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Although 2D materials hold great potential for next-generation pressure sensors, recent studies revealed that gases permeate along the membrane-surface interface that is only weakly bound by van der Waals interactions, necessitating additional sealing procedures. In this work, we demonstrate the use of free-standing complex oxides as self-sealing membranes that allow the reference cavity of pressure sensors to be sealed by a simple anneal. To test the hermeticity, we study the gas permeation time constants in nano-mechanical resonators made from SrRuO3 and SrTiO3 membranes suspended over SiO2/Si cavities which show an improvement up to 4 orders of magnitude in the permeation time constant after annealing the devices for 15 minutes. Similar devices fabricated on Si3N4/Si do not show such improvements, suggesting that the adhesion increase over SiO2 is mediated by oxygen bonds that are formed at the SiO2/complex oxide interface during the self-sealing anneal. We confirm the enhancement of adhesion by picosecond ultrasonics measurements which show an increase in the interfacial stiffness by 70% after annealing. Since it is straigthforward to apply, the presented self-sealing method is thus a promising route toward realizing ultrathin hermetic pressure sensors., 7 pages, 5 figures

Microphones exploit the motion of suspended membranes to detect sound waves. Since the microphone performance can be improved by reducing the thickness and mass of its sensing membrane, graphene-based microphones are expected to outperform state-of-the-art microelectromechanical (MEMS) microphones and allow further miniaturization of the device. Here, we present a laser vibrometry study of the acoustic response of suspended multilayer graphene membranes for microphone applications. We address performance parameters relevant for acoustic sensing, including mechanical sensitivity, limit of detection and nonlinear distortion, and discuss the trade-offs and limitations in the design of graphene microphones. We demonstrate superior mechanical sensitivities of the graphene membranes, reaching more than 2 orders of magnitude higher compliances than commercial MEMS devices, and report a limit of detection as low as 15 dBSPL, which is 10-15 dB lower than that featured by current MEMS microphones.

Creating a good contact between electrodes and graphene nanoribbons (GNRs) has been a long-standing challenge in searching for the next GNR-based nanoelectronics. This quest requires the controlled fabrication of sub-20 nm metallic gaps, a clean GNR transfer minimizing damage and organic contamination during the device fabrication, as well as work function matching to minimize the contact resistance. Here, we transfer 9-atom-wide armchair-edged GNRs (9-AGNRs) grown on Au(111)/mica substrates to pre-patterned platinum electrodes, yielding polymer-free 9-AGNR field-effect transistor devices. Our devices have a resistance in the range of 106-108 Ω in the low-bias regime, which is 2-4 orders of magnitude lower than previous reports. Density functional theory calculations combined with the non-equilibrium Green's function method explain the observed p-type electrical characteristics and further demonstrate that platinum gives strong coupling and higher transmission in comparison to other materials, such as graphene., Applied Physics Letters, 122 (17), ISSN:0003-6951, ISSN:1077-3118

Suspended piezoelectric thin films are key elements enabling high-frequency filtering in telecommunication devices. To meet the requirements of next-generation electronics, it is essential to reduce device thickness for reaching higher resonance frequencies. Here, the high-quality mechanical and electrical properties of graphene electrodes are combined with the strong piezoelectric performance of the free-standing complex oxide, BaTiO

Porphyrin cyclophane 1, consisting of two rigidly fixed but still movable cofacial porphyrins and exposing acetate-masked thiols in opposed directions of the macrocycle, is designed, synthesized, and characterized. The functional cyclophane 1, as pioneer of mechanosensitive 3D materials, forms stable single-molecule junctions in a mechanically controlled break-junction setup. Its reliable integration in a single-molecule junction is a fundamental prerequisite to explore the potential of these structures as mechanically triggered functional units and devices.

