Showing papers by "Andras Kis published in 2014"

Electrical Transport Properties of Single-Layer WS2

Abstract: We report on the fabrication of field-effect transistors based on single layers and bilayers of the semiconductor WS2 and the investigation of their electronic transport properties. We find that the doping level strongly depends on the device environment and that long in situ annealing drastically improves the contact transparency, allowing four-terminal measurements to be performed and the pristine properties of the material to be recovered. Our devices show n-type behavior with a high room temperature on/off current ratio of similar to 10(6). They show clear metallic behavior at high charge carrier densities and mobilities as high as similar to 140 cm(2)/(V s) at low temperatures (above 300 cm(2)/(V s) in the case of bilayers). In the insulating regime, the devices exhibit variable range hopping, with a localization length of about 2 nm that starts to increase as the Fermi level enters the conduction band. The promising electronic properties of WS2, comparable to those of single layer MoS2 and WSe2, together with its strong spin-orbit coupling, make it interesting for future applications in electronic, optical, and valleytronic devices.

Large-area Epitaxial Monolayer MoS2

Abstract: Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics and energy harvesting. Large-area growth methods are needed to open the way to the applications. While significant progress to this goal was made, control over lattice orientation during growth still remains a challenge. This is needed in order to minimize or even avoid the formation of grain boundaries which can be detrimental to electrical, optical and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the uniform growth of high-quality centimeter-scale continuous monolayer MoS2 with control over lattice orientation. Using transmission electron microscopy we show that the monolayer film is composed of coalescing single islands that share a predominant lattice orientation due to an epitaxial growth mechanism. Raman and photoluminescence spectra confirm the high quality of the grown material. Optical absorbance spectra acquired over large areas show new features in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment, we can easily transfer the grown material and fabricate field-effect transistors on SiO2 substrates showing mobility superior to the exfoliated material.

Thermal Conductivity of Monolayer Molybdenum Disulfide Obtained from Temperature-Dependent Raman Spectroscopy

Abstract: Atomically thin molybdenum disulfide (MoS2) offers potential for advanced devices and an alternative to graphene due to its unique electronic and optical properties. The temperature-dependent Raman spectra of exfoliated, monolayer MoS2 in the range of 100–320 K are reported and analyzed. The linear temperature coefficients of the in-plane E2g1 and the out-of-plane A1g modes for both suspended and substrate-supported monolayer MoS2 are measured. These data, when combined with the first-order coefficients from laser power-dependent studies, enable the thermal conductivity to be extracted. The resulting thermal conductivity κ = (34.5 ± 4) W/mK at room temperature agrees well with the first-principles lattice dynamics simulations. However, this value is significantly lower than that of graphene. The results from this work provide important input for the design of MoS2-based devices where thermal management is critical.

Atomically Thin Molybdenum Disulfide Nanopores with High Sensitivity for DNA Translocation

Abstract: Atomically thin nanopore membranes are considered to be a promising approach to achieve single base resolution with the ultimate aim of rapid and cheap DNA sequencing. Molybdenum disulfide (MoS2) is newly emerging as a material complementary to graphene due to its semiconductive nature and other interesting physical properties that can enable a wide range of potential sensing and nanoelectronics applications. Here, we demonstrate that monolayer or few-layer thick exfoliated MoS2 with subnanometer thickness can be transferred and suspended on a predesigned location on the 20 nm thick SiNx membranes. Nanopores in MoS2 are further sculpted with variable sizes using a transmission electron microscope (TEM) to drill through suspended portions of the MoS2 membrane. Various types of double-stranded (ds) DNA with different lengths and conformations are translocated through such a novel architecture, showing improved sensitivity (signal-to-noise ratio >10) compared to the conventional silicon nitride (SiNx) nanopo...

