arXiv subjects

Alberto F. Morpurgo

Publications and source records attributed to Alberto F. Morpurgo.

At least 73 records · Page 4Linked to original sources

arXiv2016

Origin and magnitude of 'designer' spin-orbit interaction in graphene on semiconducting transition metal dichalcogenides

We use a combination of experimental techniques to demonstrate a general occurrence of spin-orbit interaction (SOI) in graphene on transition metal dichalcogenide (TMD) substrates. Our measurements indicate that SOI is ultra-strong and extremely robust, despite it being merely interfacially-induced, with neither graphene nor the TMD substrates changing their structure. This is found to be the case irrespective of the TMD material used, of the transport regime, of the carrier type in the graphene band, and of the thickness of the graphene multilayer. Specifically, we perform weak antilocalization measurements as the simplest and most general diagnostic of SOI, and show that the spin relaxation time is very short in all cases regardless of the elastic scattering time. Such a short spin-relaxation time strongly suggests that the SOI originates from a modification of graphene band structure. We confirmed this expectation by measuring a gate-dependent beating, and a corresponding frequency splitting, in the low-field Shubnikov-de Haas magneto-resistance oscillations in high quality bilayer graphene on WSe$_2$. These measurements provide an unambiguous diagnostic of a SOI-induced splitting in the electronic band structure, and their analysis allows us to determine the SOI coupling constants for the Rashba term and the so-called spin-valley coupling term, i.e., the terms that were recently predicted theoretically for interface-induced SOI in graphene. The magnitude of the SOI splitting is found to be on the order of 10 meV, more than 100 times greater than the SOI intrinsic to graphene. Both the band character of the interfacially induced SOI, as well as its robustness and large magnitude make graphene-on-TMD a promising system to realize and explore a variety of spin-dependent transport phenomena, such as, in particular, spin-Hall and valley-Hall topological insulating states.

cond-mat.mes-hall↗

arXiv2016

Tuning the charge transfer in Fx-TCNQ/rubrene single-crystal interfaces

Interfaces formed by two different organic semiconductors often exhibit a large conductivity, originating from transfer of charge between the constituent materials. The precise mechanisms driving charge transfer and determining its magnitude remain vastly unexplored, and are not understood microscopically. To start addressing this issue, we have performed a systematic study of highly reproducible single-crystal interfaces based on rubrene and Fx-TCNQ, a family of molecules whose electron affinity can be tuned by increasing the fluorine content. The combined analysis of transport and scanning Kelvin probe measurements reveals that the interfacial charge carrier density, resistivity, and activation energy correlate with the electron affinity of Fx-TCNQ crystals, with a higher affinity resulting in larger charge transfer. Although the transport properties can be described consistently and quantitatively using a mobility-edge model, we find that a quantitative analysis of charge transfer in terms of single-particle band diagrams reveals a discrepancy ~ 100 meV in the interfacial energy level alignment. We attribute the discrepancy to phenomena known to affect the energetics of organic semiconductors, which are neglected by a single-particle description, such as molecular relaxation and band-gap renormalization due to screening. The systematic behavior of the Fx-TCNQ/rubrene interfaces opens the possibility to investigate these phenomena experimentally, under controlled conditions.

cond-mat.mtrl-sci↗

arXiv2016

Band-like Electron Transport with Record-High Mobility in the TCNQ family

In highest quality organic single-crystal field-effect transistors, electron transport occurs in the band-like regime, with the carrier mobility increasing upon lowering temperature. Neither the microscopic nature of this regime, nor why it occurs only in a small number of materials is currently understood. Here, comparative studies of closely related materials, exhibiting high-quality reproducible transport properties are needed. We performed a study of electron transport in single-crystals of different TCNQ (tetracyanoquinodimethane) molecules, combined with band structure calculations. We show that F2-TCNQ devices exhibit very high electron mobility and an unprecedented increase in mobility upon cooling, whereas in TCNQ and F4-TCNQ the mobility is substantially lower and decreases upon cooling. We analyze the crystal and electronic structures of these materials and find that F2-TCNQ crystals are indeed ideal to achieve outstanding transport properties. Our analysis also shows that to understand the difference between the three materials, studying their band structure is not sufficient, and that the electron-phonon coupling needs to be investigated as well. Besides the outstanding transport properties of F2-TCNQ, a key result of our work is the identification of the Fx-TCNQ family as a paradigm to investigate the most fundamental aspects of electronic transport in organic crystals.

