Charge-transfer Contact to a High-Mobility Monolayer Semiconductor
Jordan Pack, Yinjie Guo, Ziyu Liu, Bjarke S. Jessen, Luke Holtzman, Song Liu, Matthew Cothrine, Kenji Watanabe, Takashi Taniguchi, David G. Mandrus, Katayun Bar… 展开作者
Jordan Pack, Yinjie Guo, Ziyu Liu, Bjarke S. Jessen, Luke Holtzman, Song Liu, Matthew Cothrine, Kenji Watanabe, Takashi Taniguchi, David G. Mandrus, Katayun Barmak, James Hone, Cory R. Dean
Two-dimensional (2D) semiconductors, such as the transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for 2D semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure magneto-transport properties of high-purity monolayer WSe$_2$. We measure a record-high hole mobility of 80,000 cm$^2$/Vs and access channel carrier densities as low as $1.6\times10^{11}$ cm$^{-2}$, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurement of correlation-driven quantum phases including observation of a low temperature metal-insulator transition in a density and temperature regime where Wigner crystal formation is expected, and observation of the fractional quantum Hall effect under large magnetic fields. The charge transfer contact scheme paves the way for discovery and manipulation of new quantum phenomena in 2D semiconductors and their heterostructures.
The room temperature carrier mobility in atomically thin 2D materials is usually far below the intrinsic limit imposed by phonon scattering as a result of scattering by remote charged impurities in its environment. We simulate the charged impurity-limited carrier mobility $μ$ in bare and encapsulated monolayer phosphorene. We find a significant temperature dependence in the carrier mobilities ($μ\propto T^{-γ}$) that results from the temperature variability of the charge screening and varies with the crystal orientation. The anisotropy in the effective mass leads to an anisotropic carrier mobi…
We address the problem of free carrier screening of exciton states in two-dimensional monolayer semiconductors. Basic theoretical considerations are presented concerning the applicability of the commonly used static approximation of the screening effect and the implications are discussed. We show that the low-frequency models lead to a major overestimation of the free carrier response and are inadequate to describe the screening of strongly bound excitons in monolayer materials. The presented arguments are consistent with existing high-level many-body theories and transparently illustrate the …
We calculate an electron-phonon scattering and intrinsic transport properties of black phosphorus monolayer using tight-binding and Boltzmann treatments as a function of temperature, carrier density, and electric field. The low-field mobility shows weak dependence on density and, at room temperature, falls in the range of 300 - 1000 cm^2/Vs in the armchair direction and 50 - 120 cm^2/Vs in the zig-zag direction with the anisotropy due to an effective mass difference. At high fields, drift velocity is linear with electric field up to 1 - 2 V/micron reaching values of 10^7 cm/s in the armchair d…
Half-metals and spin gapless semiconductors are promising candidates for spintronic applications due to the complete (100%) spin polarization of electrons around the Fermi level. Based on recent experimental and theoretical findings of graphene-like monolayer transition metal carbides and nitrides (also known as MXenes), we demonstrate from first-principles calculations that monolayer Ti2C and Ti2N exhibit nearly half-metallic ferromagnetism with the magnetic moments of 1.91 and 1.00 UB per formula unit, respectively, while monolayer V2C is a metal with instable antiferromagnetism, and monolay…
High charge mobility in active layers of organic electronic devices is often necessary for their efficient operation. As a result, search for high-mobility materials among the plethora of synthesizable organic semiconductors is of paramount importance for organic electronics. However, a model for rapid but reliable prediction of charge mobility in various organic semiconductors is still lacking. To solve this issue, we propose a simple analytical model that considers the most essential factors governing the charge transport in these materials: intermolecular electronic coupling, charge delocal…
We demonstrate robust power- and wavelength-dependent optical bistability in fully suspended monolayers of WSe2 near the exciton resonance. Bistability has been achieved under continuous-wave optical excitation at an intensity level of 10^3 W/cm^2. The observed bistability is originated from a photo-thermal mechanism, which provides both optical nonlinearity and passive feedback, two essential elements for optical bistability. Under a finite magnetic field, the exciton bistability becomes helicity dependent, which enables repeatable switching of light purely by its polarization.