Optically Active Quantum Dots in Monolayer WSe$_2$

Abstract: Semiconductor quantum dots have emerged as promising candidates for implementation of quantum information processing since they allow for a quantum interface between stationary spin qubits and propagating single photons. In the meanwhile, transition metal dichalcogenide (TMD) monolayers have moved to the forefront of solid-state research due to their unique band structure featuring a large band gap with degenerate valleys and non-zero Berry curvature. Here we report the observation of quantum dots in monolayer tungsten-diselenide with an energy that is 20 to 100 meV lower than that of two dimensional excitons. Photon antibunching in second-order photon correlations unequivocally demonstrates the zero-dimensional anharmonic nature of these quantum emitters. The strong anisotropic magnetic response of the spatially localized emission peaks strongly indicates that radiative recombination stems from localized excitons that inherit their electronic properties from the host TMD. The large $\sim$ 1 meV zero-field splitting shows that the quantum dots have singlet ground states and an anisotropic confinement most likely induced by impurities or defects in the host TMD. Electrical control in van der Waals heterostructures and robust spin-valley degree of freedom render TMD quantum dots promising for quantum information processing.

Light generation and harvesting in a van der Waals heterostructure

Abstract: Two-dimensional (2D) materials are a new type of materials under intense study because of their interesting physical properties and wide range of potential applications from nanoelectronics to sensing and photonics. Monolayers of semiconducting transition metal dichalcogenides MoS2 or WSe2 have been proposed as promising channel materials for field-effect transistors. Their high mechanical flexibility, stability, and quality coupled with potentially inexpensive production methods offer potential advantages compared to organic and crystalline bulk semiconductors. Due to quantum mechanical confinement, the band gap in monolayer MoS2 is direct in nature, leading to a strong interaction with light that can be exploited for building phototransistors and ultrasensitive photodetectors. Here, we report on the realization of light-emitting diodes based on vertical heterojunctions composed of n-type monolayer MoS2 and p-type silicon. Careful interface engineering allows us to realize diodes showing rectification an...

Light Generation and Harvesting in a Van der Waals Heterostructure

Abstract: Two-dimensional (2D) materials are a new type of materials under intense study because of their interesting physical properties and wide range of potential applications from nanoelectronics to sensing and photonics. Monolayers of semiconducting transition metal dichalcogenides MoS2 or WSe2 have been proposed as promising channel materials for field-effect transistors. Their high mechanical flexibility, stability, and quality coupled with potentially inexpensive production methods offer potential advantages compared to organic and crystalline bulk semiconductors. Due to quantum mechanical confinement, the band gap in monolayer MoS2 is direct in nature, leading to a strong interaction with light that can be exploited for building phototransistors and ultrasensitive photodetectors. Here, we report on the realization of light-emitting diodes based on vertical heterojunctions composed of n-type monolayer MoS2 and p-type silicon. Careful interface engineering allows us to realize diodes showing rectification and light emission from the entire surface of the heterojunction. Electroluminescence spectra show clear signs of direct excitons related to the optical transitions between the conduction and valence bands. Our p–n diodes can also operate as solar cells, with typical external quantum efficiency exceeding 4%. Our work opens up the way to more sophisticated optoelectronic devices such as lasers and heterostructure solar cells based on hybrids of 2D semiconductors and silicon.

Electron and hole mobilities in single-layer WSe2.

Abstract: Single-layer transition metal dichalcogenide WSe2 has recently attracted a lot of attention because it is a 2D semiconductor with a direct band gap. Due to low doping levels, it is intrinsic and shows ambipolar transport. This opens up the possibility to realize devices with the Fermi level located in the valence band, where the spin/valley coupling is strong and leads to new and interesting physics. As a consequence of its intrinsically low doping, large Schottky barriers form between WSe2 and metal contacts, which impede the injection of charges at low temperatures. Here, we report on the study of single-layer WSe2 transistors with a polymer electrolyte gate (PEO:LiClO4). Polymer electrolytes allow the charge carrier densities to be modulated to very high values, allowing the observation of both the electron- and the hole-doped regimes. Moreover, our ohmic contacts formed at low temperatures allow us to study the temperature dependence of electron and hole mobilities. At high electron densities, a re-en...

MoS2 transistors operating at gigahertz frequencies.

