Study of charge density waves in suspended 2H-TaS 2 and 2H-TaSe 2 by nanomechanical resonance

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-TaS…

Enhanced superconductivity in atomically thin TaS2

The ability to exfoliate layered materials down to the single layer limit has presented the opportunity to understand how a gradual reduction in dimensionality affects the properties of bulk materials. Here we use this top–down approach to address the problem of superconductivity in the two-dimensional limit. The transport properties of electronic devices based on 2H tantalum disulfide flakes of different thicknesses are presented. We observe that superconductivity persists down to the thinnest layer investigated (3.5 nm), and interestingly, we find a pronounced enhancement in the critical temperature from 0.5 to 2.2 K as the layers are thinned down. In addition, we propose a tight-binding …

Effect of Metal Complexation on the Conductance of Single-Molecular Wires Measured at Room Temperature

The present work aims to give insight into the effect that metal coordination has on the room-temperature conductance of molecular wires. For that purpose, we have designed a family of rigid, highly conductive ligands functionalized with different terminations (acetylthiols, pyridines, and ethynyl groups), in which the conformational changes induced by metal coordination are negligible. The single-molecule conductance features of this series of molecular wires and their corresponding Cu(I) complexes have been measured in break-junction setups at room temperature. Experimental and theoretical data show that no matter the anchoring group, in all cases metal coordination leads to a shift towar…

Room-temperature electrical addressing of a bistable spin-crossover molecular system.

Chemical Design and Magnetic Ordering in Thin Layers of 2D Metal–Organic Frameworks (MOFs)

Through rational chemical design, and thanks to the hybrid nature of metal−organic frameworks (MOFs), it is possible to prepare molecule-based 2D magnetic materials stable at ambient conditions. Here, we illustrate the versatility of this approach by changing both the metallic nodes and the ligands in a family of layered MOFs that allows the tuning of their magnetic properties. Specifically, the reaction of benzimidazole-type ligands with different metal centers (MII = Fe, Co, Mn, Zn) in a solventfree synthesis produces a family of crystalline materials, denoted as MUV-1(M), which order antiferromagnetically with critical temperatures that depend on M. Furthermore, the incorporation o…

Charge Mobility and Dynamics in Spin-Crossover Nanoparticles Studied by Time-Resolved Microwave Conductivity

We use the electrode-less time-resolved microwave conductivity (TRMC) technique to characterize spin-crossover (SCO) nanoparticles. We show that TRMC is a simple and accurate mean for simultaneously as-sessing the magnetic state of SCO compounds and charge transport information on the nanometre length scale. In the low-spin state from liquid nitrogen temperature up to 360 K the TRMC measurements present two well-defined regimes in the mobility and in the half-life times, possessing similar transition tempera-tures TR near 225 K. Below TR, an activation-less regime associated with short lifetimes of the charge carri-ers points at the presence of shallow-trap states. Above TR, these states ar…

Nanomechanical probing and strain tuning of the Curie temperature in suspended Cr2Ge2Te6-based heterostructures

AbstractTwo-dimensional magnetic materials with strong magnetostriction are attractive systems for realizing strain-tuning of the magnetization in spintronic and nanomagnetic devices. This requires an understanding of the magneto-mechanical coupling in these materials. In this work, we suspend thin Cr2Ge2Te6 layers and their heterostructures, creating ferromagnetic nanomechanical membrane resonators. We probe their mechanical and magnetic properties as a function of temperature and strain by observing magneto-elastic signatures in the temperature-dependent resonance frequency near the Curie temperature, TC. We compensate for the negative thermal expansion coefficient of Cr2Ge2Te6 by fabrica…

Sensing of the Molecular Spin in Spin-Crossover Nanoparticles with Micromechanical Resonators

In the past years, the use of highly sensitive silicon microelectromechanical cantilevers has been proposed as a tool to characterize the spin-crossover phenomenon by employing fast optical readout of the motion. In this work, Fe II -based spin-crossover nanoparticles of the well-known [Fe(Htrz) 2 (trz)](BF 4 ) complex wrapped with thin silica shells of different sizes will be studied by means of silicon microresonators. The silica shell will enhance its chemical stability, whereas the low thickness will allow a proper mechanical coupling between the cantilever and the spin-crossover core. To maximize the sensing of the spin-crossover phenomena, different cantilever geometries and flexural…

Spin switching in electronic devices based on 2D assemblies of spin-crossover nanoparticles