Manipulation of Rashba effects in two-dimensional (2D) electron systems is highly desirable for controllable applications in spintronics and optoelectronics. Here, by combining first-principles investigation and model analysis, we use uniaxial stress to control BiTeI monolayer as a Rashba 2D semiconductor for useful spin and transport properties. We find that the stress-driven electron system can be described by an effective anisotropic Rashba model including all the three Pauli matrixes, and uniaxial stress allows an out-of-plane spin component. When appropriate electron carriers are introduc…
Recently an air-stable layered semiconductor Bi2O2Se was discovered to exhibit an ultrahigh mobility in transistors fabricated with its thin layers. In this work, we explored the mechanism that induces the high mobility and distinguishes Bi2O2Se from other semiconductors. We found that the electron donor states lie above the lowest conduction band. Thus, electrons get spontaneously ionized from donor sites (e.g., Se vacancies) without involving the thermal activation, different from the donor ionization in conventional semiconductors. Consequently, the resistance decreases as reducing the temp…
We study the interface exciton at lateral type II heterojunctions of monolayer transition metal dichalcogenides (TMDs), where the electron and hole prefer to stay at complementary sides of the junction. We find that the 1D interface exciton has giant binding energy in the same order as 2D excitons in pristine monolayer TMDs although the effective radius (electron-hole seperation) of interface exciton is much larger than that of 2D excitons. The binding energy, exciton radius and optical dipole strongly depends on the band offset at the junction. The inter-valley coupling induced by the electro…
Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN en…
We directly monitor exciton propagation in freestanding and SiO2-supported WS2 monolayers through spatially- and time-resolved micro-photoluminescence under ambient conditions. We find highly nonlinear behavior with characteristic, qualitative changes in the spatial profiles of the exciton emission and an effective diffusion coefficient increasing from 0.3 to more than 30 cm2/s, depending on the injected exciton density. Solving the diffusion equation while accounting for Auger recombination allows us to identify and quantitatively understand the main origin of the increase in the observed dif…
A new two-dimensional (2D) layered material, namely, titanium trisulfide (TiS$_3$) monolayer sheet, is predicted to possess desired electronic properties for nanoelectronic applications. On basis of the first-principles calculations within the framework of density functional theory and deformation theory, we show that the TiS$_3$ 2D crystal is a direct gap semiconductor with a band gap of 1.06 eV and high carrier mobility. More remarkably, the in-plane electron mobility of the 2D TiS$_3$ is highly anisotropic, amounting to $\sim$10,000 cm$^2$V$^{-1}$s$^{-1}$ in the \emph{b} direction, which is…
We study the Landau level spectrum using a multi-band $\mathbf{k}\cdot\mathbf{p}$ theory in monolayer transition metal dichalcogenide semiconductors. We find that in a wide magnetic field range the Landau levels can be characterized by a harmonic oscillator spectrum and a linear-in-magnetic field term which describes the valley degeneracy breaking. The effect of the non-parabolicity of the band-dispersion on the Landau level spectrum is also discussed. Motivated by recent magnetotransport experiments, we use the self-consistent Born approximation and the Kubo formalism to calculate the Shubnik…
A vertical transistor based on a double gated, atomically thin heterojunction is theoretically examined. Both p-type and n-type transistor operations can be conveniently achieved by using one of the two gates as the switching gate. The transistor shows excellent saturation of output I-V characteristics due to drain-induced depletion and lack of tunneling barrier layers. The subthreshold slope could be below the thermionic limit due to band filtering as the switching mechanism. The atomically thin vertical PN heterojunction can be electrostatically modulated from a type II heterojunction to a b…
Strong coupling between light and the fundamental excitations of a two-dimensional electron gas (2DEG) are of foundational importance both to pure physics and to the understanding and development of future photonic nanotechnologies. Here we study the relationship between spin polarization of a 2DEG in a monolayer semiconductor, MoSe$_2$, and light-matter interactions modified by a zero-dimensional optical microcavity. We find robust spin-susceptibility of the 2DEG to simultaneously enhance and suppress trion-polariton formation in opposite photon helicities. This leads to observation of a gian…
