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Register a new userIdentifying atomically thin crystals with diffusively reflected light
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The field of two-dimensional materials has been developing at an impressive pace, with atomically thin crystals of an increasing number of different compounds that have become available, together with techniques enabling their assembly into functional heterostructures. The strategy to detect these atomically thin crystals has however remained unchanged since the discovery of graphene. Such an absence of evolution is starting to pose problems because for many of the 2D materials of current interest the optical contrast provided by the commonly used detection procedure is insufficient to identify the presence of individual monolayers or to determine unambiguously the thickness of atomically thin multilayers. Here we explore an alternative detection strategy, in which the enhancement of optical contrast originates from the use of optically inhomogeneous substrates, leading to diffusively reflected light. Owing to its peculiar polarization properties and to its angular distribution, diffusively reflected light allows a strong contrast enhancement to be achieved through the implementation of suitable illumination-detection schemes. We validate this conclusion by carrying out a detailed quantitative analysis of optical contrast, which fully reproduces our experimental observations on over 60 WSe$_2$ mono-, bi-, and trilayers. We further validate the proposed strategy by extending our analysis to atomically thin phosphorene, InSe, and graphene crystals. Our conclusion is that the use of diffusively reflected light to detect and identify atomically thin layers is an interesting alternative to the common detection scheme based on Fabry-Perot interference, because it enables atomically thin layers to be detected on substrates others than the commonly used Si/SiO$_2$, and it may offer higher sensitivity depending on the specific 2D material considered.
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Monolayers of graphene and hexagonal boron nitride (hBN) are highly permeable to thermal protons. For thicker two-dimensional (2D) materials, proton conductivity diminishes exponentially so that, for example, monolayer MoS2 that is just three atoms thick is completely impermeable to protons. This seemed to suggest that only one-atom-thick crystals could be used as proton conducting membranes. Here we show that few-layer micas that are rather thick on the atomic scale become excellent proton conductors if native cations are ion-exchanged for protons. Their areal conductivity exceeds that of graphene and hBN by one-two orders of magnitude. Importantly, ion-exchanged 2D micas exhibit this high conductivity inside the infamous gap for proton-conducting materials, which extends from 100 C to 500 C. Areal conductivity of proton-exchanged monolayer micas can reach above 100 S cm-2 at 500 C, well above the current requirements for the industry roadmap. We attribute the fast proton permeation to 5 A-wide tubular channels that perforate micas crystal structure which, after ion exchange, contain only hydroxyl groups inside. Our work indicates that there could be other 2D crystals with similar nm-scale channels, which could help close the materials gap in proton-conducting applications.
The magnetic state of atomically thin semiconducting layered antiferromagnets such as CrI$_3$ and CrCl$_3$ can be probed by forming tunnel barriers and measuring their resistance as a function of magnetic field ($H$) and temperature ($T$). This is possible because the tunneling magnetoresistance originates from a spin-filtering effect sensitive to the relative orientation of the magnetization in different layers, i.e., to the magnetic state of the multilayers. For systems in which antiferromagnetism occurs within an individual layer, however, no spin-filtering occurs: it is unclear whether this strategy can work. To address this issue, we investigate tunnel transport through atomically thin crystals of MnPS$_3$, a van der Waals semiconductor that in the bulk exhibits easy-axis antiferromagnetic order within the layers. For thick multilayers below $Tsimeq 78$ K, a $T$-dependent magnetoresistance sets-in at $sim 5$ T, and is found to track the boundary between the antiferromagnetic and the spin-flop phases known from bulk magnetization measurements. The magnetoresistance persists down to individual MnPS$_3$ monolayers with nearly unchanged characteristic temperature and magnetic field scales, albeit with a different dependence on $H$. We discuss the implications of these finding for the magnetic state of atomically thin MnPS$_3$ crystals, conclude that antiferromagnetic correlations persist down to the level of individual monolayers, and that tunneling magnetoresistance does allow magnetism in 2D insulating materials to be detected even in the absence of spin-filtering.
The resonance frequency of membranes depends on the gas pressure due to the squeeze-film effect, induced by the compression of a thin gas film that is trapped underneath the resonator by the high frequency motion. This effect is particularly large in low-mass graphene membranes, which makes them promising candidates for pressure sensing applications. Here, we study the squeeze-film effect in single layer graphene resonators and find that their resonance frequency is lower than expected from models assuming ideal compression. To understand this deviation, we perform Boltzmann and continuum finite-element simulations, and propose an improved model that includes the effects of gas leakage and can account for the observed pressure dependence of the resonance frequency. Thus, this work provides further understanding of the squeeze-film effect and provides further directions into optimizing the design of squeeze-film pressure sensors from 2D materials.
Chromium triiodide, CrI$_3$, is emerging as a promising magnetic two-dimensional semiconductor where spins are ferromagnetically aligned within a single layer. Potential applications in spintronics arise from an antiferromagnetic ordering between adjacent layers that gives rise to spin filtering and a large magnetoresistance in tunnelling devices. This key feature appears only in thin multilayers and it is not inherited from bulk crystals, where instead neighbouring layers share the same ferromagnetic spin orientation. This discrepancy between bulk and thin samples is unexpected, as magnetic ordering between layers arises from exchange interactions that are local in nature and should not depend strongly on thickness. Here we solve this controversy and show through polarization resolved Raman spectroscopy that thin multilayers do not undergo a structural phase transition typical of bulk crystals. As a consequence, a different stacking pattern is present in thin and bulk samples at the temperatures at which magnetism sets in and, according to previous first-principles simulations, this results in a different interlayer magnetic ordering. Our experimental findings provide evidence for the strong interplay between stacking order and magnetism in CrI$_3$, opening interesting perspectives to design the magnetic state of van der Waals multilayers.
We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe$_{2}$, WSe$_{2}$ and MoS$_{2}$ by encapsulation within few nanometer thick hBN. Encapsulation is shown to result in a significant reduction of the 10K excitonic linewidths down to $sim3.5 text{ meV}$ for n-MoSe$_{2}$, $sim5.0 text{ meV}$ for p-WSe$_{2}$ and $sim4.8 text{ meV}$ for n-MoS$_{2}$. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton emission in n-doped TMDCs and towards charged exciton emission in p-doped TMDCs. Moreover, we find that fully encapsulated MoS$_{2}$ shows resolvable exciton and trion emission even after high power density excitation in contrast to non-encapsulated materials. Our findings suggest that encapsulation of mechanically exfoliated few-monolayer TMDCs within nanometer thick hBN dramatically enhances optical quality, producing ultra-narrow linewidths that approach the homogeneous limit.
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