This paper describes the conductance of single-molecules and self-assembled monolayers comprising an oligophenyleneethynylene core, functionalized with acenes of increasing length that extend conjugation perpendicular to the path of tunneling electrons. In the Mechanically Controlled Break Junction (MCBJ) experiment, multiple conductance plateaus were identified. The high conductance plateau, which we attribute to the single molecule conformation, shows an increase of conductance as a function of acene length, in good agreement with theoretical predictions. The lower plateau is attributed to multiple molecules bridging the junctions with intermolecular interactions playing a role. In junctions comprising a self-assembled monolayer with eutectic Ga–In top-contacts (EGaIn), the pentacene derivative exhibits unusually low conductance, which we ascribe to the inability of these molecules to pack in a monolayer without introducing significant intermolecular contacts. This hypothesis is supported by the MCBJ data and theoretical calculations showing suppressed conductance through thePCfilms. These results highlight the role of intermolecular effects and junction geometries in the observed fluctuations of conductance values between single-molecule and ensemble junctions, and the importance of studying molecules in both platforms.

Intra- and intermolecular interactions are dominating chemical processes, and their concerted interplay enables complex nonequilibrium states like life. While the responsible basic forces are typically investigated spectroscopically, a conductance measurement to probe and control these interactions in a single molecule far out of equilibrium is reported here. Specifically, by separating macroscopic metal electrodes, two π-conjugated, bridge-connected porphyrin decks are peeled off on one side, but compressed on the other side due to the covalent mechanical fixation. We observe that the conductance response shows an exceptional exponential rise by two orders of magnitude in individual breaking events during the stretching. Theoretical studies atomistically explain the measured conductance behavior by a mechanically activated increase in through-bond transport and a simultaneous strengthening of through-space coupling. Our results not only reveal the various interacting intramolecular transport channels in a molecular set of levers, but also the molecules' potential to serve as molecular electro-mechanical sensors and switches.

The possibility to study quantum interference phenomena at ambient conditions is an appealing feature of molecular electronics. By connecting two porphyrins in a cofacial cyclophane, we create an attractive platform for mechanically controlling electric transport through the intramolecular extent of π-orbital overlap of the porphyrins facing each other and through the angle of xanthene bridges with regard to the porphyrin planes. We analyze theoretically the evolution of molecular configurations in the pulling process and the corresponding changes in electric conduction by combining density functional theory (DFT) with Landauer scattering theory of phase-coherent elastic transport. Predicted conductances during the stretching process show order of magnitude variations caused by two robust destructive quantum interference features that span through the whole electronic gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO). Mechanically-controlled break junction (MCBJ) experiments at room temperature verify the mechanosensitive response of the molecular junctions. During the continuous stretching of the molecule, they show conductance variations of up to 1.5 orders of magnitude over single breaking events. Uncommon triple-and quadruple-frequency responses are observed in periodic electrode modulation experiments with amplitudes of up to 10 Å. This further confirms the theoretically predicted double transmission dips caused by the spatial and energetic rearrangement of molecular orbitals, with contributions from both through-space and through-bond transport. This journal is

The Kagome lattice is an important fundamental structure in condensed matter physics for investigating the interplay of electron correlation, topology, and frustrated magnetism. Recent work on Kagome metals in the AV3Sb5 (A = K, Rb, and Cs) family has shown a multitude of correlation-driven distortions, including symmetry breaking charge density waves and nematic superconductivity at low temperatures. Here, we study the new Kagome metal Yb0.5Co3Ge3 and find a temperature-dependent kink in the resistivity that is highly similar to the AV3Sb5 behavior and is commensurate with an in-plane structural distortion of the Co Kagome lattice along with a doubling of the c-axis. The symmetry is lower below the transition temperature, with a breaking the in-plane mirror planes and C6 rotation, while gaining a screw axis along the c-direction. At very low temperatures, anisotropic negative magnetoresistance is observed, which may be related to anisotropic magnetism. This raises questions about the types of the distortions in Kagome nets and their resulting physical properties including superconductivity and magnetism.

