We report a comprehensive determination of the broadband dielectric permittivity tensor of van der Waals (vdW) muscovite also referred to as mica, establishing it as a low-index low-loss platform for ultrathin nanophotonics. Resolving its anisotropic vibrational response and extracting accurate tensor components across broadband ultraviolet (UV) to near-infrared (NIR) spectral region, we show that vdW muscovite exhibits consistently low refractive indices negligible extinction and weak in-plane anisotropy allowing its effective treatment as a uniaxial dielectric in thin-film limits. Leveraging these properties, we design muscovite based vdW heterostructures pairing it MoS2, engineering few-layer distributed Bragg reflectors (DBR) and dichroic beam splitters (DBS) with high efficiency robust optical performance in a broad NIR spectral region achieved with sub-micron thicknesses. Our findings spotlight the high significance of low-index extinctionless vdW crystals, positioning muscovite as a highly perspective atomically flat building block for next-generation, broadband, all-vdW nanophotonic components.
The X-ray Integral Field Unit (X-IFU) is an instrument being developed for the New Advanced Telescope for High ENergy Astrophysics observatory satellite. It utilizes an array of X-ray transition-edge sensor (TES) microcalorimeter pixels, with the instrument designed to achieve an energy resolution of 4 eV at photon energies up to 7 keV. Vibration of individual TES pixels in the array has the potential to degrade this performance predominantly through time-varying thermal dissipation. To mitigate this, in the X-IFU design, the first vibrational eigenfrequency of the TES pixels is required to be greater than 25 kHz. This is to ensure that the first eigenfrequency is significantly larger than the bandwidth of known vibration drivers, such as cryocoolers, and therefore coupling and dissipation in the pixels is negligible. We present theoretical and experimental determination of the eigenfrequencies and eigenmodes of prototype TES pixels designed for X-IFU. We show that the first eigenfrequency is 89 kHz at room temperature and decreases to 86 kHz at 5.6 K.
Abstract The advent of van der Waals (vdW) heterostructures has enabled formation of bespoke materials with atomic precision, where numerous quantum and topological phenomena have already been discovered. This atomic-layer tunability, however, comes at a cost: individual 2D layers must be picked up, moved, and placed in a deterministic manner while keeping their interfaces atomically clean. Recent advances in machine learning and robotics place even stronger emphasis on the deterministic aspect of vdW assembly. Current polymer-based transfer methods satisfy neither the determinism nor cleanliness requirements. To this end, solutions are needed where adhesion can be dynamically and deterministically controlled without leaving organic contamination. Here, we present a polymer-free transfer technique employing thin muscovite (mica) crystals. Temperature control over mica adhesion enables deterministic pick-up, stacking, and release of 2D materials, while their crystalline, inorganic nature ensures pristine interfaces and suppresses strain. Fully compatible with existing fabrication workflows, this approach enables the assembly of demanding vdW heterostructures, including those with exposed conductive layers, moiré superlattices and suspended membranes. Our method represents a promising strategy for vdW heterostructure fabrication toward its automatisation.
Atomically thin mechanical resonators have been realized predominantly in crystalline two-dimensional (2D) materials, such as graphene, where long-range crystalline order sets their elastic properties and defines their nonlinear resonant behavior. Extending these concepts to the amorphous 2D limit has remained largely unexplored. Here, we demonstrate that monolayer amorphous carbon (MAC) forms suspended membranes that support optothermal actuation and sensitive interferometric readout across both linear and nonlinear regimes of its resonant motion. We resolve thermomechanical motion, driven resonances, and multimode spectra in MAC nanodrums. The frequencies of fundamental vibration modes correspond to unusually low pretensions, placing monolayer MAC nanodrums in a regime where geometric nonlinearities, stress heterogeneity, and mode coupling emerge at comparatively low drive powers. Consistently, we observe pronounced nonlinear dynamics, including hardening, softening, and mixed Duffing responses, nonlinear damping, parametrically excited modes, and signatures of intermodal coupling. These results establish MAC as a robust nanoelectromechanical platform and open an experimental route to disorder-governed nanomechanics in the 2D amorphous limit.