The recent discovery of exciton quantum emitters in transition metal dichalcogenides (TMDCs) has triggered renewed interest of localized excitons in low-dimensional systems. Open questions remain about the microscopic origin previously attributed to dopants and/or defects as well as strain potentials. Here we show that the quantum emitters can be deliberately induced by nanobubble formation in WSe2 and BN/WSe2 heterostructures. Correlations of atomic-force microscope and hyperspectral photoluminescence images reveal that the origin of quantum emitters and trion disorder is extrinsic and relate…
Semiconductor microcavity polaritons, formed via strong exciton-photon coupling, provide a quantum many-body system on a chip, featuring rich physics phenomena for better photonic technology. However, conventional polariton cavities are bulky, difficult to integrate, and inflexible for mode control, especially for room temperature materials. Here we demonstrate sub-wavelength thick one-dimensional photonic crystals (PCs) as a designable, compact and practical platform for strong coupling with atomically thin van der Waals Crystals (vdWCs). Polariton dispersions and mode anti-crossings are meas…
Monolayers (MLs) of transition metal dichalcogenides (TMDs) such as WSe2 and MoSe2 can be placed by dry stamping directly on broadband dielectric resonators, which have the ability to enhance the spontaneous emission rate and brightness of solid-state emitters at room temperature. We show strongly enhanced emission and directivity modifications in room temperature photoluminescence mapping experiments. By varying TMD material (WSe2 versus MoSe2) transferred on silicon nanoresonators with various designs (planarized versus non-planarized), we experimentally separate the different physical mecha…
Regulation of electronic structure and mobility cut-on rate in two-dimensional transition metal dichalcogenides (TMDs) has attracted much attention because of its potential in electronic device design. The anisotropic Raman scattering and mobility cut-on rate of monolayer unique distorted-1T(1Td) ReS2 with external strain are determined theoretically based on the density function theory. The angle-dependent Raman spectrum of Ag-like, Eg-like and Cp models are used to discriminate and analysis structural anisotropy; the strain is exploited to adjust the structural symmetry and electronic struct…
Atomic disorder is a common limiting factor for the low-temperature mobility in monolayer transition-metal dichalcogenides (TMDs; MX2). Here, we study the effect of often occurring atomic vacancies on carrier scattering and transport in p- and n-type monolayer MoS2. Due to charge trapping in vacancy-induced in-gap states, both neutral and charged vacancies resembling, respectively, short-range and combined short-range and long-range Coulomb scatterers, must be considered. Using the T-matrix formalism, we demonstrate a strong renormalization of the Born description of short-range scattering, ma…
Monolayer transition metal dichalcogenides feature tightly bound bright excitons at the degenerate valleys, where electron-hole Coulomb exchange interaction strongly couples the valley pseudospin to the momentum of exciton. Placed on periodically structured dielectric substrate, the spatial modulation of the Coulomb interaction leads to the formation of exciton Bloch states with real-space valley pseudospin texture displayed in a mesoscopic supercell. We find this spatial valley texture in the exciton Bloch function is pattern-locked to the propagation direction, enabling nano-optical excitati…
Electrons in monolayer transition metal dichalcogenides (TMDs) possess both the valley and spin degree of freedom. These internal quantum degrees of freedom have provided an ideal laboratory for exploring both new physical phenomena and electronics and photonics applications. Valley- and spin-dependent optical and electrical properties, originated from Berry curvature effects, have been recently demonstrated. Such Berry curvature effects, together with strong spin-orbit interactions, can further generate unconventional Landau levels (LLs) under a perpendicular magnetic field that support valle…