Abstract: The presence of a direct band gap 1−4 and an ultrathin form factor 5 has caused a considerable interest in two-dimensional (2D) semiconductors from the transition metal dichalcogenides (TMD) family with molybdenum disulfide (MoS2) being the most studied representative of this family of materials. While diverse electronic elements, 6,7 logic circuits, 8,9 and optoelectronic devices 12,13 have been demonstrated using ultrathin MoS2, very little is known about their performance at high frequencies where commercial devices are expected to function. Here, we report on top-gated MoS2 transistors operating in the gigahertz range of frequencies. Our devices show cutoff frequencies reaching 6 GHz. The presence of a band gap also gives rise to current saturation, 10 allowing power and voltage gain, all in the gigahertz range. This shows that MoS2 could be an interesting material for realizing high-speed amplifiers and logic circuits with device scaling expected to result in further improvement of performance. Our work represents the first step in the realization of high-frequency analog and digital circuits based on 2D semiconductors.

Electron and Hole Mobilities in Single-Layer WSe2

Abstract: Single-layer transition metal dichalcogenide (TMD) WSe2 has recently attracted a lot of attention because it is a 2D semiconductor with a direct band-gap. Due to low doping levels it is intrinsic and shows ambipolar transport. This opens up the possibility to realize devices with the Fermi level located in valence band, where the spin/valley coupling is strong and leads to new and interesting physics. As a consequence of its intrinsically low doping, large Schottky barriers form between WSe2 and metal contacts, which impede the injection of charges at low temperatures. Here, we report on the study of single-layer WSe2 transistors with a polymer electrolyte gate (PEO:LiClO4). Polymer electrolytes allow the charge carrier densities to be modulated to very high values, allowing the observation of both the electron- and the hole-doped regimes. Moreover, our ohmic contacts formed at low temperatures allow us to study the temperature dependence of electron and hole mobilities. At high electron densities, a re-entrant insulating regime is also observed, a feature which is absent at high hole densities.

Light Generation and Harvesting in a Van der Waals Heterostructure

Abstract: Two-dimensional (2D) materials are a new type of materials under intense study because of their interesting physical properties and wide range of potential applications from nanoelectronics to sensing and photonics. Monolayers of semiconducting transition metal dichalcogenides MoS2 or WSe2 have been proposed as promising channel materials for field-effect transistors (FETs). Their high mechanical flexibility, stability and quality coupled with potentially inexpensive production methods offer potential advantages compared to organic and crystalline bulk semiconductors. Due to quantum mechanical confinement, the band gap in monolayer MoS2 is direct in nature, leading to a strong interaction with light that can be exploited for building phototransistors and ultrasensitive photodetectors. Here, we report on the realization of light-emitting diodes based on vertical heterojunctions composed of n-type monolayer MoS2 and p-type silicon. Careful interface engineering allows us to realize diodes showing rectification and light emission from the entire surface of the heterojunction. Electroluminescence spectra show clear signs of direct excitons related to the optical transitions between the conduction and valence bands. Our pn diodes can also operate as solar cells, with typical external quantum efficiency exceeding 4%. Our work opens up the way to more sophisticated optoelectronic devices such as lasers and heterostructure solar cells based on hybrids of two-dimensional (2D) semiconductors and silicon.

Electrical Transport Properties of Single-Layer WS 2

Abstract: We report on the fabrication of field-effect transis- tors based on single layers and bilayers of the semiconductor WS2 and the investigation of their electronic transport properties. We find that the doping level strongly depends on the device environ- mentandthatlonginsituannealingdrasticallyimprovesthecontact transparency, allowing four-terminal measurements to be per- formed and the pristine properties of the material to be recovered. Our devices show n-type behavior with a high room-temperature on/off current ratio of ∼10 6 . They show clear metallic behavior at high charge carrier densities and mobilities as high as ∼140 cm 2 /(V s) at low temperatures (above 300 cm 2 /(V s) in the case of bilayers). In the insulating regime, the devices exhibit variable-range hopping, with a localization length of about 2 nm that starts to increase as the Fermi level enters the conduction band. The promising electronic properties of WS2, comparable to those of single-layer MoS2 and WSe2, together with its strong spinorbit coupling, make it interesting for future applications in electronic, optical, and valleytronic devices.

Can 2D-Nanocrystals Extend the Lifetime of Floating-Gate Transistor Based Nonvolatile Memory?