Alkanes serve an important role as benchmark system in molecular electronics. However, a large variation in the conductance values is reported in the literature. To better understand these fluctuations, in this study we measure large molecular data sets (up to 100 000 breaking traces) of a series of alkanes with different lengths and anchoring groups using the mechanically controlled break junction (MCBJ) technique. Employing an unsupervised learning algorithm, we investigate both the time evolution and the distance dependence of the measured traces. For all the molecules considered, we have been able to identify the single-molecule conductance value for the fully stretched molecular configuration. For alkanedithiols, the corresponding extracted β decay constant of 1.05 ± 0.08 per CH2group agrees well with literature values. In the case of the stronger thiol bonding, additional peaks in the conductance histograms are found, suggesting the formation of molecular junctions containing a single molecule plus additional gold/molecule unit(s). The results shine light on the dispersion in reported conductance values and show that the evolution of the molecule as a function of stretching and time contains crucial information in determining the molecular junction configuration in MCBJs.

Spin-crossover (SCO) active iron(II) complexes are an integral class of switchable and bistable molecular materials. Spin-state switching properties of the SCO complexes have been studied in the bulk and single-molecule levels to progress toward fabricating molecule-based switching and memory elements. Supramolecular SCO complexes featuring anchoring groups for metallic electrodes, for example, gold (Au), are ideal candidates to study spin-state switching at the single-molecule level. In this study, we report on the spin-state switching characteristics of supramolecular iron(II) complexes

We demonstrate charge detection with single-electron resolution at high readout frequency using a silicon field-effect transistor (FET) integrated with double resonant circuits. A FET, whose channel of 10-nm width enables a single electron to be detected at room temperature, is connected to resonant circuits composed of coupled inductors and capacitors, and these double resonant circuits provide two resonance frequencies. When the FET is driven by a carrier signal at the lower resonance frequency, a small signal applied to the FET's gate modulates the resonance condition, resulting in a reflected signal appearing near the higher resonance frequency. Such operation utilizing the double resonant circuits enables charge detection with a single-electron resolution of 3 × 10−3 e/Hz0.5 and a readout frequency of 200 MHz at room temperature. In addition, a variable capacitor used in the double resonant circuits allows charge-sensing characteristics to be controlled in situ.

Biological electron transport is classically thought to occur over nanometre distances, yet recent studies suggest that electrical currents can run along centimetre-long cable bacteria. The phenomenon remains elusive, however, as currents have not been directly measured, nor have the conductive structures been identified. Here we demonstrate that cable bacteria conduct electrons over centimetre distances via highly conductive fibres embedded in the cell envelope. Direct electrode measurements reveal nanoampere currents in intact filaments up to 10.1 mm long (>2000 adjacent cells). A network of parallel periplasmic fibres displays a high conductivity (up to 79 S cm−1), explaining currents measured through intact filaments. Conductance rapidly declines upon exposure to air, but remains stable under vacuum, demonstrating that charge transfer is electronic rather than ionic. Our finding of a biological structure that efficiently guides electrical currents over long distances greatly expands the paradigm of biological charge transport and could enable new bio-electronic applications., Cable bacteria’ form long multicellular filaments that can transfer electrical currents over centimetre-long distances. Here, Meysman et al. show that the electrical currents run along highly conductive fibres embedded in the cell envelope, and charge transfer is electronic rather than ionic.

Despite theoretical predictions that graphene should be impermeable to all gases, practical experiments on sealed graphene nanodrums show small leak rates. Thus far, the exact mechanism for this permeation has remained unclear, because different potential leakage pathways have not been studied separately. Here, we demonstrate a sealing method that consists of depositing SiO2 across the edge of suspended multilayer graphene flakes using electron beam-induced deposition. By sealing, leakage along the graphene-SiO2 interface is blocked, which is observed to result in a reduction in permeation rate by a factor of 104. The experiments thus demonstrate that gas flow along the graphene-SiO2 interface tends to dominate the leak rate in unsealed graphene nanodrums. Moreover, the presented sealing method enables the study of intrinsic gas leakage through graphene membranes and can enable hermetic graphene membranes for pressure sensing applications.

