arXiv subjects

Enrico Giannini

Publications and source records attributed to Enrico Giannini.

At least 37 records · Page 2Linked to original sources

arXiv2019

Determining the phase diagram of atomically thin layered antiferromagnet CrCl$_3$

Changes in the spin configuration of atomically-thin, magnetic van-der-Waals multilayers can cause drastic modifications in their opto-electronic properties. Conversely, the opto-electronic response of these systems provides information about the magnetic state, very difficult to obtain otherwise. Here we show that in CrCl$_3$ multilayers, the dependence of the tunnelling conductance on applied magnetic field ($H$), temperature ($T$), and number of layers ($N$) tracks the evolution of the magnetic state, enabling the magnetic phase diagram of these systems to be determined experimentally. Besides a high-field spin-flip transition occurring for all thicknesses, the in-plane magnetoconductance exhibits an even-odd effect due to a low-field spin-flop transition. If the layer number $N$ is even, the transition occurs at $μ_0 H \sim 0$ T due to the very small in-plane magnetic anisotropy, whereas for odd $N$ the net magnetization of the uncompensated layer causes the transition to occur at finite $H$. Through a quantitative analysis of the phenomena, we determine the interlayer exchange coupling as well as the staggered magnetization, and show that in CrCl$_3$ shape anisotropy dominates. Our results reveal the rich behaviour of atomically-thin layered antiferromagnets with weak magnetic anisotropy.

cond-mat.mes-hall↗

arXiv2019

Spin-flop transition in atomically thin MnPS$_3$ crystals

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 $T\simeq 78$ 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.

cond-mat.mes-hall↗

arXiv2019

Low-temperature monoclinic layer stacking in atomically thin CrI$_3$ crystals

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.

cond-mat.mes-hall↗

arXiv2019

Probing magnetism in 2D materials at the nanoscale with single spin microscopy

The recent discovery of ferromagnetism in 2D van der Waals (vdw) crystals has generated widespread interest, owing to their potential for fundamental and applied research. Advancing the understanding and applications of vdw magnets requires methods to quantitatively probe their magnetic properties on the nanoscale. Here, we report the study of atomically thin crystals of the vdw magnet CrI$_3$ down to individual monolayers using scanning single-spin magnetometry, and demonstrate quantitative, nanoscale imaging of magnetisation, localised defects and magnetic domains. We determine the magnetisation of CrI$_3$ monolayers to be $\approx16~μ_B/$nm$^2$ and find comparable values in samples with odd numbers of layers, whereas the magnetisation vanishes when the number of layers is even. We also establish that this inscrutable even-odd effect is intimately connected to the material structure, and that structural modifications can induce switching between ferro- and anti-ferromagnetic interlayer ordering. Besides revealing new aspects of magnetism in atomically thin CrI$_3$ crystals, these results demonstrate the power of single-spin scanning magnetometry for the study of magnetism in 2D vdw magnets.

cond-mat.mes-hall↗

arXiv2018

Energy-dependent spatial texturing of the charge order in $1T$-Cu$_x$TiSe$_2$

We report a detailed study of the microscopic effects of Cu intercalation on the charge density wave (CDW) in 1\textit{T}-Cu$_x$TiSe$_2$. Scanning tunneling microscopy and spectroscopy (STM/STS) reveal a unique, Cu driven spatial texturing of the charge ordered phase, with the appearance of energy dependent CDW patches and sharp $π$-phase shift domain walls ($π$DWs). The energy and doping dependencies of the patchwork are directly linked to the inhomogeneous potential landscape due to the Cu intercalants. They imply a CDW gap with unusual features, including a large amplitude, the opening below the Fermi level and a shift to higher binding energy with electron doping. Unlike the patchwork, the $π$DWs occur independently of the intercalated Cu distribution. They remain atomically sharp throughout the investigated phase diagram and occur both in superconducting and non-superconducting specimen. These results provide unique atomic-scale insight on the CDW ground state, questioning the existence of incommensurate CDW domain walls and contributing to understand its formation mechanism and interplay with superconductivity.

cond-mat.str-el↗

arXiv2018

Microfocus laser-ARPES on encapsulated mono-, bi-, and few-layer 1T'-WTe$_2$

Two-dimensional crystals of semimetallic van der Waals materials hold much potential for the realization of novel phases, as exemplified by the recent discoveries of a polar metal in few layer 1T'-WTe$_2$ and of a quantum spin Hall state in monolayers of the same material. Understanding these phases is particularly challenging because little is known from experiment about the momentum space electronic structure of ultrathin crystals. Here, we report direct electronic structure measurements of exfoliated mono-, bi-, and few-layer 1T'-WTe$_2$ by laser-based micro-focus angle resolved photoemission. This is achieved by encapsulating with monolayer graphene a flake of WTe$_2$ comprising regions of different thickness. Our data support the recent identification of a quantum spin Hall state in monolayer 1T'-WTe$_2$ and reveal strong signatures of the broken inversion symmetry in the bilayer. We finally discuss the sensitivity of encapsulated samples to contaminants following exposure to ambient atmosphere.