Abstract: Conventional floating-gate (FG) transistors (made with Si/poly-Si) that form the building blocks of the widely employed nonvolatile flash memory technology face severe scaling challenges beyond the 12-nm node. In this paper, for the first time, a comprehensive evaluation of the FG transistor made from emerging nanocrystals in the form of 2-dimensional (2D) transition metal dichalcogenides (TMDs) and multilayer graphene (MLG) is presented. It is shown that TMD based 2D channel materials have excellent gate length scaling potential due to their atomic scale thicknesses. On the other hand, employing MLG as FG greatly reduces cell-to-cell interference and alleviates reliability concerns. Moreover, it is also revealed that TMD/MLG heterostructures enable new mechanism for improving charge retention, thereby allowing the effective oxide thickness of gate dielectrics to be scaled to a few nanometers. Thus, this work indicates that judiciously selected 2D-nanocrystals can significantly extend the lifetime of the FG-based memory cell.

Avalanche photodiodes based on MoS2/Si heterojunctions

Abstract: Avalanche photodiodes (APDs) are the semiconducting analogue of photomultiplier tubes offering very high internal current gain and fast response. APDs are interesting for a wide range of applications in communications1, laser ranging2, biological imaging3, and medical imaging4 where they offer speed and sensitivity superior to those of classical p-n junction-based photodetectors. The APD principle of operation is based on photocurrent multiplication through impact ionization in reverse-biased p-n junctions. APDs can either operate in proportional mode, where the bias voltage is below breakdown, or in Geiger mode, where the bias voltage is above breakdown. In proportional mode, the multiplication gain is finite, thus allowing for photon energy discrimination, while in Geiger mode of operation the multiplication gain is virtually infinite and a self-sustaining avalanche may be triggered, thus allowing detection of single photons5. Here, we demonstrate APDs based on vertically stacked monolayer MoS2 and p-Si, forming an abrupt p-n heterojunction. With this device, we demonstrate carrier multiplication exceeding 1000. Even though such multiplication factors in APDs are commonly accompanied by high noise, our devices show extremely low noise levels comparable with those in regular photodiodes. These heterostructures allow the realization of simple and inexpensive high-performance and low-noise photon counters based on transition metal dichalcogenides.

Numerical correction of anti-symmetric aberrations in single HRTEM images

Abstract: Here, we present a numerical post-processing method for removing the effect of anti-symmetric residual aberrations in high-resolution transmission electron microscopy (HRTEM) images of weakly scattering 2D-objects. The method is based on applying the same aberrations with the opposite phase to the Fourier transform of the recorded image intensity and subsequently inverting the Fourier transform. We present the theoretical justification of the method and its verification based on simulated images in the case of low-order anti-symmetric aberrations. Ultimately the method is applied to experimental hardware aberration-corrected HRTEM images of single-layer graphene and MoSe2 resulting in images with strongly reduced residual low-order aberrations, and consequently improved interpretability. Alternatively, this method can be used to estimate by trial and error the residual anti-symmetric aberrations in HRTEM images of weakly scattering objects.

Published as part of the Accounts of Chemical Research special issue "2D Nanomaterials beyond Graphene".