Single-molecule junctions — devices in which a single molecule is electrically connected by two electrodes — enable the study of a broad range of quantum-transport phenomena even at room temperature. These quantum features are related to molecular orbital and spin degrees of freedom and are characterized by various energy scales that can be chemically and physically tuned: level spacings, charging energies, tunnel couplings, exchange energies, vibrational energies and Kondo correlation energies. The competition between these different energy scales leads to a rich variety of processes, which researchers are now starting to be able to control and tune experimentally. In this Technical Review, we present the status of the molecular electronics field from this quantum-transport perspective with a focus on recent experimental results obtained using break-junction devices, including scanning probe and mechanically controlled break junctions, as well as electromigrated gold and graphene break junctions.

Strain engineering is one of the most effective approaches to manipulate the physical state of materials, control their electronic properties, and enable crucial functionalities. Because of their rich phase diagrams arising from competing ground states, quantum materials are an ideal playground for on-demand material control, and can be used to develop emergent technologies, such as adaptive electronics or neuromorphic computing. It was recently suggested that complex oxides could bring unprecedented functionalities to the field of nanomechanics, but the possibility of precisely controlling the stress state of materials is so far lacking. Here we demonstrate the wide and reversible manipulation of the stress state of single-crystal WO3 by strain engineering controlled by catalytic hydrogenation. Progressive incorporation of hydrogen in freestanding ultra-thin structures determines large variations of their mechanical resonance frequencies and induces static deformation. Our results demonstrate hydrogen doping as a new paradigm to reversibly manipulate the mechanical properties of nanodevices based on materials control., 6 pages, 4 figures, 9 supplementary sections

Unsupervised machine learning, and in particular data clustering, is a powerful approach for the analysis of datasets and identification of characteristic features occurring throughout a dataset. It is gaining popularity across scientific disciplines and is particularly useful for applications without a priori knowledge of the data structure. Here, we introduce an approach for unsupervised data classification of any dataset consisting of a series of univariate measurements. It is therefore ideally suited for a wide range of measurement types. We apply it to the field of nanoelectronics and spectroscopy to identify meaningful structures in data sets. We also provide guidelines for the estimation of the optimum number of clusters. In addition, we have performed an extensive benchmark of novel and existing machine learning approaches and observe significant performance differences. Careful selection of the feature space construction method and clustering algorithms for a specific measurement type can therefore greatly improve classification accuracies.

Quantum interference (QI) of electron waves passing through a single-molecule junction provides a powerful means to influence its electrical properties. Here, we investigate the correlation between substitution pattern, conductance, and mechanosensitivity in [2.2]paracyclophane (PCP)-based molecular wires in a mechanically controlled break junction experiment. The effect of themetaversusparaconnectivity in both the central PCP core and the phenyl ring connecting the terminal anchoring group is studied. We find that themeta-phenyl-anchored PCP yields such low conductance levels that molecular features cannot be resolved; in the case ofpara-phenyl-coupled anchoring, however, large variations in conductance values for modulations of the electrode separation occur for the pseudo-para-coupled PCP core, while this mechanosensitivity is absent for the pseudo-meta-PCP core. The experimental findings are interpreted in terms of QI effects between molecular frontier orbitals by theoretical calculations based on density functional theory and the Landauer formalism.

Direct measurement of single-molecule electrical transparency by break junction experiments has become a major field of research over the two last decades. This review specifically and comprehensively highlights the use of porphyrins as molecular components and discusses their potential use for the construction of future devices. Throughout the review, the features provided by porphyrins, such as low level misalignments and very low attenuation factors, are shown with numerous examples, illustrating the potential and limitations of these molecular junctions, as well as differences emerging from applied integration/investigation techniques., Porphyrins have unique properties in electronic circuits. This review summarizes single molecule junction experiments and encourages the development of next generation molecular devices based on such building blocks.