The integration of polarization-control elements into nanoscale photonic circuits remains a central challenge for modern on-chip optical technologies, which call for continuous miniaturization. Van der Waals (vdW) crystals provide a versatile platform for the creation of such components owing to their strong optical anisotropy, high-refractive indices and atomically precise heterostructure assembly capabilities. In this work, we demonstrate an approach towards the creation of all-vdW on-chip polarization optical components, exemplified with quarter-wave plates operating in the near-infrared (NIR) spectral region, realized in specifically twisted ReSe2/alpha-MoO3 vdW heterostructures on a Si/SiO2 platform. Here, low-symmetry ReSe2 layer serves as a source of exceptionally high linearly polarized excitonic emission, whereas in-plane birefringent alpha-MoO_3 provides polarization-state conversion. Furthermore, our finite-difference time-domain (FDTD) simulations quantitatively reproduce the experimental observations with high accuracy revealing the critical roles of layer thicknesses, twist-angle, Fabry-Perot interference and emitter distribution effects in the determination of polarization conversion efficiency, which yields up to 95
Traditional magnetic phase diagram represents a transition between the ferromagnetic and paramagnetic states of a material under the influence of varied temperature, magnetic field, and pressure. So far, the ferromagnetic phase has been considered predominantly as a single type of magnetization texture extending macroscopically in the bulk of a crystal, existing as a ground state determined by the interactions between localized magnetic moments arranged in a lattice. Here, it is demonstrated that an unconventional magnetic order composed of vertically correlated planar magnetic sub-domains occurs intrinsically in mechanically exfoliated layers of van der Waals ferromagnet CrBr3. Based on the visualization of the magnetic textures through magnetic force microscopy in conjunction with the ab initio calculations of the crystal structure in the magnetic phase and micromagnetic simulations, the origin of the magnetic sub-domains is attributed to stacking faults isolating a van der Waals ferromagnetic well from the bulk film due to modifications in the interlayer exchange coupling. This enables to create a phase diagram describing the magnetic states unique to van der Waals ferromagnets in terms of the degree of correlation between the magnetic sub-domains, dependent on the exchange coupling constants and tuneable by magnetic field and temperature.
Magnetic skyrmions are topologically protected quasi-particles with a well-defined chirality. Control over their chirality is proposed as an additional feature for encoding data bits or as qubits in quantum computing due to their high efficiency and stability against achiral magnetic textures. Here it is shown that an in-plane magnetic field can be utilized to reshape the energy barriers between different skyrmionic bubbles (e.g., Bloch type, type-II) enabling spontaneous chirality fluctuations with a frequency that increases with the strength of the in-plane field. The insulating van der Waals ferromagnet CrBr3 is used as an archetypal system for low damping, reduced energy dissipation and a high number of magnetic phases to capture the chirality dynamics in real time through cryo-Lorentz transmission electron microscopy. It is observed that the interplay between the intrinsic Dzyaloshinskii-Moriya interaction and out-of-plane field biased the chirality dynamics, favoring one handedness over the other. A remarkable consequence of the spontaneous chirality switching mechanism is that it induces a freezing (or crystallization) process in the skyrmion lattice. As the bubbles fluctuate between Bloch and type-II they elongate and shrink parallel to the in-plane field. Subsequently, the overall lattice crystallizes along the in-plane field direction, inducing a phase transition from a disordered liquid state to a hexatic phase where skyrmions are highly ordered resembling that of a solid. The results indicate chirality as an active element in the creation of topologically protected skyrmion crystals unveiling pathways toward chiral spintronic device platforms with tunable embedded configuration.
Two-dimensional (2D) materials have disrupted materials science due to the development of van der Waals technology. It enables the stacking of ultrathin layers of materials characterized by vastly different electronic structures to create man-made heterostructures and devices with rationally tailored properties, circumventing limitations of matching crystal structures, lattice constants, and geometry of constituent materials and supporting substrates. 2D materials exhibit extraordinary mechanical flexibility, strong light-matter interactions driven by their excitonic response, single photon emission from atomic centers, stable ferromagnetism in sub-nm thin films, fractional quantum Hall effect in high-quality devices, and chemoselectivity at ultrahigh surface-to-volume ratio. Consequently, van der Waals heterostructures with atomically flat interfaces demonstrate an unprecedented degree of intertwined mechanical, chemical, optoelectronic, and magnetic properties. This constitutes a foundation for multiproperty sensing, based on complex intra- and intermaterial interactions, and a robust response to external stimuli originating from the environment. Here, we review recent progress in the development of sensing applications with 2D materials, highlighting the areas where van der Waals heterostructures offer the highest sensitivity, simultaneous responses to multiple distinct externalities due to their atomic thickness in conjunction with unique material combinations, and conceptually new sensing methodology.
