Realizing an excitonic insulator phase from narrow-gap semiconductors remains challenging, as unambiguous experimental signatures are difficult to establish. Ta$_2$NiSe$_5$ has been widely regarded as a leading candidate, yet the nature of its phase transition and insulating state remains controversial. Here, we report a systematic Raman spectroscopy study of Ta$_2$NiSe$_5$ as a function of thickness and field-effect doping, complemented by electrical transport measurements. The phase transition persists down to the monolayer limit, with the critical temperature increasing as thickness decreases. In bilayer samples, both electron and hole doping suppress the insulating state, with electron doping lowering and hole doping raising the transition temperature. Importantly, the quasi-elastic scattering, previously attributed to excitonic fluctuations, evolves monotonically across the entire doping range, inconsistent with the expected suppression of excitonic correlations by Coulomb screening. These findings rule out a dominant excitonic mechanism and instead point to a coupled electronic and structural phase transition, whose stability is tunable by carrier doping. Our doping-based approach offers a general strategy for evaluating the role of excitonic effects in candidate excitonic insulators.
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 at…
Two-dimensional (2D) layered materials-based field-effect transistors (FETs) are promising for ultimate scaled electron device applications because of the improved electrostatics to atomically thin body thickness. However, compared with the typical thickness of ~5-nm for Si-on-insulator (SOI), the advantage of the ultimate thickness limit of monolayer for the device performance has not been fully proved yet, especially for the on-state at the accumulation region. Here, we present much stronger quantum-mechanical effect at the accumulation region based on the C-V analysis for top-gate MoS2 FETs…
We have developed a technology to reproducibly make gaps with distance control on the single atom scale. The gold contacts are flat on the nanometre scale and are fabricated on an oxidized aluminium film that serves as a gate. We show that these contacts are clean and can be stabilized via chemical functionalization. Deposition of conjugated molecules leads to an increase in the gap conductance of several orders of magnitude. Stable current-voltage characteristics at room temperature are slightly nonlinear. At low temperature, they are highly nonlinear and show a clear gate effect.
Transient currents in atomically thin MoTe$_2$ field-effect transistor are measured during cycles of pulses through the gate electrode. The transients are analyzed in light of a newly proposed model for charge trapping dynamics that renders a time-dependent change in threshold voltage the dominant effect on the channel hysteretic behavior over emission currents from the charge traps. The proposed model is expected to be instrumental in understanding the fundamental physics that governs the performance of atomically thin FETs and is applicable to the entire class of atomically thin-based device…
Raman spectroscopy, a fast and nondestructive imaging method, can be used to monitor the doping level in graphene devices. We fabricated chemical vapor deposition (CVD) grown graphene on atomically flat hexagonal boron nitride (hBN) flakes and SiO$_2$ substrates. We compared their Raman response as a function of charge carrier density using an ion gel as a top gate. The G peak position, 2D peak position, 2D peak width and the ratio of the 2D peak area to the G peak area show a dependence on carrier density that differs for hBN compared to SiO$_2$. Histograms of two-dimensional mapping are used…
Two-dimensional dilute magnetic semiconductors can provide fundamental insights in the very nature of magnetic orders and their manipulation through electron and hole doping. Despite the fundamental physics, due to the large charge density control capability in these materials, they can be extremely important in spintronics applications such as spin valve and spin-based transistors. In this article, we studied a two-dimensional dilute magnetic semiconductors consisting of phosphorene monolayer doped with cobalt atoms in substitutional and interstitial defects. We show that these defects can be…
Material research has been a major driving force in the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices; identifying new magnetic materials is key to better device performance and new device paradigm. The advent of two-dimensional van der Waals crystals creates new possibilities. This family of materials retain their chemical stability and structural integrity down to monolayers and, being atomically thin, are readily tuned by various kinds of gate modulation. Recent experiments have demonstr…