cond-mat.mtrl-sci↗

arXiv2016

Charge transfer, band-like transport, and magnetic ions at F16CoPc/rubrene interfaces

Organic semiconductors offer an unprecedented flexibility to control the electronic state of interfacial electronic systems. Here we present a first step in realizing organic charge transfer interfaces that combine both a large electrical conductivity and the presence of magnetic ions. We have performed a detailed investigation of F16CoPc/rubrene interface by means of temperature dependent charge transport measurements, Hall effect, scanning Kelvin probe microscopy and photoelectron spectroscopy. Our finding is that the charge transfer leads to significantly enhanced electrical conductivity and the band-like transport. We have determined the density, mobility and nature of charge carriers in the system (holes in rubrene). We have also found that the amount of charge transfer in F16CoPc/rubrene is high enough to cause the band-like transport in rubrene crystals at the interface. Finally, our XPS and UPS measurements have shown that the charge transfer in F16CoPc/rubrene involves electronic orbitals centered on the magnetic Co ions of the phthalocyanine molecules causing a change in their spin. Thus, F16CoPc/rubrene is the first organic interface where the charge transfer responsible for the interfacial conductivity fully involves the metal Co core of the phthalocyanine molecules, providing a link between charge transport and magnetic properties.

cond-mat.mtrl-sci↗

arXiv2016

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.

cond-mat.mes-hall↗

arXiv2015

Gate-induced Superconductivity in atomically thin MoS2 crystals

When thinned down to the atomic scale, many layered van der Waals materials exhibit an interesting evolution of their electronic properties, whose main aspects can be accounted for by changes in the single-particle band structure. Phenomena driven by interactions are also observed, but identifying experimentally systematic trends in their thickness dependence is challenging. Here, we explore the evolution of gate-induced superconductivity in exfoliated MoS2 multilayers ranging from bulk-like to individual monolayers. We observe a clear transition for all the thicknesses down to the ultimate atomic limit, providing the first demonstration of superconductivity in atomically thin exfoliated crystals. Additionally, we characterize the superconducting state by measuring the critical temperature (TC) and magnetic field (BC) in a large number of multilayer devices, upon decreasing their thickness. The superconducting properties change smoothly down to bilayers, and a pronounced reduction in TC and BC is found to occur when going from bilayers to monolayers, for which we discuss possible microscopic mechanisms. Finding that gate-induced superconductivity persists in individual monolayers, which form the basic building blocks of more sophisticated van der Waals heterostructures, opens new possibilities for the engineering of the electronic properties of materials at the atomic scale.

cond-mat.supr-con↗

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↗

arXiv2015

Strong interface-induced spin-orbit coupling in graphene on WS2

Interfacial interactions allow the electronic properties of graphene to be modified, as recently demonstrated by the appearance of satellite Dirac cones in the band structure of graphene on hexagonal boron nitride (hBN) substrates. Ongoing research strives to explore interfacial interactions in a broader class of materials in order to engineer targeted electronic properties. Here we show that at an interface with a tungsten disulfide (WS2) substrate, the strength of the spin-orbit interaction (SOI) in graphene is very strongly enhanced. The induced SOI leads to a pronounced low-temperature weak anti-localization (WAL) effect, from which we determine the spin-relaxation time. We find that spin-relaxation time in graphene is two-to-three orders of magnitude smaller on WS2 than on SiO2 or hBN, and that it is comparable to the intervalley scattering time. To interpret our findings we have performed first-principle electronic structure calculations, which both confirm that carriers in graphene-on-WS2 experience a strong SOI and allow us to extract a spin-dependent low-energy effective Hamiltonian. Our analysis further shows that the use of WS2 substrates opens a possible new route to access topological states of matter in graphene-based systems.

cond-mat.mes-hall↗

arXiv2015

Insulating state in tetralayers reveals an even-odd interaction effect in multilayer graphene

