Search

We present a benchmarking protocol that combines the characterization of boron nitride (BN) crystals and films with the evaluation of the electronic properties of graphene on these substrates. Our study includes hBN crystals grown under different conditions and scalable BN films deposited by either chemical or physical vapor deposition (CVD or PVD). We explore the complete process from boron nitride growth, over its optical characterization by time-resolved cathodoluminescence (TRCL), to the optical and electronic characterization of graphene by Raman spectroscopy after encapsulation and Hall bar processing. Within our benchmarking protocol we achieve a homogeneous electronic performance within each Hall bar device through a fast and reproducible processing routine. We find that a free exciton lifetime of 1 ns measured on as-grown hBN crystals by TRCL is sufficient to achieve high graphene room temperature charge carrier mobilities of 80,000 cm$^2$/(Vs) at a carrier density of |n| = 10$^{12}$ cm$^{-2}$, while respective exciton lifetimes around 100 ps yield mobilities up to 30,000 cm$^2$/(Vs). For scalable PVD-grown BN films, we measure carrier mobilities exceeding 10,000 cm$^2$/(Vs) which correlates with a graphene Raman 2D peak linewidth of 22 cm$^{-1}$. Our work highlights the importance of the Raman 2D linewidth of graphene as a critical metric that effectively assesses the interface quality (i.e. surface roughness) to the BN substrate, which directly affects the charge carrier mobility of graphene. Graphene 2D linewidth analysis is suitable for all BN substrates and is particularly advantageous when TRCL or BN Raman spectroscopy cannot be applied to specific BN materials such as amorphous or thin films. This underlines the superior role of spatially-resolved spectroscopy in the evaluation of BN crystals and films for the use of high-mobility graphene devices., Comment: 18 pages, 11 figures more...

We present the electrostatic control of photoluminescence of monolayer MoS$_2$ at room temperature via integration of free-standing BaTiO$_3$ (BTO), a ferroelectric perovskite oxide, layers. We show that the use of BTO leads to highly tunable exciton emission of MoS$_2$ in a minimal range of gate voltages, effectively controlling the neutral excitons to charged excitons (trions) conversion. Due to BTO's ferroelectric polarization-induced doping we observe large peak emission shifts as well as a large and tunable A trion binding energy in the range of 40-100 meV. To further investigate the efficacy of electrostatic control, we compared our measurements with those carried out when the BTO is replaced by a hexagonal boron nitride (hBN) dielectric layer of comparable thickness, confirming BTO's superior gating properties and thus lower power consumption. Additionally, we take advantage of the ferroelectric switching of BTO by fabricating devices where the BTO layer is decoupled from the gate electrode with a SiO$_2$ layer. Choosing to isolate the BTO allows us to induce large remanent behavior of MoS$_2$'s excitonic features, observing hysteretic behavior in the peak energy ratio between A exciton and its trion, as well as hysteretic behavior in the doping-related trion energy shift. This study illustrates the rich physics involved in combining free-standing complex oxide layers with two-dimensional materials. more...

The wealth of complex polar topologies recently found in nanoscale ferroelectrics result from a delicate balance between the materials intrinsic tendency to develop a homogeneous polarization and the electric and mechanic boundary conditions imposed upon them. Ferroelectric dielectric interfaces are model systems where polarization curling originates from open circuit like electric boundary conditions, to avoid the build-up of polarization charges through the formation of flux closure domains that evolve into vortex like structures at the nanoscale. Interestingly, while ferroelectricity is known to couple strongly to strain (both homogeneous and inhomogeneous), the effect of mechanical constraints on thin film nanoscale ferroelectrics has been comparatively less explored because of the relative paucity of strain patterns that can be implemented experimentally. Here we show that the stacking of freestanding ferroelectric perovskite layers with controlled twist angles opens an unprecedented opportunity to tailor these topological nanostructures in a way determined by the lateral strain modulation associated to the twisting. Interestingly, we find that a peculiar pattern of polarization vortices and antivortices emerges from the flexoelectric coupling of polarization to strain gradients. This finding opens exciting opportunities to create two-dimensional high density vortex crystals that would allow us to explore novel physical effects and functionalities. more...