cond-mat.mtrl-sci↗

arXiv2018

Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI$_3$

Magnetic layered van der Waals crystals are an emerging class of materials giving access to new physical phenomena, as illustrated by the recent observation of 2D ferromagnetism in Cr2Ge2Te6 and CrI3. Of particular interest in semiconductors is the interplay between magnetism and transport, which has remained unexplored. Here we report first magneto-transport measurements on exfoliated CrI3 crystals. We find that tunneling conduction in the direction perpendicular to the crystalline planes exhibits a magnetoresistance as large as 10 000 %. The evolution of the magnetoresistance with magnetic field and temperature reveals that the phenomenon originates from multiple transitions to different magnetic states, whose possible microscopic nature is discussed on the basis of all existing experimental observations. This observed dependence of the conductance of a tunnel barrier on its magnetic state is a new phenomenon that demonstrates the presence of a strong coupling between transport and magnetism in magnetic van der Waals semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Holographic imaging of the complex charge density wave order parameter

The charge density wave (CDW) in solids is a collective ground state combining lattice distortions and charge ordering. It is defined by a complex order parameter with an amplitude and a phase. The amplitude and wavelength of the charge modulation are readily accessible to experiment. However, accurate measurements of the corresponding phase are significantly more challenging. Here we combine reciprocal and real space information to map the full complex order parameter based on topographic scanning tunneling microscopy (STM) images. Our technique overcomes limitations of earlier Fourier space based techniques to achieve distinct amplitude and phase images with high spatial resolution. Applying this analysis to transition metal dichalcogenides provides striking evidence that their CDWs consist of three individual charge modulations whose ordering vectors are connected by the fundamental rotational symmetry of the crystalline lattice. Spatial variations in the relative phases of these three modulations account for the different contrasts often observed in STM topographic images. Phase images further reveal topological defects and discommensurations, a singularity predicted by theory for a nearly commensurate CDW. Such precise real space mapping of the complex order parameter provides a powerful tool for a deeper understanding of the CDW ground state whose formation mechanisms remain largely unclear.

cond-mat.str-el↗

arXiv2017

Dimensional cross-over of the charge density wave order parameter in thin exfoliated 1T-VSe$_2$

The capability to isolate one to few unit-cell thin layers from the bulk matrix of layered compounds opens fascinating prospects to engineer novel electronic phases. However, a comprehensive study of the thickness dependence and of potential extrinsic effects are paramount to harness the electronic properties of such atomic foils. One striking example is the charge density wave (CDW) transition temperature in layered dichalcogenides whose thickness dependence remains unclear in the ultrathin limit. Here we present a detailed study of the thickness and temperature dependences of the CDW in VSe$_2$ by scanning tunnelling microscopy (STM). We show that mapping the real-space CDW periodicity over a broad thickness range unique to STM provides essential insight. We introduce a robust derivation of the local order parameter and transition temperature based on the real space charge modulation amplitude. Both quantities exhibit a striking non-monotonic thickness dependence that we explain in terms of a 3D to 2D dimensional crossover in the FS topology. This finding highlights thickness as a true tuning parameter of the electronic ground state and reconciles seemingly contradicting thickness dependencies determined in independent transport studies.

cond-mat.str-el↗

arXiv2016

Direct Observation of Long-range field-effect from gate tuning of non-local conductivity

We report the observation of an unexpected, long-range field-effect in WTe$_2$ devices, leading to large gate-induced changes of the transport properties of crystals much thicker than the electrostatic screening length. The phenomenon --which manifests itself very differently from the conventional field-effect-- originates from the non-local nature of transport in the devices that are thinner than the carrier mean free path, because of the dominant role of surface scattering. We reproduce theoretically the gate dependence of the measured classical and quantum magneto-transport in all detail, and show that the phenomenon is caused by the gate-tuning of the bulk carrier mobility by changing the scattering at the surface. Our results demonstrate the possibility to gate tune the electronic properties deep in the interior of conducting materials, avoiding limitations imposed by electrostatic screening.

cond-mat.mes-hall↗

arXiv2016

High-pressure melt growth and transport properties of SiP, SiAs, GeP, and GeAs 2D layered semiconductors

