The unique properties of two-dimensional (2D) materials bring great promise to improve sensor performance and realise novel sensing principles. However, to enable their high-volume production, wafer-scale processes that allow integration with electronic readout circuits need to be developed. In this perspective, we review recent progress in on-chip 2D material sensors, and compare their performance to the state-of-the-art, with a focus on results achieved in the Graphene Flagship programme. We discuss transfer-based and transfer-free production flows and routes for complementary metal-oxide-semiconductor integration and prototype development. Finally, we give an outlook on the future of 2D material sensors, and sketch a roadmap towards realising their industrial and societal impact.@en

Graphene has garnered significant interest in optoelectronics due to its unique properties, including broad wavelength absorption and high mobility. However, its weak stability in ambient conditions requires encapsulation for practical applications. In this study, we investigate graphene CVD-grown field-effect transistors fabricated on Si/SiO2 wafers, encapsulated with aluminum oxide (Al2O3) of different thicknesses. We measure and analyze their optoelectronic response across wavelengths from near-ultraviolet to near-infrared. We find that, while having a negligible role in the photogating process, the Al2O3 layer leads to stable and reproducible transferring curves operating in ambient conditions for over a month, with stable responsivities up to 1.5 A W−1 at the shortest wavelength. Moreover, the transferring curves are stable at elevated temperatures up to 107 ∘C. We also show that the sample performance can be tuned by changing the thickness of the SiO2 and Al2O3 layer which brings further perspectives in developing robust sample technologies, especially in the ultraviolet region where the responsivity increases. Aluminum oxide encapsulated graphene-based photodetectors can thus be interesting for applications in air and at elevated temperatures.@en

Organic radicals are promising candidates for molecular spintronics due to their intrinsic magnetic moment, their low spin-orbit coupling, and their weak hyperfine interactions. Using a mechanically controlled break junction setup at both room and low temperatures (6 K), we analyze the difference in charge transport between two nitronyl nitroxide radicals (NNR): one with a backbone in the para configuration, the other with a backbone in the meta configuration. We find that para-NNR displays a Kondo resonance at 6 K, while meta-NNR does not. Additionally, the observed Kondo peak in the differential conductance has a roughly constant width independent of the conductance, consistent with a scenario where the molecule is coupled asymmetrically to the electrodes.

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The layered metamagnet CrSBr offers a rich interplay between magnetic, optical, and electrical properties that can be extended down to the two-dimensional (2D) limit. Despite the extensive research regarding the long-range magnetic order in magnetic van der Waals materials, short-range correlations have been loosely investigated. By using small-angle neutron scattering (SANS) the formation of short-range magnetic regions in CrSBr with correlation lengths that increase upon cooling up to ≈3 nm at the antiferromagnetic ordering temperature (T _N ≈ 140 K) is shown. Interestingly, these ferromagnetic correlations start developing below 200 K, i.e., well above T _N. Below T _N, these correlations rapidly decrease and are negligible at low-temperatures. The experimental results are well-reproduced by an effective spin Hamiltonian, which pinpoints that the short-range correlations in CrSBr are intrinsic to the monolayer limit, and discard the appearance of any frustrated phase in CrSBr at low-temperatures within the experimental window between 2 and 200 nm. Overall, the obtained results are compatible with a spin freezing scenario of the magnetic fluctuations in CrSBr and highlight SANS as a powerful technique for characterizing the rich physical phenomenology beyond the long-range order paradigm offered by van der Waals magnets.

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Multicellular cable bacteria display an exceptional form of biological conduction, channeling electric currents across centimeter distances through a regular network of protein fibers embedded in the cell envelope. The fiber conductivity is among the highest recorded for biomaterials, but the underlying mechanism of electron transport remains elusive. Here, we performed detailed characterization of the conductance from room temperature down to liquid helium temperature to attain insight into the mechanism of long-range conduction. A consistent behavior is seen within and across individual filaments. The conductance near room temperature reveals thermally activated behavior, yet with a low activation energy. At cryogenic temperatures, the conductance at moderate electric fields becomes virtually independent of temperature, suggesting that quantum vibrations couple to the charge transport through nuclear tunneling. Our data support an incoherent multistep hopping model within parallel conduction channels with a low activation energy and high transfer efficiency between hopping sites. This model explains the capacity of cable bacteria to transport electrons across centimeter-scale distances, thus illustrating how electric currents can be guided through extremely long supramolecular protein structures.@en

The addition of a lateral alkyl chain is a well-known strategy to reduce π-stacked ensembles of molecules in solution, with the intention to minimize the interactions between the molecules’ backbones. In this paper, we study whether this concept generalizes to single-molecule junctions by using a combination of mechanically controllable break junction (MCBJ) measurements and clustering-based data analysis with two small series of model compounds decorated with various bulky groups. The systematic study suggests that introducing alkyl side chains also favors the formation of electrode-molecule configurations that are not observed in their absence, thereby inducing broadening of the conductance peak in the one-dimensional histograms. Thus, the introduction of alkyl chains in aromatic compounds for molecular electronics must be carefully designed and optimized for the specific purpose, balancing between increased solubility and the possibility of additional junction configurations.