The electronic bandstructure of Au$_2$Pb has a Dirac cone which gaps when undergoing a structural transition into a low temperature superconducting phase. This suggests that the superconducting phase ($T_c=1.1$ K) might hold topological properties at the surface. Here we make Scanning Tunneling Microscopy experiments on the surface of superconducting Au$_2$Pb. We measure the superconducting gap and find a sizeable superconducting density of states at the Fermi level. We discuss possible origins for this finding in terms of superconductivity induced into surface states. more...

Paper has the potential to dramatically reduce the cost of electronic components. In fact, paper is 10 000 times cheaper than crystalline silicon, motivating the research to integrate electronic materials on paper substrates. Among the different electronic materials, van der Waals materials are attracting the interest of the scientific community working on paper-based electronics because of the combination of high electrical performance and mechanical flexibility. Up to now, different methods have been developed to pattern conducting, semiconducting and insulating van der Waals materials on paper but the integration of superconductors remains elusive. Here, the deposition of NbSe2, an illustrative van der Waals superconductor, on standard copy paper is demonstrated. The deposited NbSe2 films on paper display superconducting properties (e.g. observation of Meissner effect and resistance drop to zero-resistance state when cooled down below its critical temperature) similar to those of bulk NbSe2., Comment: 6 figures in main text, 8 figures in Supp. Info more...

Bound states in superconductors are expected to exhibit a spatially resolved electron-hole asymmetry which is the hallmark of their quantum nature. This asymmetry manifests as oscillations at the Fermi wavelength, which is usually tiny and thus washed out by thermal broadening or by scattering at defects. Here we demonstrate theoretically and confirm experimentally that, when coupled to magnetic impurities, bound states in a vortex core exhibit an emergent axial electron-hole asymmetry on a much longer scale, set by the coherence length. We study vortices in 2H-NbSe$_2$ and in 2H-NbSe$_{1.8}$S_{0.2}$ with magnetic impurities, characterizing these with detailed Hubbard-corrected density functional calculations. We find that the induced electron-hole imbalance depends on the band character of the superconducting material. Our results open interesting prospects for the study of coupled superconducting bound states. more...

The magnetoresistance of iron pnictide superconductors is often dominated by electron-electron correlations and deviates from the H$^2$ or saturating behaviors expected for uncorrelated metals. Contrary to similar Fe-based pnictide systems, the superconductor LaRu$_2$P$_2$ (T$_c$ = 4 K) shows no enhancement of electron-electron correlations. Here we report a non-saturating magnetoresistance deviating from the H$^2$ or saturating behaviors in LaRu$_2$P$_2$. We have grown and characterized high quality single crystals of LaRu$_2$P$_2$ and measured a magnetoresistance following H$^{1.3}$ up to 22 T. We discuss our result by comparing the bandstructure of LaRu$_2$P$_2$ with Fe based pnictide superconductors. The different orbital structures of Fe and Ru leads to a 3D Fermi surface with negligible bandwidth renormalization in LaRu$_2$P$_2$, that contains a large open sheet over the whole Brillouin zone. We show that the large magnetoresistance in LaRu$_2$P$_2$ is unrelated to the one obtained in materials with strong electron-electron correlations and that it is compatible instead with conduction due to open orbits on the rather complex Fermi surface structure of LaRu$_2$P$_2$., Comment: 12 pages, 4 figures more...

We fabricate large-area atomically thin MoS$_2$ layers through the direct transformation of crystalline molybdenum MoS$_2$ (MoO$_3$) by sulfurization at relatively low temperatures. The obtained MoS2 sheets are polycrystalline (~10-20 nm single-crystal domain size) with areas of up to 300x300 um$^2$ with 2-4 layers in thickness and show a marked p-type behaviour. The synthesized films are characterized by a combination of complementary techniques: Raman spectroscopy, X-ray diffraction, transmission electron microscopy and electronic transport measurements., Comment: 6 figures in main text, 2 figures in supp. info more...