Abstract: CONSPECTUS: Atomic crystals of two-dimensional materials consisting of single sheets extracted from layered materials are gaining increasing attention. The most well-known material from this group is graphene, a single layer of graphite that can be extracted from the bulk material or grown on a suitable substrate. Its discovery has given rise to intense research effort culminating in the 2010 Nobel Prize in physics awarded to Andre Geim and Konstantin Novoselov. Graphene however represents only the proverbial tip of the iceberg, and increasing attention of researchers is now turning towards the veritable zoo of so-called “other 2D materials”. They have properties complementary to graphene, which in its pristine form lacks a bandgap: MoS2, for example, is a semiconductor, while NbSe2 is a superconductor. They could hold the key to important practical applications and new scientific discoveries in the two-dimensional limit. This family of materials has been studied since the 1960s, but most of the research focused on their tribological applications: MoS2 is best known today as a high-performance dry lubricant for ultrahigh-vacuum applications and in car engines. The realization that single layers of MoS2 and related materials could also be used in functional electronic devices where they could offer advantages compared with silicon or graphene created a renewed interest in these materials. MoS2 is currently gaining the most attention because the material is easily available in the form of a mineral, molybdenite, but other 2D transition metal dichalcogenide (TMD) semiconductors are expected to have qualitatively similar properties. In this Account, we describe recent progress in the area of single-layer MoS2-based devices for electronic circuits. We will start with MoS2 transistors, which showed for the first time that devices based on MoS2 and related TMDs could have electrical properties on the same level as other, more established semiconducting materials. This allowed rapid progress in this area and was followed by demonstrations of basic digital circuits and transistors operating in the technologically relevant gigahertz range of frequencies, showing that the mobility of MoS2 and TMD materials is sufficiently high to allow device operation at such high frequencies. Monolayer MoS2 and other TMDs are also direct band gap semiconductors making them interesting for realizing optoelectronic devices. These range from simple phototransistors showing high sensitivity and low noise, to light emitting diodes and solar cells. All the electronic and optoelectronic properties of MoS2 and TMDs are accompanied by interesting mechanical properties with monolayer MoS2 being as stiff as steel and 30× stronger. This makes it especially interesting in the context of flexible electronics where it could combine the high degree of mechanical flexibility commonly associated with organic semiconductors with high levels of electrical performance. All these results show that MoS2 and TMDs are promising materials for electronic and optoelectronic applications.

Numerical correction of anti-symmetric aberrations in single HRTEM images of weakly scattering 2D-objects

Abstract: Here, we present a numerical post-processing method for removing the effect of anti-symmetric residual aberrations in high-resolution transmission electron microscopy (HRTEM) images of weakly scattering 2D-objects. The method is based on applying the same aberrations with the opposite phase to the Fourier transform of the recorded image intensity and subsequently inverting the Fourier transform. We present the theoretical justification of the method and its verification based on simulated images in the case of low-order anti-symmetric aberrations. Ultimately the method is applied to experimental hardware aberration-corrected HRTEM images of single-layer graphene and MoSe2 resulting in images with strongly reduced residual low-order aberrations, and consequently improved interpretability. Alternatively, this method can be used to estimate by trial and error the residual anti-symmetric aberrations in HRTEM images of weakly scattering objects.

Electrical Transport Properties of Single-Layer WS2

Abstract: We report on the fabrication of field-effect transistors based on single and bilayers of the semiconductor WS2 and the investigation of their electronic transport properties. We find that the doping level strongly depends on the device environment and that long in-situ annealing drastically improves the contact transparency allowing four-terminal measurements to be performed and the pristine properties of the material to be recovered. Our devices show n-type behavior with high room-temperature on/off current ratio of ~106. They show clear metallic behavior at high charge carrier densities and mobilities as high as ~140 cm2/Vs at low temperatures (above 300 cm2/Vs in the case of bi-layers). In the insulating regime, the devices exhibit variable-range hopping, with a localization length of about 2 nm that starts to increase as the Fermi level enters the conduction band. The promising electronic properties of WS2, comparable to those of single-layer MoS2 and WSe2, together with its strong spin-orbit coupling, make it interesting for future applications in electronic, optical and valleytronic devices.

MoS2 Transistors Operating at Gigahertz Frequencies

Abstract: The presence of a direct band gap and an ultrathin form factor has caused a considerable interest in two-dimensional (2D) semiconductors from the transition metal dichalcogenides (TMD) family with molybdenum disulphide (MoS2) being the most studied representative of this family of materials. While diverse electronic elements, logic circuits and optoelectronic devices have been demonstrated using ultrathin MoS2, very little is known about their performance at high frequencies where commercial devices are expected to function. Here, we report on top-gated MoS2 transistors operating in the gigahertz range of frequencies. Our devices show cutoff frequencies reaching 6 GHz. The presence of a band gap also gives rise to current saturation, allowing power and voltage gain, all in the gigahertz range. This shows that MoS2 could be an interesting material for realizing high-speed amplifiers and logic circuits with device scaling expected to result in further improvement of performance. Our work represents the first step in the realization of high-frequency analog and digital circuits based on two-dimensional semiconductors.