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To investigate interference phenomena and conductance properties in mechanically controlled break junctions (MCBJs), macrocycles 1 and 2 (BMCs: for BenzeneMacroCycles), containing a meta-substituted benzene moiety with solubilizing tert-butyl groups, as well as structures 3 and 4 (TMCs: for ThiopheneMacroCycles), featuring 2,5-connected 3,4-hexyl-thiophene corners, were synthesized. Macrocycles 1 and 2 respectively 3 and 4 differ in the positions of the acetyl-protected sulfur anchoring groups, which impacts both, the individual transport efficiency of their parallel electronic pathways and their overall molecular wire lengths. All macrocycles were synthesized based on a series of Sonogashira cross-coupling reactions. For 3 and 4, a 2-(4-pyridinyl)ethyl protecting group for the sulfur atoms was successful, while for macrocycles 1 and 2 the more common tert-butyl protecting group did the job. To our delight, proof-of-concept charge transport studies conducted in an MCBJ setup demonstrated the expected trends regarding improved conductance intensities for the TMCs compared to the BMCs. Furthermore, the corresponding molecular plateaus from the breaking experiments were in the expected length range of the S−S distances for all compounds. We also found that the overall conductance seems to follow a more complex transport mechanism than just the sum of contributions from both channels.@en

The achievement of valley-polarized electron currents is a cornerstone for the realization of valleytronic devices. Here, we report on ballistic coherent transport experiments where two opposite quantum point contacts (QPCs) are defined by electrostatic gating in a bilayer graphene (BLG) channel. By steering the ballistic currents with an out-of-plane magnetic field we observe two current jets, a consequence of valley-dependent trigonal warping. Tuning the BLG carrier density and number of QPC modes (𝑚) with a gate voltage we find that the two jets are present for 𝑚=1 and up to 𝑚=6, indicating the robustness of the effect. Semiclassical simulations confirm the origin of the signals by quantitatively reproducing the jet separations without fitting parameters. In addition, our model shows that the ballistic current jets have opposite valley polarization. As a consequence, by steering each jet toward the detector using a magnetic field, we achieve full control over the valley polarization of the collected currents, envisioning such devices as ballistic current sources with tunable valley polarization. We also show that collimation experiments are a sensitive probe to the trigonal warping of the Fermi surface.@en

The high susceptibility of ultrathin two-dimensional (2D) material resonators to force and temperature makes them ideal systems for sensing applications and exploring thermomechanical coupling. Although the dynamics of these systems at high stress has been thoroughly investigated, their behavior near the buckling transition has received less attention. Here, we demonstrate that the force sensitivity and frequency tunability of 2D material resonators are significantly enhanced near the buckling bifurcation. This bifurcation is triggered by compressive displacement that we induce via thermal expansion of the devices, while measuring their dynamics via an optomechanical technique. We understand the frequency tuning of the devices through a mechanical buckling model, which allows to extract the central deflection and boundary compressive displacement of the membrane. Surprisingly, we obtain a remarkable enhancement of up to 14× the vibration amplitude attributed to a very low stiffness of the membrane at the buckling transition, as well as a high frequency tunability by temperature of more than 4.02$\%$ K−1. The presented results provide insights into the effects of buckling on the dynamics of free-standing 2D materials and thereby open up opportunities for the realization of 2D resonant sensors with buckling-enhanced sensitivity.@en

Helical molecules have been proposed as candidates for producing spin-polarized currents, even at room conditions, due to their chiral asymmetry. However, describing their transport mechanism in single molecular junctions is not straightforward. In this work, we show the synthesis of two novel kinds of dithia[11]helicenes to study their electronic transport in break junctions among a series of three helical molecules: dithia[n]helicenes, with n = 7, 9, and 11 molecular units. Our experimental measurements and clustering-based analysis demonstrate low conductance values that remain similar across different applied voltages and molecules. Additionally, we assess the length dependence of the conductance for each helicene, revealing an exponential decay characteristic of off-resonant transport. This behavior is primarily attributed to the misalignment between the energy levels of the molecule-electrodes system. The length dependence trend described above is supported by ab initio calculations, further confirming an off-resonant transport mechanism.

