Three-terminal graphene single-electron transistor fabricated using feedback-controlled electroburning

We report room-temperature Coulomb blockade in a single layer graphene three-terminal single-electron transistor (SET) fabricated using feedback-controlled electroburning. The small separation between the side gate electrode and the graphene quantum dot results in a gate coupling up to 3 times larger compared to the value found for the back gate electrode. This allows for an effective tuning between the conductive and Coulomb blocked state using a small side gate voltage of about 1V. The technique can potentially be used in the future to fabricate all-graphene based room temperature single-electron transistors or three terminal single molecule transistors with enhanced gate coupling.

cond-mat.mes-hall

A Natural Topological Insulator

The earth's crust and outer space are rich sources of technologically relevant materials which have found application in a wide range of fields. Well-established examples are diamond, one of the hardest known materials, or graphite as a suitable precursor of graphene. The ongoing drive to discover novel materials useful for (opto)electronic applications has recently drawn strong attention to topological insulators. Here, we report that Kawazulite, a mineral with the approximate composition Bi$_2$(Te,Se)$_2$(Se,S), represents a naturally occurring topological insulator whose electronic properties compete well with those of its synthetic counterparts. Kawazulite flakes with a thickness of a few tens of nanometers were prepared by mechanical exfoliation. They exhibit a low intrinsic bulk doping level and correspondingly a sizable mobility of surface state carriers of more than $1000 \text{cm}^2/(\text{V s})$ at low temperature. Based on these findings, further minerals which due to their minimized defect densities display even better electronic characteristics may be identified in the future.

cond-mat.mtrl-sci

Growth of High-Mobility Bi2Te2Se Nanoplatelets on hBN Sheets by van der Waals Epitaxy

The electrical detection of the surface states of topological insulators is strongly impeded by the interference of bulk conduction, which commonly arises due to pronounced doping associated with the formation of lattice defects. As exemplified by the topological insulator Bi2Te2Se, we show that via van der Waals epitaxial growth on thin hBN substrates the structural quality of such nanoplatelets can be substantially improved. The surface state carrier mobility of nanoplatelets on hBN is increased by a factor of about 3 compared to platelets on conventional Si/SiOx substrates, which enables the observation of well-developed Shubnikov-de Haas oscillations. We furthermore demonstrate the possibility to effectively tune the Fermi level position in the films with the aid of a back gate.

cond-mat.mtrl-sci

Two-dimensional magnetotransport in Bi2Te2Se nanoplatelets

Single-crystalline Bi2Te2Se nanoplates with thicknesses between 8 and 30 nm and lateral sizes of several micrometers were synthesized by a vapour-solid growth method. Angle-dependent magnetoconductance measurements on individual nanoplates revealed the presence of a two-dimensional weak anti-localization effect. In conjunction with gate-dependent charge transport studies performed at different temperatures, evidence was gained that this effect originates from the topologically protected surface states of the nanoplates.

cond-mat.mes-hall