In scaling of transistor dimensions with low source-to-drain currents, 1D semiconductors with certain electronic properties are highly desired. We discover three new 1D materials, SbSeI, SbSI and SbSBr with high stability and novel electronic properties based on first principles calculations. Both dynamical and thermal stability of these 1D materials are examined. The bulk-to-1D transition results in dramatic changes in band gap, effective mass and static dielectric constant due to quantum confinement, making 1D SbSeI a highly promising channel material for transistors with gate length shorter…
Atomically precise tailoring of graphene can enable unusual transport pathways and new nanometer-scale functional devices. Here we describe a recipe for the controlled production of highly regular "5-5-8" line defects in graphene by means of simultaneous electron irradiation and Joule heating by applied electric current. High-resolution transmission electron microscopy reveals individual steps of the growth process. Extending earlier theoretical work suggesting valley-discriminating capabilities of a graphene 5-5-8 line defect, we perform first-principles calculations of transport and find a s…
Two-dimensional (2D) layered semiconductors, with their ultimate atomic thickness, have shown promise to scale down transistors for modern integrated circuitry. However, the electrical contacts that connect these materials with external bulky metals are usually unsatisfactory, which limits the transistor performance. Recently, contacting 2D semiconductors using coplanar 2D conductors has shown promise in reducing the problematic high resistance contacts. However, many of these methods are not ideal for scaled production. Here, we report on the large-scale, spatially controlled chemical assembl…
We report an atomically-precise integration of individual nitrogen (N) dopant as an in-plane artificial nucleus in a graphene device by atomic implantation to probe its gate-tunable quantum states and correlation effects. The N dopant creates the characteristic resonance state in the conduction band, revealing a giant carrier-dependent energetic renormalization up to 350 meV with respect to the Dirac point, accompanied by the observation of long-range screening effects. Joint density functional theory and tight-binding calculations with modified perturbation potential corroborate experimental …
Energy band realignment at the interfaces between materials in heterostructures can give rise to unique electronic characteristics and non-trivial low-dimensional charge states. In a homojunction of monolayer and multilayer MoS$_2$, the thickness-dependent band structure implies the possibility of band realignment and a new interface charge state with properties distinct from the isolated layers. In this report, we probe the interface charge state using scanning photocurrent microscopy and gate-dependent transport with source-drain bias applied along the interface. Enhanced photoresponse obser…
The honeycomb lattice of graphene is a unique two-dimensional (2D) system where the quantum mechanics of electrons is equivalent to that of relativistic Dirac fermions. Novel nanometer-scale behavior in this material, including electronic scattering, spin-based phenomena, and collective excitations, is predicted to be sensitive to charge carrier density. In order to probe local, carrier-density dependent properties in graphene we have performed atomically-resolved scanning tunneling spectroscopy measurements on mechanically cleaved graphene flake devices equipped with tunable back-gate electro…
Recent experimental advances in atomically thin transition metal dichalcogenide (TMD) metals have unveiled a range of interesting phenomena including the coexistence of charge-density-wave (CDW) order and superconductivity down to the monolayer limit. The atomic thickness of two-dimensional (2D) TMD metals also opens up the possibility for control of these electronic phase transitions by electrostatic gating. Here we demonstrate reversible tuning of superconductivity and CDW order in model 2D TMD metal NbSe$_2$ by an ionic liquid gate. A variation up to ~ 50% in the superconducting transition …
Atomically thin layered two-dimensional materials, including transition-metal dichacolgenide (TMDC) and black phosphorus (BP), (1) have been receiving much attention, because of their promising physical properties and potential applications in flexible and transparent electronic devices . Here, for the first time we show non-volatile chargetrap memory devices, based on field-effect transistors with large hysteresis, consisting of a few-layer black phosphorus channel and a three dimensional (3D) Al2O3 /HfO2 /Al2O3 charge-trap gate stack. An unprecedented memory window exceeding 12 V is observed…