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The recent discovery of cable bacteria has greatly expanded the known length scale of biological electron transport, as these multi-cellular bacteria are capable of mediating electrical currents across centimeter-scale distances. To enable such long-range conduction, cable bacteria embed a network of regularly spaced, parallel protein fibers in their cell envelope. These fibers exhibit extraordinary electrical properties for a biological material, including an electrical conductivity that can exceed 100 S cm ⁻¹. Traditionally, long-range electron transport through proteins is described as a multi-step hopping process, in which the individual hopping steps are described by Marcus electron transport theory. Here, we investigate to what extent such a classical hopping model can explain the conductance data recorded for individual cable bacterium filaments. To this end, the conductive fiber network in cable bacteria is modelled as a set of parallel one-dimensional hopping chains. Comparison of model simulated and experimental current(I)/voltage(V) curves, reveals that the charge transport is field-driven rather than concentration-driven, and there is no significant injection barrier between electrodes and filaments. However, the observed high conductivity levels (>100 S cm ⁻¹) can only be reproduced, if we include much longer hopping distances (a > 10 nm) and lower reorganisation energies (λ < 0.2 eV) than conventionally used in electron relay models of protein structures. Overall, our model analysis suggests that the conduction mechanism in cable bacteria is markedly distinct from other known forms of long-range biological electron transport, such as in multi-heme cytochromes.

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Heterostructures, composed of semiconducting transition-metal dichalcogenides (TMDC) and magnetic van-der-Waals materials, offer exciting prospects for the manipulation of the TMDC valley properties via proximity interaction with the magnetic material. We show that the atomic proximity of monolayer MoSe2 and the antiferromagnetic van-der-Waals crystal CrSBr leads to an unexpected breaking of time-reversal symmetry, with originally perpendicular spin directions in both materials. The observed effect can be traced back to a proximity-induced exchange interaction via first-principles calculations. The resulting spin splitting in MoSe2 is determined experimentally and theoretically to be on the order of a few meV. Moreover, we find a more than 2 orders of magnitude longer valley lifetime of spin-polarized charge carriers in the heterostructure, as compared to monolayer MoSe2/SiO2, driven by a Mott transition in the type-III band-aligned heterostructure.@en

Heat transport in two dimensions is fundamentally different from that in three dimensions. As a consequence, the thermal properties of 2D materials are of great interest, from both scientific and application points of view. However, few techniques are available for the accurate determination of these properties in ultrathin suspended membranes. Here, we present an optomechanical methodology for extracting the thermal expansion coefficient, specific heat, and thermal conductivity of ultrathin membranes made of 2H-TaS₂, FePS₃, polycrystalline silicon, MoS₂, and WSe₂. The obtained thermal properties are in good agreement with the values reported in the literature for the same materials. Our work provides an optomechanical method for determining the thermal properties of ultrathin suspended membranes, which are difficult to measure otherwise. It provides a route toward improving our understanding of heat transport in the 2D limit and facilitates engineering of 2D structures with a dedicated thermal performance.

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Open-shell polycyclic aromatic hydrocarbons (PAHs) represent promising building blocks for carbon-based functional magnetic materials. Their magnetic properties stem from the presence of unpaired electrons localized in radical states of π character. Consequently, these materials are inclined to exhibit spin delocalization, form extended collective states, and respond to the flexibility of the molecular backbones. However, they are also highly reactive, requiring structural strategies to protect the radical states from reacting with the environment. Here, we demonstrate that the open-shell ground state of the diradical 2-OS survives on a Au(111) substrate as a global singlet formed by two unpaired electrons with antiparallel spins coupled through a conformational-dependent interaction. The 2-OS molecule is a “protected” derivative of the Chichibabin’s diradical, featuring a nonplanar geometry that destabilizes the closed-shell quinoidal structure. Using scanning tunneling microscopy (STM), we localized the two interacting spins at the molecular edges, and detected an excited triplet state a few millielectronvolts above the singlet ground state. Mean-field Hubbard simulations reveal that the exchange coupling between the two spins strongly depends on the torsional angles between the different molecular moieties, suggesting the possibility of influencing the molecule’s magnetic state through structural changes. This was demonstrated here using the STM tip to manipulate the molecular conformation, while simultaneously detecting changes in the spin excitation spectrum. Our work suggests the potential of these PAHs as all-carbon spin-crossover materials.@en

Heat-to-charge conversion efficiency of thermoelectric materials is closely linked to the entropy per charge carrier. Thus, magnetic materials are promising building blocks for highly efficient energy harvesters as their carrier entropy is boosted by a spin degree of freedom. In this work, we investigate how this spin-entropy impacts heat-to-charge conversion in the A-type antiferromagnet CrSBr. We perform simultaneous measurements of electrical conductance and thermocurrent while changing magnetic order using the temperature and magnetic field as tuning parameters. We find a strong enhancement of the thermoelectric power factor at around the Néel temperature. We further reveal that the power factor at low temperatures can be increased by up to 600% upon applying a magnetic field. Our results demonstrate that the thermoelectric properties of 2D magnets can be optimized by exploiting the sizable impact of spin-entropy and confirm thermoelectric measurements as a sensitive tool to investigate subtle magnetic phase transitions in low-dimensional magnets.