Nano letters 21(18), 7617-7624 (2021). doi:10.1021/acs.nanolett.1c02237, Published by ACS Publ., Washington, DC

The dynamics of suspended two-dimensional (2D) materials has received increasing attention during the last decade, yielding new techniques to study and interpret the physics that governs the motion of atomically thin layers. This has led to insights into the role of thermodynamic and nonlinear effects as well as the mechanisms that govern dissipation and stiffness in these resonators. In this review, we present the current state-of-the-art in the experimental study of the dynamics of 2D membranes. The focus will be both on the experimental measurement techniques and on the interpretation of the physical phenomena exhibited by atomically thin membranes in the linear and nonlinear regimes. We will show that resonant 2D membranes have emerged both as sensitive probes of condensed matter physics in ultrathin layers, and as sensitive elements to monitor small external forces or other changes in the environment. New directions for utilizing suspended 2D membranes for material characterization, thermal transport, and gas interactions will be discussed and we conclude by outlining the challenges and opportunities in this upcoming field., Comment: 39 pages, 16 figures

Probing the universal low temperature magnetic field scaling of Kondo-correlated quantum dots via electrical conductance has proved to be experimentally challenging. Here, we show how to probe this in nonlinear thermocurrent spectroscopy applied to a molecular quantum dot in the Kondo regime. Our results demonstrate that the bias-dependent thermocurrent is a sensitive probe of universal Kondo physics, directly measures the splitting of the Kondo resonance in a magnetic field, and opens up possibilities for investigating nanosystems far from thermal and electrical equilibrium., Comment: Published version, including Supplementary Material main text:6 pages, 4 figures. SI: 55 pages, 22 figures

Theoretical studies suggest that mastering the thermocurrent through single molecules can lead to thermoelectric energy harvesters with unprecedentedly high efficiencies.1,2,3,4,5,6This can be achieved by engineering molecule length,7optimizing the tunnel coupling strength of molecules via chemical anchor groups8or by creating localized states in the backbone with resulting quantum interference features.4Empirical verification of these predictions, however, faces considerable experimental challenges and is still awaited. Here we use a novel measurement protocol that simultaneously probes the conductance and thermocurrent flow as a function of bias voltage and gate voltage. We find that the resulting thermocurrent is strongly asymmetric with respect to the gate voltage, with evidence of molecular excited states in the thermocurrent Coulomb diamond maps. These features can be reproduced by a rate-equation model only if it accounts for both the vibrational coupling and the electronic degeneracies, thus giving direct insight into the interplay of electronic and vibrational degrees of freedom, and the role of spin entropy in single molecules. Overall these results show that thermocurrent measurements can be used as a spectroscopic tool to access molecule-specific quantum transport phenomena.

The charge density wave (CDW) state in van der Waals systems shows interesting scaling phenomena as the number of layers can significantly affect the CDW transition temperature, $T_{CDW}$. However, it is often difficult to use conventional methods to study the phase transition in these systems due to their small size and sensitivity to degradation. Degradation is an important parameter which has been shown to greatly influence the superconductivity in layered systems. Since the CDW state competes with the onset of superconductivity, it is expected that $T_{CDW}$ will also be affected by the degradation. Here, we probe the CDW phase transition by the mechanical resonances of suspended 2H-TaS2 and 2H-TaSe2 membranes and study the effect of disorder on the CDW state. Pristine flakes show the transition near the reported values of 75 K and 122 K respectively. We then study the effect of degradation on 2H-TaS2 which displays an enhancement of $T_{CDW}$ up to 129 K after degradation in ambient air. Finally, we study a sample with local degradation and observe that multiple phase transitions occur at 87 K, 103 K and 118 K with a hysteresis in temperature in the same membrane. The observed spatial variations in the Raman spectra suggest that variations in crystal structure cause domains with different transition temperatures which could result in the hysteresis. This work shows the potential of using nanomechanical resonance to characterize the CDW in suspended 2D materials and demonstrate that degradation can have a large effect on transition temperatures., The following article has been accepted by Applied Physics Letters. After it is published, it will be found at [https://doi.org/10.1063/5.0051112]