Many recent studies show that superconductivity not only exists in atomically thin monolayers but can exhibit enhanced properties such as higher transition temperature and stronger critical field. Nevertheless, besides being air unstable, weak tunability in these intrinsically metallic monolayers has posed a severe limitation in exploring monolayer superconductivity, hence hindering possible applications in electronic devices. Using field effect gating, we prepared monolayer superconductivity in easily accessible CVD-grown WS2, a typical ambient stable semiconducting transition metal dichalcog…
The p-n junction diode and field-effect transistor (FET) are the two most ubiquitous building blocks of modern electronics and optoelectronics. In recent years, the emergence of reduced dimensionality materials has suggested that these components can be scaled down to atomic thicknesses. Although high performance field-effect devices have been achieved from monolayered materials and their heterostructures, a p-n heterojunction diode derived from ultrathin materials is notably absent and constrains the fabrication of complex electronic and optoelectronic circuits. Here, we demonstrate a gate-tu…
Atomically-thin two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have been extensively studied in recent years because of their appealing electrical and optical properties. Here, we report on the fabrication of ReS2 field-effect transistors via the encapsulation of ReS2 nanosheets in a high-\k{appa} Al2O3 dielectric environment. Low-temperature transport measurements allowed us to observe a direct metal-to-insulator transition originating from strong electron-electron interactions. Remarkably, the photodetectors based on ReS2 exhibit gate-tunable photoresponsivity up to 16.…
Electrical transport in monolayer graphene on SrTiO3 (STO) thin film is examined in order to promote gate-voltage scaling using a high-k dielectric material. The atomically flat surface of thin STO layer epitaxially grown on Nb-doped STO single-crystal substrate offers good adhesion between the high-k film and graphene, resulting in nonhysteretic conductance as a function of gate voltage at all temperatures down to 2 K. The two-terminal conductance quantization under magnetic fields corresponding to quantum Hall states survives up to 200 K at a magnetic field of 14 T. In addition, the substant…
A1-xFe2-ySe2 (A = K, Cs, Rb, Tl) are recently discovered iron-based superconductors with critical temperatures (Tc) ranging up to 32 K. Their parent phases have unique properties when compared with other iron-based superconductors; e.g., their crystal structures include ordered Fe vacancies, their normal states are antiferromagnetic (AFM) insulating phases, and they have extremely high Néel transition temperatures. However, control of carrier doping into the parent AFM insulators has been difficult due to their intrinsic phase separation. Here, we fabricated an Fe-vacancy-ordered TlFe1.6Se2 in…
Atomically Thin Amorphous Carbon with an Ultralow Dielectric Constant
National University of Singapore（新加坡国立大学）；Centre for Advanced 2D materials, National University of Singapore（新加坡国立大学二维材料中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；IKERBASQUE Basque Foundation for Science（伊克尔巴斯克巴斯克科学基金会）；Freie Universität Berlin（柏林自由大学）；Leibniz Institute for Solid State and Materials Research（莱布尼茨固体与材料研究所）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Joint Laboratory “Functional Quantum Materials” at BESSY II（BESSY II功能量子材料联合实验室）；Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)（新加坡科技研究局材料研究与工程研究所）；Sanken, Osaka University（大阪大学三冈研究所）；Nanomaterials Research Institute, National Institute of Advanced Industrial Science and Technology (AIST)（日本产业技术综合研究所纳米材料研究所）；Institute for Functional Intelligent Materials, National University of Singapore（新加坡国立大学功能智能材料研究所）
Dynamic control of conductivity and optical properties via atomic structure changes is of tremendous technological importance in information storage. Energy consumption considerations provide a driving force toward employing thin materials in devices. Monolayer transition metal dichalcogenides are nearly atomically-thin materials that can exist in multiple crystal structures, each with distinct electrical properties. Using density functional approaches, we discover that electrostatic gating device configurations have the potential to drive structural semiconductor-to-semimetal phase transition…