Nanomechanical resonances of two-dimensional (2D) materials are sensitive probes for condensedmatter physics, offering new insights into magnetic and electronic phase transitions. Despite extensive research, the influence of the spin dynamics near a phase transition on the nonlinear dynamics of 2D membranes has remained largely unexplored. Here, we investigate nonlinear magneto-mechanical coupling to antiferromagnetic order in suspended FePS3-based heterostructure membranes. By monitoring the motion of these membranes as a function of temperature, we observe characteristic features in both nonlinear stiffness and damping close to the Néel temperature TN. We account for these experimental observations with an analytical magnetostriction model in which these nonlinearities emerge from a coupling between mechanical and magnetic oscillations, demonstrating that magneto-elasticity can lead to nonlinear damping. Our findings thus provide insights into the thermodynamics and magneto-mechanical energy dissipation mechanisms in nanomechanical resonators due to the material’s phase change and magnetic order relaxation. Magnetic phase transitions typically lead to changes in a materials magnetostrictive properties. Here, Šiškins et al use the motion of a nanodrum to study the nonlinear magneto-mechanical response of FePS3, and observe changes in the nonlinear stiffness and damping near the Neel temperature.
A quantitative understanding of the microscopic mechanisms responsible for damping in van der Waals nanomechanical resonators remains elusive. In this work, we investigate van der Waals magnets, where the thermal expansion coefficient exhibits an anomaly at the magnetic phase transition due to magnetoelastic coupling. Thermal expansion mediates the coupling between mechanical strain and heat flow and determines the strength of thermoelastic damping (TED). Consequently, variations in the thermal expansion coefficient are reflected directly in TED, motivating our focus on this mechanism. We extend existing TED models to incorporate anisotropic thermal conduction, a critical property of van der Waals materials. By combining the thermodynamic properties of the resonator material with the anisotropic TED model, we examine dissipation as a function of temperature. Our findings reveal a pronounced impact of the phase transition on dissipation, along with transitions between distinct dissipation regimes controlled by geometry and the relative contributions of in-plane and out-of-plane thermal conductivity. These regimes are characterized by the resonant interplay between strain and in-plane or through-plane heat propagation. To validate our theory, we compare it to experimental data of the temperature-dependent mechanical resonances of FePS_3 resonators.
Generation and control of topological spin textures constitutes one of the most exciting challenges of modern spintronics given their potential applications in information storage technologies. Of particular interest are magnetic insulators, which due to low damping, absence of Joule heating and reduced dissipation can provide energy-efficient spin-textures platform. Here, it is demonstrated that the interplay between sample thickness, external magnetic fields, and optical excitations can generate a prolific paramount of spin textures, and their coexistence in insulating CrBr3 van der Waals (vdW) ferromagnets. Using high-resolution magnetic force microscopy and large-scale micromagnetic simulation methods, the existence of a large region in T-B phase diagram is demonstrated where different stripe domains, skyrmion crystals, and magnetic domains exist and can be intrinsically selected or transformed to each-other via a phase-switch mechanism. Lorentz transmission electron microscopy unveils the mixed chirality of the magnetic textures that are of Bloch-type at given conditions but can be further manipulated into Néel-type or hybrid-type via thickness-engineering. The topological phase transformation between the different magnetic objects can be further inspected by standard photoluminescence optical probes resolved by circular polarization indicative of an existence of exciton-skyrmion coupling mechanism. The findings identify vdW magnetic insulators as a promising framework of materials for the manipulation and generation of highly ordered skyrmion lattices relevant for device integration at the atomic level.
Antiferromagnetic materials feature intrinsic ultrafast spin dynamics, making them ideal candidates for future magnonic devices operating at THz frequencies. A major focus of current research is the investigation of optical methods for the efficient generation of coherent magnons in antiferromagnetic insulators. In magnetic lattices endowed with orbital angular momentum, spin-orbit coupling enables spin dynamics through the resonant excitation of low-energy electric dipoles such as phonons and orbital resonances which interact with spins. However, in magnetic systems with zero orbital angular momentum, microscopic pathways for the resonant and low-energy optical excitation of coherent spin dynamics are lacking. Here, we consider experimentally the relative merits of electronic and vibrational excitations for the optical control of zero orbital angular momentum magnets, focusing on a limit case: the antiferromagnet manganese phosphorous trisulfide (MnPS_{3}), constituted by orbital singlet Mn^{2+} ions. We study the correlation of spins with two types of excitations within its band gap: a bound electron orbital excitation from the singlet orbital ground state of Mn^{2+} into an orbital triplet state, which causes coherent spin precession, and a vibrational excitation of the crystal field that causes thermal spin disorder. Our findings cast orbital transitions as key targets for magnetic control in insulators constituted by magnetic centers of zero orbital angular momentum.