In this communication we study the transport properties of two-dimensional assemblies of [Fe(Htrz)2(trz)](BF4) spin-crossover nanoparticles (NPs) with two different morphologies. The NPs have been synthesized made in a similar manner than in our previous study in which single NPs were measured. We prepared free-standing self-assembled monolayer sheets of both SCO NPs formed at the air/liquid interface on holey carbon TEM grids to extract their global arrangement and NP size distributions by STEM-HAADF technique. The SCO NP systems present a rod-like shape and possess two different volumes, corresponding to lengths of 25 nm and 44 nm along the rod direction and average diameters of 10 nm and…

Magnetic order in 2D antiferromagnets revealed by spontaneous anisotropic magnetostriction

The temperature dependent order parameter provides important information on the nature of magnetism. Using traditional methods to study this parameter in two-dimensional (2D) magnets remains difficult, however, particularly for insulating antiferromagnetic (AF) compounds. Here, we show that its temperature dependence in AF MPS$_{3}$ (M(II) = Fe, Co, Ni) can be probed via the anisotropy in the resonance frequency of rectangular membranes, mediated by a combination of anisotropic magnetostriction and spontaneous staggered magnetization. Density functional calculations followed by a derived orbital-resolved magnetic exchange analysis confirm and unravel the microscopic origin of this magnetiza…

Near Room-Temperature Memory Devices Based on Hybrid Spin-Crossover@SiO2Nanoparticles Coupled to Single-Layer Graphene Nanoelectrodes

The charge transport properties of SCO [Fe(Htrz)2 (trz)](BF4 ) NPs covered with a silica shell placed in between single-layer graphene electrodes are reported. A reproducible thermal hysteresis loop in the conductance above room-temperature is evidenced. This bistability combined with the versatility of graphene represents a promising scenario for a variety of technological applications but also for future sophisticated fundamental studies.

Tunable Strong Coupling of Mechanical Resonance between Spatially Separated FePS3 Nanodrums

Coupled nanomechanical resonators made of two-dimensional materials are promising for processing information with mechanical modes. However, the challenge for these types of systems is to control the coupling. Here, we demonstrate strong coupling of motion between two suspended membranes of the magnetic 2D material FePS$_3$. We describe a tunable electromechanical mechanism for control over both the resonance frequency and the coupling strength using a gate voltage electrode under each membrane. We show that the coupling can be utilized for transferring data from one drum to the other by amplitude modulation. Finally, we also study the temperature dependence of the coupling, and in particul…

Magnetic and electronic phase transitions probed by nanomechanical resonators

The reduced dimensionality of two-dimensional (2D) materials results in characteristic types of magnetically and electronically ordered phases. However, only few methods are available to study this order, in particular in ultrathin insulating antiferromagnets that couple weakly to magnetic and electronic probes. Here, we demonstrate that phase transitions in thin membranes of 2D antiferromagnetic FePS3, MnPS3 and NiPS3 can be probed mechanically via the temperature-dependent resonance frequency and quality factor. The observed relation between mechanical motion and antiferromagnetic order is shown to be mediated by the specific heat and reveals a strong dependence of the Néel temperature of…

Controlling the anisotropy of a van der Waals antiferromagnet with light

Ultrafast optical control of magnetic anisotropy in a van der Waals antiferromagnet activates a sub-THz two-dimensional magnon.

CCDC 2068294: Experimental Crystal Structure Determination

Related Article: Javier Lo��pez-Cabrelles, Samuel Man��as-Valero, In��igo J. Vito��rica-Yreza��bal, Makars S��is��kins, Martin Lee, Peter G. Steeneken, Herre S. J. van der Zant, Guillermo Mi��nguez Espallargas, Eugenio Coronado|2021|J.Am.Chem.Soc.|143|18502|doi:10.1021/jacs.1c07802

CCDC 2068293: Experimental Crystal Structure Determination

Related Article: Javier Lo��pez-Cabrelles, Samuel Man��as-Valero, In��igo J. Vito��rica-Yreza��bal, Makars S��is��kins, Martin Lee, Peter G. Steeneken, Herre S. J. van der Zant, Guillermo Mi��nguez Espallargas, Eugenio Coronado|2021|J.Am.Chem.Soc.|143|18502|doi:10.1021/jacs.1c07802

CCDC 2068295: Experimental Crystal Structure Determination

Related Article: Javier Lo��pez-Cabrelles, Samuel Man��as-Valero, In��igo J. Vito��rica-Yreza��bal, Makars S��is��kins, Martin Lee, Peter G. Steeneken, Herre S. J. van der Zant, Guillermo Mi��nguez Espallargas, Eugenio Coronado|2021|J.Am.Chem.Soc.|143|18502|doi:10.1021/jacs.1c07802