The absence of an energy gap separating valence and conduction bands makes the low-energy electronic properties of graphene and its multi-layers sensitive to electron-electron interactions. In bilayers, for instance, interactions are predicted to open a gap at charge neutrality, turning the system into an insulator, as observed experimentally. In mono and (Bernal-stacked) trilayers, interactions, although still important, do not have an equally drastic effect, and these systems remain conducting at low temperature. It may be expected that interaction effects become weaker for thicker multilayers, whose behavior should eventually converge to that of graphite. Here we show that this expectation does not correspond to reality by investigating the case of Bernal-stacked tetralayer graphene (4LG). We reveal the occurrence of a robust insulating state in a narrow range of carrier densities around charge neutrality, incompatible with the behavior expected from the single-particle band structure. The phenomenology resembles that observed in bilayers, but the stronger conductance suppression makes the insulating state in 4LG visible at higher temperature. To account for our findings, we suggest a natural generalization of the interaction-driven, symmetry-broken states proposed for bilayers. This generalization also explains the systematic even-odd effect of interactions in Bernal-stacked layers of different thickness that is emerging from experiments, and has implications for the multilayer-to-graphite crossover.

cond-mat.mes-hall↗

arXiv2015

Electrostatically Induced Superconductivity at the Surface of WS$_2$

We investigate transport through ionic liquid gated field effect transistors (FETs) based on exfoliated crystals of semiconducting WS$_2$. Upon electron accumulation, at surface densities close to -or just larger than- 10$^{14}$ cm$^{-2}$, transport exhibits metallic behavior, with the surface resistivity decreasing pronouncedly upon cooling. A detailed characterization as a function of temperature and magnetic field clearly shows the occurrence of a gate-induced superconducting transition below a critical temperature $T_c \approx 4$ K, a finding that represents the first demonstration of superconductivity in tungsten-based semiconducting transition metal dichalcogenides. We investigate the nature of superconductivity and find significant inhomogeneity, originating from the local detaching of the frozen ionic liquid from the WS$_2$ surface. Despite the inhomogeneity, we find that in all cases where a fully developed zero resistance state is observed, different properties of the devices exhibit a behavior characteristic of a Berezinskii-Kosterlitz-Thouless transition, as it could be expected in view of the two-dimensional nature of the electrostatically accumulated electron system.

cond-mat.mes-hall↗

arXiv2014

Random strain fluctuations as dominant disorder source for high-quality on-substrate graphene devices

We have performed systematic investigations of transport through graphene on hexagonal boron nitride (hBN) substrates, together with confocal Raman measurements and a targeted theoretical analysis, to identify the dominant source of disorder in this system. Low-temperature transport measurements on many devices reveal a clear correlation between the carrier mobility $μ$ and the width $n^*$ of the resistance peak around charge neutrality, demonstrating that charge scattering and density inhomogeneities originate from the same microscopic mechanism. The study of weak-localization unambiguously shows that this mechanism is associated to a long-ranged disorder potential, and provides clear indications that random pseudo-magnetic fields due to strain are the dominant scattering source. Spatially resolved Raman spectroscopy measurements confirm the role of local strain fluctuations, since the line-width of the Raman 2D-peak --containing information of local strain fluctuations present in graphene-- correlates with the value of maximum observed mobility. The importance of strain is corroborated by a theoretical analysis of the relation between $μ$ and $n^*$ that shows how local strain fluctuations reproduce the experimental data at a quantitative level, with $n^*$ being determined by the scalar deformation potential and $μ$ by the random pseudo-magnetic field (consistently with the conclusion drawn from the analysis of weak-localization). Throughout our study, we compare the behavior of devices on hBN substrates to that of devices on SiO$_2$ and SrTiO$_3$, and find that all conclusions drawn for the case of hBN are compatible with the observations made on these other materials. These observations suggest that random strain fluctuations are the dominant source of disorder for high-quality graphene on many different substrates, and not only on hexagonal boron nitride.

cond-mat.mes-hall↗

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

Scanning photocurrent microscopy reveals electron-hole asymmetry in ionic liquid-gated WS2 transistors

We perform scanning photocurrent microscopy on WS2 ionic liquid-gated field effect transistors exhibiting high-quality ambipolar transport. By properly biasing the gate electrode we can invert the sign of the photocurrent showing that the minority photocarriers are either electrons or holes. Both in the electron- and the hole-doping regimes the photocurrent decays exponentially as a function of the distance between the illumination spot and the nearest contact, in agreement with a two-terminal Schottky-barrier device model. This allows us to compare the value and the doping dependence of the diffusion length of the minority electrons and holes on a same sample. Interestingly, the diffusion length of the minority carriers is several times larger in the hole accumulation regime than in the electron accumulation regime, pointing out an electron-hole asymmetry in WS2.