We present magnetoresistivity measurements in high-quality single crystals of the Nowotny chimney ladder compound Ru$_2$Sn$_3$. We find a linear and nonsaturating magnetoresistance up to 20 T. The magnetoresistance changes with the magnetic field orientation at small magnetic fields, from a positive to a negative curvature. Above 5 T, the magnetoresistance shows no sign of saturation up to 20 T for any measured angle. The shape of the anisotropy in the magnetoresistance remains when increasing temperature and Kohler's rule is obeyed. We associate the linear and nonsaturating magnetoresistance to a small Fermi surface with hot spots, possibly formed as a consequence of the structural transition. We discuss the relevance of electron-electron interactions under magnetic fields and aspects of the topologically nontrivial properties expected in Ru$_2$Sn$_3$., Comment: 6 pages, 5 figures more...

The successful application of titanium oxide-graphene hybrids in the fields of photocatalysis, photovoltaics and photodetection strongly depends on the interfacial contact between both materials. The need to provide a good coupling between the enabling conductor and the photoactive phase prompted us to directly grow conducting graphenic structures on TiO2 crystals. We here report on the direct synthesis of tailored graphenic structures by using Plasma Assisted Chemical Vapour Deposition that present a clean junction with the prototypical titanium oxide (110) surface. Chemical analysis of the interface indicates chemical bonding between both materials. Photocurrent measurements under UV light illumination manifest that the charge transfer across the interface is efficient. Moreover, the influence of the synthesis atmosphere, gas precursor (C2H2) and diluents (Ar, O2), on the interface and on the structure of the as-grown graphenic material is assessed. The inclusion of O2 promotes vertical growth of partially oxidized carbon nanodots/rods with controllable height and density. The deposition with Ar results in continuous graphenic films with low resistivity (6.8x10-6 ohm x m). The synthesis protocols developed here are suitable to produce tailored carbon-semiconductor structures on a variety of practical substrates as thin films, pillars or nanoparticles., Comment: 24 pages, 8 figures, original research paper more...

Franckeite is a naturally occurring layered mineral with a structure composed of alternating stacks of SnS2-like and PbS-like layers. Although this superlattice is composed of a sequence of isotropic two-dimensional layers, it exhibits a spontaneous rippling that makes the material structurally anisotropic. We demonstrate that this rippling comes hand in hand with an inhomogeneous in-plane strain profile and anisotropic electrical, vibrational and optical properties. We argue that this symmetry breakdown results from a spatial modulation of the van der Waals interaction between layers due to the SnS2-like and PbS-like lattices incommensurability., Comment: 6 main text figures, Supp. Info. available upon request more...

Here, we propose a method to determine the thickness of the most common transition metal dichalcogenides (TMDCs) placed on the surface of transparent stamps, used for the deterministic placement of two-dimensional materials, by analyzing the red, green and blue channels of transmission-mode optical microscopy images of the samples. In particular, the blue channel transmittance shows a large and monotonic thickness dependence, making it a very convenient probe of the flake thickness. The method proved to be robust given the small flake-to-flake variation and the insensitivity to doping changes of MoS2. We also tested the method for MoSe2, WS2 and WSe2. These results provide a reference guide to identify the number of layers of this family of materials on transparent substrates only using optical microscopy., Comment: 4 figures in main text, 2 figures in supp. info more...

We report the isolation of thin flakes of cylindrite, a naturally occurring van der Waals superlattice, by means of mechanical and liquid phase exfoliation. We find that this material is a heavily doped p-type semiconductor with a narrow gap (<0.85 eV) with intrinsic magnetic interactions that are preserved even in the exfoliated nanosheets. Due to its environmental stability and high electrical conductivity, cylindrite can be an interesting alternative to the existing two-dimensional magnetic materials., Comment: 5 figures in main text, 1 supp. info. figure. Available open access at the publisher's web more...

