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Ignacio Gutiérrez-Lezama

Publications and source records attributed to Ignacio Gutiérrez-Lezama.

29 records · Page 2Linked to original sources

Synthetic Semimetals with van der Waals Interfaces

The assembly of suitably designed van der Waals (vdW) heterostructures represents a new approach to produce artificial systems with engineered electronic properties. Here, we apply this strategy to realize synthetic semimetals based on vdW interfaces formed by two different semiconductors. Guided by existing ab-initio calculations, we select WSe$_2$ and SnSe$_2$ mono and multilayers to assemble vdW interfaces, and demonstrate the occurrence of semimetallicity by means of different transport experiments. Semimetallicity manifests itself in a finite minimum conductance upon sweeping the gate over a large range in ionic liquid gated devices, which also offer spectroscopic capabilities enabling the quantitative determination of the band overlap. The semimetallic state is additionally revealed in Hall effect measurements by the coexistence of electrons and holes, observed by either looking at the evolution of the Hall slope with sweeping the gate voltage or with lowering temperature. Finally, semimetallicity results in the low-temperature metallic conductivity of interfaces of two materials that are themselves insulating. These results demonstrate the possibility to implement a state of matter that had not yet been realized in vdW interfaces, and represent a first step towards using these interfaces to engineer topological or excitonic insulating states.

cond-mat.mes-hall↗

Scanning Tunneling Microscopy of an Air Sensitive Dichalcogenide Through an Encapsulating Layer

Many atomically thin exfoliated 2D materials degrade when exposed to ambient conditions. They can be protected and investigated by means of transport and optical measurements if they are encapsulated between chemically inert single layers in the controlled atmosphere of a glove box. Here, we demonstrate that the same encapsulation procedure is also compatible with scanning tunneling microscopy (STM) and spectroscopy (STS). To this end, we report a systematic STM/STS investigation of a model system consisting of an exfoliated 2H-NbSe2 crystal capped with a protective 2H-MoS2 monolayer. We observe different electronic coupling between MoS2 and NbSe2, from a strong coupling when their lattices are aligned within a few degrees to 2 essentially no coupling for 30° misaligned layers. We show that STM always probes intrinsic NbSe2 properties such as the superconducting gap and charge density wave at low temperature when setting the tunneling bias inside the MoS2 band gap, irrespective of the relative angle between the NbSe2 and MoS2 lattices. This study demonstrates that encapsulation is fully compatible with STM/STS investigations of 2D materials.

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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.

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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↗

Lithium-ion conducting glass ceramics for electrostatic gating

We explore solid electrolytes for electrostatic gating using field-effect transistors (FETs) in which thin WSe$_2$ crystals are exfoliated and transferred onto a lithium-ion conducting glass ceramic substrate. For negative gate voltages ($V_G < 0$) the devices work equally well as ionic liquid gated FETs while offering specific advantages, whereas no transistor action is seen for $V_G>0$. For $V_G <0$ the devices can nevertheless be driven into the ambipolar injection regime by applying a large source-drain bias, and strong electroluminescence is observed when direct band-gap WSe$_2$ monolayers are used. Detecting and imaging the emitted light is much simpler in these FETs as compared to ionic liquid gated transistors, because the semiconductor surface is exposed (i.e., not covered by another material). Our results show that solid electrolytes are complementary to existing liquid gates, as they enable experiments not possible when the semiconductor is buried under the liquid itself.

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Semiconducting van der Waals Interfaces as Artificial Semiconductors

Recent technical progress demonstrates the possibility of stacking together virtually any combination of atomically thin crystals of van der Waals bonded compounds to form new types of heterostructures and interfaces. As a result, there is the need to understand at a quantitative level how the interfacial properties are determined by the properties of the constituent 2D materials. We address this problem by studying the transport and optoelectronic response of two different interfaces based on transition-metal dichalcogenide monolayers, namely WSe2-MoSe2 and WSe2-MoS2. By exploiting the spectroscopic capabilities of ionic liquid gated transistors, we show how the conduction and valence bands of the individual monolayers determine the bands of the interface, and we establish quantitatively (directly from the measurements) the energetic alignment of the bands in the different materials as well as the magnitude of the interfacial band gap. Photoluminescence and photocurrent measurements allow us to conclude that the band gap of the WSe2-MoSe2 interface is direct in k space, whereas the gap of WSe2/MoS2 is indirect. For WSe2/MoSe2, we detect the light emitted from the decay of interlayer excitons and determine experimentally their binding energy using the values of the interfacial band gap extracted from transport measurements. The technique that we employed to reach this conclusion demonstrates a rather-general strategy for characterizing quantitatively the interfacial properties in terms of the properties of the constituent atomic layers. The results presented here further illustrate how van der Waals interfaces of two distinct 2D semiconducting materials are composite systems that truly behave as artificial semiconductors, the properties of which can be deterministically defined by the selection of the appropriate constituent semiconducting monolayers.

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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↗

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.

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Ambipolar Light-Emitting Transistors on Chemical Vapor Deposited Monolayer MoS2

We realize and investigate ionic liquid gated field-effect transistors (FETs) on large-area MoS2 monolayers grown by chemical vapor deposition (CVD). Under electron accumulation, the performance of these devices is comparable to that of FETs based on exfoliated flakes. FETs on CVD-grown material, however, exhibit clear ambipolar transport, which for MoS2 monolayers had not been reported previously. We exploit this property to estimate the bandgap Δ of monolayer MoS2 directly from the device transfer curves and find Δ $\approx$ 2.4-2.7 eV. In the ambipolar injection regime, we observe electroluminescence due to exciton recombination in MoS2, originating from the region close to the hole-injecting contact. Both the observed transport properties and the behavior of the electroluminescence can be consistently understood as due to the presence of defect states at an energy of 250-300 meV above the top of the valence band, acting as deep traps for holes. Our results are of technological relevance, as they show that devices with useful optoelectronic functionality can be realized on large-area MoS2 monolayers produced by controllable and scalable techniques.

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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.

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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.

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