Silicon and Germanium monopnictides SiP, SiAs, GeP and GeAs form a family of 2D layered semiconductors. We have succeeded in growing bulk single crystals of these compounds by melt-growth under high pressure (0.5-1 GPa) in a cubic anvil hot press. Large (mm-size), shiny, micaceous crystals of GeP, GeAs and SiAs were obtained, and could be exfoliated into 2D flakes. Small and brittle crystals of SiP were yielded by this method. High-pressure sintered polycrystalline SiP and GeAs have also been successfully used as a precursor in the Chemical Vapor Transport growth of these crystals in the presence of I$_{2}$ as a transport agent. All compounds are found to crystallize in the expected layered structure and do not undergo any structural transition at low temperature, as shown by Raman spectroscopy down to T=5K. All materials exhibit a semiconducting behavior. The electrical resistivity of GeP, GeAs and SiAs is found to depend on temperature following a 2D-Variable Range Hopping conduction mechanism. The availability of bulk crystals of these compounds opens new perspectives in the field of 2D semiconducting materials for device applications.

cond-mat.mtrl-sci↗

arXiv2015

Tuning Magnetotransport in a Compensated Semimetal at the Atomic Scale

Either in bulk form, or when exfoliated into atomically thin crystals, layered transition metal dichalcogenides are continuously leading to the discovery of new phenomena. The latest example is provided by 1T'-WTe$_2$, a semimetal recently found to exhibit the largest known magnetoresistance in bulk crystals, and predicted to become a two-dimensional topological insulator in strained monolayers. Here, we show that reducing the thickness through facile exfoliation provides an effective experimental knob to tune the electronic properties of WTe$_2$, which allows us to identify the microscopic mechanisms responsible for the observed classical and quantum magnetotransport down to the ultimate atomic scale. We find that the longitudinal resistance and the very unconventional B-dependence of the Hall resistance are reproduced quantitatively in terms of a classical two-band model for crystals as thin as six monolayers, and that for thinner crystals a crossover to an insulating, Anderson-localized state occurs. Besides establishing the origin of the very large magnetoresistance of bulk WTe$_2$, our results represent the first, complete validation of the classical theory for two-band electron-hole transport, and indicate that atomically thin WTe$_2$ layers remain gapless semimetals, from which we conclude that searching for a topological insulating state by straining monolayers is a challenging, but feasible experiment.

cond-mat.mes-hall↗

arXiv2015

Indirect-to-direct band-gap crossover in few-layer MoTe$_2$

We study the evolution of the band-gap structure in few-layer MoTe$_2$ crystals, by means of low-temperature micro-reflectance (MR) and temperature-dependent photoluminescence (PL) measurements. The analysis of the measurements indicate that, in complete analogy with other semiconducting transition metal dichalchogenides (TMDs), the dominant PL emission peaks originate from direct transitions associated to recombination of excitons and trions. When we follow the evolution of the PL intensity as a function of layer thickness, however, we observe that MoTe$_2$ behaves differently from other semiconducting TMDs investigated earlier. Specifically, the exciton PL yield (integrated PL intensity) is identical for mono and bilayer and it starts decreasing for trilayers. A quantitative analysis of this behavior and of all our experimental observations is fully consistent with mono and bilayer MoTe$_2$ being direct band-gap semiconductors, with tetralayer MoTe$_2$ being an indirect gap semiconductor, and with trilayers having nearly identical direct and indirect gaps.This conclusion is different from the one reached for other recently investigated semiconducting transition metal dichalcogenides, for which only monolayers are found to be direct band-gap semiconductors, with thicker layers having indirect band gaps that are significantly smaller, by hundreds of meV, than the direct gap. We discuss the relevance of our findings for experiments of fundamental interest and possible future device applications.

cond-mat.mes-hall↗

arXiv2014

Bi2Te_xSe_y series studied by resistivity and thermopower

We study the detailed temperature and composition dependence of the resistivity, $ρ(T)$, and thermopower, $S(T)$, for a series of layered bismuth chalcogenides Bi$_2$Te$_{3-x}$Se$_x$, and report the stoichiometry dependence of the optical band gap. In the resistivity of the most compensated member, Bi$_2$Te$_{2.1}$Se$_{0.9}$, we find a low-temperature plateau whose onset temperature correlates with the high-temperature activation energy. For the whole series $S(T)$ can be described by a simple model for an extrinsic semiconductor. By substituting Se for Te, the Fermi level is tuned from the valence band into the conduction band. The maximum values of $S(T)$, bulk band gap as well the activation energy in the resistivity are found for $x \approx 0.9$.