Technologically useful and robust graphene-based interfaces for devices require the introduction of highly selective, stable, and covalently bonded functionalities on the graphene surface, whilst essentially retaining the electronic properties of the pristine layer. This work demonstrates that highly controlled, ultrahigh vacuum covalent chemical functionalization of graphene sheets with a thiol-terminated molecule provides a robust and tunable platform for the development of hybrid nanostructures in different environments. We employ this facile strategy to covalently couple two representative systems of broad interest: metal nanoparticles, via S-metal bonds, and thiol-modified DNA aptamers, via disulfide bridges. Both systems, which have been characterized by a multi-technique approach, remain firmly anchored to the graphene surface even after several washing cycles. Atomic force microscopy images demonstrate that the conjugated aptamer retains the functionality required to recognize a target protein. This methodology opens a new route to the integration of high-quality graphene layers into diverse technological platforms, including plasmonics, optoelectronics, or biosensing. With respect to the latter, the viability of a thiol-functionalized chemical vapor deposition graphene-based solution-gated field-effect transistor array was assessed. more...

A gel consists of a network of particles or molecules formed for example using the sol-gel process, by which a solution transforms into a porous solid. Particles or molecules in a gel are mainly organized on a scaffold that makes up a porous system. Quantized vortices in type II superconductors mostly form spatially homogeneous ordered or amorphous solids. Here we present high-resolution imaging of the vortex lattice displaying dense vortex clusters separated by sparse or entirely vortex-free regions in $\beta$-Bi$_2$Pd superconductor. We find that the intervortex distance diverges upon decreasing the magnetic field and that vortex lattice images follow a multifractal behavior. These properties, characteristic of gels, establish the presence of a novel vortex distribution, distinctly different from the well-studied disordered and glassy phases observed in high-temperature and conventional superconductors. The observed behavior is caused by a scaffold of one-dimensional structural defects with enhanced stress close to the defects. The vortex gel might often occur in type-II superconductors at low magnetic fields. Such vortex distributions should allow to considerably simplify control over vortex positions and manipulation of quantum vortex states. more...

The antiferromagnet Mn$_5$Si$_3$ has recently attracted attention because a noncollinear spin arrangement has been shown to produce a topological anomalous Hall effect and an inverse magnetocaloric effect. Here we synthesize single crystals of Mn$_5$Si$_3$ using flux growth. We determine the phase diagram through magnetization and measure the magnetoresistance and the Hall effect. We find the collinear and noncollinear antiferromagnetic phases at low temperatures and, in addition, a third magnetic phase, in between the two antiferromagnetic phases which has ferromagnetic character. The latter magnetic phase might be caused by strain produced by Cu inclusions that lead to quenched fluctuations of the mixed character magnetic ordering in this compound. more...

Gallium selenide (GaSe) is a novel two-dimensional material, which belongs to the layered III-VIA semiconductors family and attracted interest recently as it displays single-photon emitters at room temperature and strong optical non-linearity. Nonetheless, few-layer GaSe is not stable under ambient conditions and it tends to degrade over time. Here we combine atomic force microscopy, Raman spectroscopy and optoelectronic measurements in photodetectors based on thin GaSe to study its long-term stability. We found that the GaSe flakes exposed to air tend to decompose forming firstly amorphous selenium and Ga2Se3 and subsequently Ga2O3. While the first stage is accompanied by an increase in photocurrent, in the second stage we observe a decrease in photocurrent which leads to the final failure of GaSe photodetectors. Additionally, we found that the encapsulation of the GaSe photodetectors with hexagonal boron nitride (h-BN) can protect the GaSe from degradation and can help to achieve long-term stability of the devices., Comment: 23 pages, 5 figures, supporting information more...

