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.

Nanomechanical spectroscopy (NMS) is a recently developed approach to determine optical absorption spectra of nanoscale materials via mechanical measurements. It is based on measuring changes in the resonance frequency of a membrane resonator vs. the photon energy of incoming light. This method is a direct measurement of absorption, which has practical advantages compared to common optical spectroscopy approaches. In the case of two-dimensional (2D) materials, NMS overcomes limitations inherent to conventional optical methods, such as the complications associated with measurements at high magnetic fields and low temperatures. In this work, we develop a protocol for NMS of 2D materials that yields two orders of magnitude improved sensitivity compared to previous approaches, while being simpler to use. To this end, we use mechanical sample actuation, which simplifies the experiment and provides a reliable calibration for greater accuracy. Additionally, the use of low-stress silicon nitride membranes as our substrate reduces the noise-equivalent power to NEP = 890 fW H z − 1 , comparable to commercial semiconductor photodetectors. We use our approach to spectroscopically characterize a 2D transition metal dichalcogenide (WS₂), a layered magnetic semiconductor (CrPS₄), and a plasmonic super-crystal consisting of gold nanoparticles.

CoPS₃ stands out in the family of the van der Waals antiferromagnets XPS₃ (X = Mn, Ni, Fe, and Co) due to the unquenched orbital momentum of the magnetic Co²⁺ ions, which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump-probe technique, we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and, thus, results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the ⁴T_1g → ⁴T_2g electronic transition in Co²⁺ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent B_g phonon mode at the frequency of about 4.7 THz.

The authors present magnetotransport measurements to demonstrate multistep magnetization switching in orthogonally twisted CrSBr ferromagnetic monolayers.

Semiconducting van der Waals magnets exhibit a rich physical phenomenology with different collective excitations, as magnons or excitons, that can be coupled, thereby offering new opportunities for optoelectronic, spintronic, and magnonic devices. In contrast with the well-studied van der Waals magnets CrI₃ or Fe₃GeTe₂, CrPS₄ is a layered metamagnet with a high optical and magnon transport anisotropy. Here, the structural anisotropy of CrPS₄ above and below the magnetic phase transition is investigated by fabricating nanomechanical resonators. A large anisotropy is observed in the resonance frequency of resonators oriented along the crystalline a- and b-axis, indicative of a lattice expansion along the b-axis, boosted at the magnetic phase transition, and a rather small continuous contraction along the a-axis. This behavior in the mechanical response differs from that previously reported in van der Waals magnets, as FePS₃ or CoPS₃, and can be understood from the quasi-1D nature of CrPS₄. The results pinpoint CrPS₄ as a promising material in the field of low-dimensional magnetism and show the potential of mechanical resonators for unraveling the in-plane structural anisotropy coupled to the magnetic ordering that, in a broader context, can be extended to studying structural modifications in other 2D materials and van der Waals heterostructures.

Magnetostrictive coupling has recently attracted interest as a sensitive method for studying magnetism in two-dimensional (2D) materials by mechanical means. However, its application in high-frequency magnetic actuators and transducers requires rapid modulation of the magnetic order, which is difficult to achieve with external magnets, especially when dealing with antiferromagnets. Here, we optothermally modulate the magnetization in antiferromagnetic 2D material membranes of metal phosphor trisulfides (MPS₃), to induce a large high-frequency magnetostrictive driving force. From the analysis of the temperature-dependent resonance amplitude, we provide evidence that the force is due to a thermo-magnetostrictive effect, which significantly increases near the Neél temperature, due to the strong temperature dependence of the magnetization. By studying its angle dependence, we find the effect is observed to follow anisotropic magnetostriction of the crystal lattice. The results show that the thermo-magnetostrictive effect results in a strongly enhanced thermal expansion force near the critical temperature of magnetostrictive 2D materials, which can enable more efficient actuation of nano-magnetomechanical devices and can also provide a route for studying the high-frequency coupling among magnetic, mechanical, and thermodynamic degrees of freedom down to the 2D limit.

Two-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, T_C. We compensate for the negative thermal expansion coefficient of Cr₂Ge₂Te₆ by fabricating heterostructures with thin layers of WSe₂ and antiferromagnetic FePS₃, which have positive thermal expansion coefficients. Thus we demonstrate the possibility of probing multiple magnetic phase transitions in a single heterostructure. Finally, we demonstrate a strain-induced enhancement of T_C in a suspended Cr₂Ge₂Te₆-based heterostructure by 2.5 ± 0.6 K by applying a strain of 0.026% via electrostatic force.

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 solvent-free 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 of additional substituents in the ligand results in a novel system, denoted as MUV-8, formed by covalently bound magnetic double layers interconnected by van der Waals interactions, a topology that is very rare in the field of 2D materials and unprecedented for 2D magnets. These layered materials are robust enough to be mechanically exfoliated down to a few layers with large lateral dimensions. Finally, the robustness and crystallinity of these layered MOFs allow the fabrication of nanomechanical resonators that can be used to detect-through laser interferometry-the magnetic order in thin layers of these 2D molecule-based antiferromagnets.

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 demonstrates that the degradation can have a large effect on transition temperatures.

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 FePS₃ on electrostatically induced strain. The methodology is not restricted to magnetic order, as we demonstrate by probing an electronic charge-density-wave phase in 2H-TaS₂. It thus offers the potential to characterize phase transitions in a wide variety of materials, including those that are antiferromagnetic, insulating or so thin that conventional bulk characterization methods become unsuitable.

It is known that the quantum mechanical ground state of a nanoscale junction has a significant impact on its electrical transport properties. This becomes particularly important in transistors consisting of a single molecule. Because of strong electron-electron interactions and the possibility of accessing ground states with high spins, these systems are eligible hosts of a current-blockade phenomenon called a 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 a 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.

A chemical protocol to design robust hybrid [Fe(Htrz)₂(trz)](BF₄)@SiO₂ nanoparticles (NPs) with sizes as small as 28 nm and ultrathin silica shells below 3 nm has been developed. These NPs present a characteristic abrupt spin transition with a subsequent decrease in the width of the thermal hysteresis upon reducing the NP size.

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 modes were employed. In addition, the experimental observations were also compared with COMSOL numerical simulations, which are in close agreement with them. The probe of spin-crossover phenomena with micro- and nanoelectromechanical actuators offers the possibility of preparing smart sensing memory devices near/above room temperature.

We use the electrodeless time-resolved microwave conductivity (TRMC) technique to characterize spin-crossover (SCO) nanoparticles. We show that TRMC is a simple and accurate means for simultaneously assessing the magnetic state of SCO compounds and charge transport information on the nanometer 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, in which the former transition temperature T_R occurs near 225 K. Below T_R, we propose that an activationless regime taking place associated with short lifetimes of the charge carriers points at the presence of shallow-trap states. Above T_R, these states are thermally released, yielding a thermally activated hopping regime where longer hops increase the mobility and, concomitantly, the barrier energy. The activation energy could originate not only from intricate contributions such as polaronic self-localizations but also from dynamic disorder due to phonons and/or thermal fluctuations of SCO moieties.

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 model, which allows us to attribute this phenomenon to an enhancement of the effective electron-phonon coupling constant. This work provides evidence that reducing the dimensionality can strengthen superconductivity as opposed to the weakening effect that has been reported in other 2D materials so far.