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 magnetization-induced anisotropic strain. We further show that the temperature and thickness dependent order parameter allows to deduce the material’s critical exponents characterising magnetic order. Nanomechanical sensing of magnetic order thus provides a future platform to investigate 2D magnetism down to the single-layer limit.
In van der Waals (vdW) materials, the electron mean free path (MFP) is largely influenced by the discrete states in the unoccupied band structure. So far, the influence of these states has only been measured in graphene, while all measurements on other vdW materials lack energy resolution. Here, we present reflection and transmission spectra of freestanding, few-layered molybdenum disulfide (MoS2) samples in the 0-55 eV electron range. Our measurements reveal states of enhanced electron transmissivity above the vacuum level, that correspond to the (unoccupied) density of states. We also show a full quantum-mechanical calculation that confirms a good understanding of the elastic scattering in MoS2. A model is developed to extract the inelastic MFP spectrum, which is a measure of the inelastic scattering cross section. As MoS2 is a complicated system of different atomic planes, we expect that our methods generalize well to other van der Waals materials and heterostacks thereof.
Heat transport by acoustic phonons in two-dimensional (2D) materials is fundamentally different from that in 3D crystals because the out-of-plane phonons propagate in a unique way that strongly depends on tension and bending rigidity. Here, using optomechanical techniques, we experimentally demonstrate that the heat transport time in freestanding graphene membranes is significantly higher than the theoretical prediction, and decreases by as much as 33% due to an electrostatically induced tension of 0.07 N/m. Using phonon scattering and Debye models, we explain these observations by the tension-enhanced acoustic impedance match of flexural phonons at the boundary of the graphene membrane. Thus, we experimentally elucidate the tunability of phononic heat transport in 2D materials by tension, and open a route towards electronic devices and circuits for high-speed control of temperature at the nanoscale.
We developed a theoretical scheme of incorporating the magnetoelastic contribution into the thermal elastic dynamics for the thin membranes of 2D antiferromagnetic material with restricted geometry. We extended the elastic Gr\"uneisen relation into an effective version which includes the magnetic counterpart to the volume change of internal energy. Based on the specific heat and thermal conductivity from the elastic and magnetic origins we predicted the dependency of observables, such as effective Gr\"uneisen parameter, thermal expansion coefficient, and the damping factor, with respect to a wide range of temperature across the phase transition. Our model of analysis as been validated by applying to the case of FePS3 flake resonator and the theoretical predictions fits well with the reported experiment data.
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.
CoPS3 stands out in the family of the van der Waals antiferromagnets XPS3 (X=Mn, Ni, Fe, 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 4T1g - 4T2g 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 Bg phonon mode at the frequency of about 4.7 THz.
Heat transport by acoustic phonons in 2D materials is fundamentally different from that in 3D crystals because the out-of-plane phonons propagate in a unique way that strongly depends on tension and bending rigidity. Since in-plane and out-of-plane phonon baths are decoupled, initial studies suggested they provide independent pathways for heat transport and storage in 2D materials. Here, we induce tension in freestanding graphene membranes by electrostatic force, and use optomechanical techniques to demonstrate that it can change the rate of heat transport by as much as 33%. Using a ballistic Debye model, we account for these observations and extract the average bending rigidity of the flexural acoustic phonons, which increases approximately linearly with the membrane's areal mass density, in contrast to the cubic dependence seen in bulk structures. Thus, we not only elucidate phononic heat transport mechanisms in suspended 2D materials, but also provide a promising route for controlling nanoscale heat transport by tension.
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 Cr 2 Ge 2 Te 6 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 Cr 2 Ge 2 Te 6 by fabricating heterostructures with thin layers of WSe 2 and antiferromagnetic FePS 3 , 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 Cr 2 Ge 2 Te 6 -based heterostructure by 2.5 ± 0.6 K by applying a strain of 0.026% via electrostatic force.