We study mechanically exfoliated nanosheets of franckeite by quantitative optical microscopy. The analysis of transmission mode and epi-illumination mode optical microscopy images provides a rapid method to estimate the thickness of the exfoliated flakes at first glance. A quantitative analysis of the optical contrast spectra by means of micro-reflectance allows one to determine the refractive index of franckeite in a broad range of the visible spectrum through a fit of the acquired spectra to a Fresnel law based model., Comment: Main text (6 figures) + Supp. Info. (6 figures) more...

Many practical applications of high T$_c$ superconductors involve layered materials and magnetic fields applied on an arbitrary direction with respect to the layers. When the anisotropy is very large, Cooper pair currents can circulate either within or perpendicular to the layers. Thus, tilted magnetic fields lead to intertwined lattices of Josephson and Abrikosov vortices, with quantized circulation across and within layers, respectively. Transport in such intertwined lattices has been studied in detail, but direct observation and manipulation of vortices remains challenging. Here we present magnetic force microscopy experiments in tilted magnetic fields in the extremely quasi-two dimensional superconductor $Bi_{2}Sr_{2}CaCu_{2}O_{8}$. We trigger Abrikosov vortex motion in between Josephson vortices, and find that Josephson vortices in different layers can be brought on top of each other. Our measurements suggest that intertwined lattices in tilted magnetic fields can be intrinsically easy to manipulate thanks to the mutual interaction between Abrikosov and Josephson vortices. more...

We show that biaxial strain induces alternating tetragonal superconducting and orthorhombic nematic domains in Co substituted CaFe2As2. We use Atomic Force, Magnetic Force and Scanning Tunneling Microscopy (AFM, MFM and STM) to identify the domains and characterize their properties, finding in particular that tetragonal superconducting domains are very elongated, more than several tens of micron long and about 30 nm wide, have the same Tc than unstrained samples and hold vortices in a magnetic field. Thus, biaxial strain produces a phase separated state, where each phase is equivalent to what is found at either side of the first order phase transition between antiferromagnetic orthorhombic and superconducting tetragonal phases found in unstrained samples when changing Co concentration. Having such alternating superconducting domains separated by normal conducting domains with sizes of order of the coherence length opens opportunities to build Josephson junction networks or vortex pinning arrays and suggests that first order quantum phase transitions lead to nanometric size phase separation under the influence of strain. more...

We examine the magnetic easy-axis directions of stoichiometric magnetite films grown on SrTiO3:Nb by infrared pulsed-laser deposition. Spin-polarized low-energy electron microscopy reveals that the individual magnetic domains are magnetized along the in-plane <100> film directions. Magneto-optical Kerr effect measurements show that the maxima of the remanence and coercivity are also along in-plane <100> film directions. This easy-axis orientation differs from bulk magnetite and films prepared by other techniques, establishing that the magnetic anisotropy can be tuned by film growth., Comment: 3 pages, 3 figures more...

The magnetic properties of La0.7Ca0.3MnO3 (LCMO) manganite thin films were studied with magnetometry and ferromagnetic resonance as a function of film thickness. They maintain the colossal magnetoresistance behavior with a pronounced metal-insulator transition around 150-200 K, except for the very thinnest films studied (3 nm). Nevertheless, LCMO films as thin as 3 nm remain ferromagnetic, without a decrease in saturation magnetization, indicating an absence of dead-layers, although below approx. 6 nm the films remain insulating at low temperature. Magnetization hysteresis loops reveal that the magnetic easy axes lie in the plane of the film for thicknesses in the range of 4-15 nm. Ferromagnetic resonance studies confirm that the easy axes are in-plane, and find a biaxial symmetry in-plane with two, perpendicular easy axes. The directions of the easy axes with respect to the crystallographic directions of the cubic SrTiO3 substrate differ by 45 degrees in 4 nm and 15 nm thick LCMO films., Comment: Presented at Intermag conference (Madrid, 2008). Accepted for publication in IEEE Transactions on Magnetics more...