cond-mat.mtrl-sci↗

arXiv2014

Surface transport and band gap structure of exfoliated 2H-MoTe$_2$ crystals

Semiconducting transition metal dichalcogenides (TMDs) have emerged as materials that can be used to realize two-dimensional (2D) crystals possessing rather unique transport and optical properties. Most research has so far focused on sulfur and selenium compounds, while tellurium-based materials attracted little attention so far. As a first step in the investigation of Te-based semiconducting TMDs in this context, we have studied MoTe$_2$ crystals with thicknesses above 4 nm, focusing on surface transport and a quantitative determination of the gap structure. Using ionic-liquid gated transistors, we show that ambipolar transport at the surface of the material is reproducibly achieved, with hole and electron mobility values between 10 and 30 cm$^2$/Vs at room temperature. The gap structure is determined through three different techniques: ionic-liquid gated transistors and scanning tunneling spectroscopy, that allow the measurement of the indirect gap ($E_{ind}$), and optical transmission spectroscopy on crystals of different thickness, that enables the determination of both the direct ($E_{dir}$) and the indirect gap. We find that at room temperature $E_{ind}$ = 0.88 eV and $E_{dir}$ = 1.02 eV. Our results suggest that thin MoTe$_2$ layers may exhibit a transition to a direct gap before mono-layer thickness. They should also drastically extend the range of direct gaps accessible in 2D semiconducting TMDs.

cond-mat.mes-hall↗

arXiv2014

Improved chemical vapor transport growth of transition metal dichalcogenides

In the crystal growth of transition metal dichalcogenides by the Chemical Vapor Transport method (CVT), the choice of the transport agent plays a key role. We have investigated the effect of various chemical elements and compounds on the growth of TiSe2, MoSe2, TaS2 and TaSe2 and found that pure I2 is the most suitable for growing TiSe2, whereas transition metal chlorides perform best with Mo- and Ta- chalcogenides. The use of TaCl5 as a transport agent in the CVT process allows to selectively growth either polymorph of TaS2 and TaSe2 and the optimum growth conditions are reported. Moreover, by using TaCl5 and tuning the temperature and the halogen starting ratio, it was possible to grow whiskers of the compounds TaS2, TaSe2, TaTe2, TaS3 and TaSe3.

cond-mat.mtrl-sci↗

arXiv2012

Optical properties of Bi2Te2Se at ambient and high pressure

The temperature dependence of the complex optical properties of the three-dimensional topological insulator Bi2Te2Se is reported for light polarized in the a-b planes at ambient pressure, as well as the effects of pressure at room temperature. This material displays a semiconducting character with a bulk optical gap of 300 meV at 295 K. In addition to the two expected infrared-active vibrations observed in the planes, there is additional fine structure that is attributed to either the removal of degeneracy or the activation of Raman modes due to disorder. A strong impurity band located at 200 cm^{-1} is also observed. At and just above the optical gap, several interband absorptions are found to show a strong temperature and pressure dependence. As the temperature is lowered these features increase in strength and harden. The application of pressure leads to a very abrupt closing of the gap above 8 GPa, and strongly modifies the interband absorptions in the mid-infrared spectral range. While ab initio calculations fail to predict the collapse of the gap, they do successfully describe the size of the band gap at ambient pressure, and the magnitude and shape of the optical conductivity.

cond-mat.mtrl-sci↗

arXiv2012

Temperature and time scaling of the peak-effect vortex configuration in FeTe$_{0.7}$Se$_{0.3}$

An extensive study of the magnetic properties of FeTe$_{0.7}$Se$_{0.3}$ crystals in the superconducting state is presented. We show that weak collective pinning, originating from spatial variations of the charge carrier mean free path ($δl$ pinning), rules in this superconductor. Our results are compatible with the nanoscale phase separation observed on this compound and indicate that in spite of the chemical inhomogeneity spatial fluctuations of the critical temperature are not important for pinning. A power law dependence of the magnetization vs time, generally interpreted as signature of single vortex creep regime, is observed in magnetic fields up to $8 ~ T$. For magnetic fields applied along the c axis of the crystal the magnetization curves exhibit a clear peak effect whose position shifts when varying the temperature, following the same dependence as observed in YBa$_2$Cu$_3$O$_{7-δ}$. The time and temperature dependence of the peak position has been investigated. We observe that the occurrence of the peak at a given magnetic field determines a specific vortex configuration that is independent on the temperature. This result indicates that the influence of the temperature on the vortex-vortex and vortex-defect interactions leading to the peak effect in FeTe$_{0.7}$Se$_{0.3}$ is negligible in the explored range of temperatures.

cond-mat.supr-con↗