cond-mat.mes-hall↗

arXiv2014

Mono- and Bilayer WS2 Light-Emitting Transistors

We have realized ambipolar ionic liquid gated field-effect transistors based on WS2 mono- and bilayers, and investigated their opto-electronic response. A thorough characterization of the transport properties demonstrates the high quality of these devices for both electron and hole accumulation, which enables the quantitative determination of the band gap (Δ1L = 2.14 eV for monolayers and Δ2L = 1.82 eV for bilayers). It also enables the operation of the transistors in the ambipolar injection regime with electrons and holes injected simultaneously at the two opposite contacts of the devices in which we observe light emission from the FET channel. A quantitative analysis of the spectral properties of the emitted light, together with a comparison with the band gap values obtained from transport, show the internal consistency of our results and allow a quantitative estimate of the excitonic binding energies to be made. Our results demonstrate the power of ionic liquid gating in combination with nanoelectronic systems, as well as the compatibility of this technique with optical measurements on semiconducting transition metal dichalcogenides. These findings further open the way to the investigation of the optical properties of these systems in a carrier density range much broader than that explored until now.

cond-mat.mes-hall↗

arXiv2014

Observation of even denominator fractional quantum Hall effect in suspended bilayer graphene

We investigate low-temperature magneto-transport in recently developed, high-quality multi-terminal suspended bilayer graphene devices, enabling the independent measurement of the longitudinal and transverse resistance. We observe clear signatures of the fractional quantum Hall effect, with different states that are either fully developed, and exhibit a clear plateau in the transverse resistance with a concomitant dip in longitudinal resistance, or incipient, and exhibit only a longitudinal resistance minimum. All observed states scale as a function of filling factor nu, as expected. An unprecedented even-denominator fractional state is observed at nu = -1/2 on the hole side, exhibiting a clear plateau in Rxy quantized at the expected value of 2h/e^2 with a precision of ~0.5%. Many of our observations, together with a recent electronic compressibility measurement performed in graphene bilayers on hexagonal boron-nitride (hBN) substrates, are consistent with a recent theory that accounts for the effect of the degeneracy between the N=0 and N=1 Landau levels in the fractional quantum Hall effect, and predicts the occurrence of a Moore-Read type nu = -1/2 state. Owing to the experimental flexibility of bilayer graphene --which has a gate-dependent band structure, can be easily accessed by scanning probes, and can be contacted with materials such as superconductors--, our findings offer new possibilities to explore the microscopic nature of even-denominator fractional quantum Hall effect.

cond-mat.mes-hall↗

arXiv2014

High-quality multi-terminal suspended graphene devices

We introduce a new scheme to realize suspended, multi-terminal graphene structures that can be current annealed successfully to obtain uniform, very high quality devices. A key aspect is that the bulky metallic contacts are not connected directly to the part of graphene probed by transport measurements, but only through etched constriction, which prevents the contacts from acting invasively. The device high quality and uniformity is demonstrated by a reproducibly narrow (delta_n ~ 10^9 cm^-2) resistance peak around charge neutrality, by carrier mobility values exceeding 10^6 cm^2/V/s, by the observation of integer quantum Hall plateaus starting at 30 mT and of symmetry broken states at about 200 mT, and by the occurrence of a negative multi-terminal resistance directly proving the occurrence of ballistic transport. As these multi-terminal devices enable measurements that cannot be done in a simpler two-terminal configuration, we anticipate that their use in future studies of graphene-based systems will be particularly relevant.

cond-mat.mes-hall↗

arXiv2013

Identification of a strong contamination source for graphene in vacuum systems

To minimize parasitic doping effects caused by uncontrolled material adsorption, graphene is often investigated under vacuum. Here we report an entirely unexpected phenomenon occurring in vacuum systems, namely strong n-doping of graphene due to chemical species generated by common ion high-vacuum gauges. The effect --reversible upon exposing graphene to air-- is significant, as doping rates can largely exceed 10^{12} cm^{-2}/hour, depending on pressure and the relative position of the gauge and the graphene device. It is important to be aware of the phenomenon, as its basic manifestation can be mistakenly interpreted as vacuum-induced desorption of p-dopants.

cond-mat.mes-hall↗

arXiv2013

Tailoring the molecular structure to suppress extrinsic disorder in organic transistors

In organic field-effect transistors, the structure of the constituent molecules can be tailored to minimize the disorder experienced by charge carriers. Experiments on two perylene derivatives show that disorder can be suppressed by attaching longer core substituents - thereby reducing potential fluctuations in the transistor channel and increasing the mobility at low temperature - without altering the intrinsic transport properties.

cond-mat.mtrl-sci↗