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Quantum interference plays an important role in charge transport through single-molecule junctions, even at room temperature. Of special interest is the measurement of the destructive quantum interference dip itself. Such measurements are especially demanding when performed in a continuous mode of operation. Here, we use mechanical modulation experiments at ambient conditions to reconstruct the destructive quantum interference dip of conductance versus displacement. Simultaneous measurements of the Seebeck coefficient show a sinusoidal response across the dip without sign change. Calculations that include electrode distance and energy alignment variations explain both observations quantitatively, emphasizing the crucial role of thermal fluctuations for measurements under ambient conditions. Our results open the way for establishing a closer link between break-junction experiments and theory in explaining single-molecule transport phenomena, especially when describing sharp features in the transmission.

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We present the electrical characterization of wafer-scale graphene devices fabricated with an industrially-relevant, contact-first integration scheme combined with Al₂O₃ encapsulation via atomic layer deposition. All the devices show a statistically significant reduction in the Dirac point position, V cnp , from around +47 V to between −5 and 5 V (on 285 nm SiO₂), while maintaining the mobility values. The data and methods presented are relevant for further integration of graphene devices, specifically sensors, at the back-end-of-line of a standard CMOS flow.

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We report on the fabrication of a single-electron transistor based on ferritin using wide self-aligned nanogap devices. A local gate below the gap area enables three-terminal electrical measurements, showing the Coulomb blockade in good agreement with the single-electron tunneling theory. Comparison with this theory allows extraction of the tunnel resistances, capacitances, and gate coupling. Additionally, the data suggest the presence of two separate islands coupled in series or in parallel: information that was not possible to distinguish by using only two-terminal measurements. To interpret the charge transport features, we propose a scenario based on the established configuration structures of ferritin involving either iron sites in the organic shell or two dissimilar clusters within the core.@en

Break-junction techniques provide the possibility to study electric and thermoelectric properties of single-molecule junctions in great detail. These techniques rely on the same principle of controllably breaking metallic contacts in order to create single-molecule junctions, whilst keeping track of the junction's conductance. Here, we compare results from mechanically controllable break junction (MCBJ) and scanning tunneling microscope (STM) methods, while characterizing conductance properties of the same novel mechanosensitive para- and meta-connected naphtalenophane compounds. In addition, thermopower measurements are carried out for both compounds using the STM break junction (STM-BJ) technique. For the conductance experiments, the same data processing using a clustering analysis is performed. We obtain to a large extent similar results for both methods, although values of conductance and stretching lengths for the STM-BJ technique are slightly larger in comparison with the MCBJ. STM-BJ thermopower experiments show similar Seebeck coefficients for both compounds. An increase in the Seebeck coefficient is revealed, whilst the conductance decreases, after which it saturates at around 10 μV K−1. This phenomenon is studied theoretically using a tight binding model. It shows that changes of molecule-electrode electronic couplings combined with shifts of the resonance energies explain the correlated behavior of conductance and Seebeck coefficient.@en

Exploiting the potential of curcuminoids (CCMoids) as molecular platforms, a new 3.53 nm extended system (pyACCMoid, 2) has been designed in two steps by reacting a CCMoid with amino-terminal groups (NH2-CCMoid, 1, of 1.79 nm length) with polycyclic aromatic hydrocarbon (PAH) aldehydes. CCMoid 2 contains pyrene units at both ends as anchoring groups to optimize its trapping in graphene nano-junctions created by feedback-controlled electro-burning. The measured I–V characteristics show gate-dependent behaviour at room temperature and 10 K, with increased conductance values compared to shorter CCMoids previously reported, and in agreement with DFT calculations. Our results show that the adjusted molecular design improves the conductance, as system 2 separates the conductive backbone from the anchor groups, which tend to adopt a planar configuration upon contact with the graphene electrodes. DFT calculations using Green functions of a set of different molecular conformations of 2 on graphene electrodes show a direct relationship between the units (e.g. pyrene, amide, etc.), in the molecule, through which electrons are injected and the conductance values; where the size of the spacing between the graphene electrodes contributes but is not the dominant factor, and thus, counter-intuitively the smallest spacing gives one of the lowest conductance values.@en