Theoretical work has suggested that monolayer MoS2 doped with Mn should behave as a two-dimensional dilute magnetic semiconductor, which would open up possibilities for spintronic applications, device physics, and novel ground states. The magnetic properties on Mn dopants in MoS2 are dependent on the mid-gap impurity states of said dopants as well as the sites of dopant incorporation and dopant concentration. In this work we use STM/STS to characterize multiple impurity types associated with Mn dopants in MoS2, and use ring features that appear in spectral maps due to tip-induced band bending …
Very recently, it was demonstrated that the carrier mobility of a molecular monolayer dioctylbenzothienobenzothiophene (C8-BTBT) on boron nitride can reach 10 cm2/Vs, the highest among the previously reported monolayer molecular field-effect transistors. Here we show that the high-quality single crystal of the C8-BTBT monolayer may be the key origin of the record-high carrier mobility. We discover that the C8-BTBT molecules prefer layer-by-layer growth on both hexagonal boron nitride and graphene. The flatness of these substrates substantially decreases the C8-BTBT nucleation density and enabl…
To reduce Schottky-barrier-induced contact and access resistance, and the impact of charged impurity and phonon scattering on mobility in devices based on 2D transition metal dichalcogenides (TMDs), considerable effort has been put into exploring various doping techniques and dielectric engineering using $high-κ$ oxides, respectively. The goal of this work is to demonstrate a $high-κ$ dielectric that serves as an effective n-type charge transfer dopant on monolayer (ML) molybdenum disulfide ($MoS_{2}$). Utilizing amorphous titanium suboxide (ATO) as the '$high-κ$ dopant', we achieved a contact…
Two-dimensional transition metal dichalcogenide (TMD) semiconductors provide a unique possibility to access the electronic valley degree of freedom using polarized light, opening the way to valley information transfer between distant systems. Excitons with a well-defined valley index (or valley pseudospin) as well as superpositions of the exciton valley states can be created with light having circular and linear polarization, respectively. However, the generated excitons have short lifetimes (ps) and are also subject to the electron-hole exchange interaction leading to fast relaxation of the v…
We propose and study theoretically a new mechanism of electron-impurity scattering in doped seminconductors with large dielectric constant. It is based upon the idea of \textit{vector} character of deformations caused in the crystalline lattice by any point defects siting asymmetrically in the unit cell. In result, local lattice compression due to the elastic deformations decay as $1/r^2$ with distance from impurity. Electron scattering (due to standard deformation potential) on such defects leads to low-temperature mobility $μ(n)$ scaling with electron density $n$ of the form $μ(n) \propto n^…
We describe recent experimental efforts to perform polarization-resolved optical spectroscopy of monolayer transition-metal dichalcogenide semiconductors in very large pulsed magnetic fields to 65 tesla. The experimental setup and technical challenges are discussed in detail, and temperature-dependent magneto-reflection spectra from atomically thin tungsten disulphide (WS$_2$) are presented. The data clearly reveal not only the valley Zeeman effect in these 2D semiconductors, but also the small quadratic exciton diamagnetic shift from which the very small exciton size can be directly inferred.…
Moiré superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moiré bands in a crystal through interlayer hybridization when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moiré bands in a monolayer semiconductor. It relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their en…
Transition metal dichalcogenides (TMDs) are layered materials that have a semiconducting phase with many advantageous optoelectronic properties, including tightly bound excitons and spin-valley locking. In Tungsten-based TMDs, spin and momentum forbidden transitions give rise to dark excitons that typically are optically inaccessible but represent the lowest excitonic states of the system. Dark excitons can deeply affect transport, dynamics and coherence of bright excitons, hampering device performance. Therefore, it is crucial to create conditions in which these excitonic states can be visual…
Strain engineering is an important method for tuning the properties of semiconductors and has been used to improve the mobility of silicon transistors for several decades. Recently, theoretical studies have predicted that strain can also improve the mobility of two-dimensional (2D) semiconductors, e.g. by reducing intervalley scattering or lowering effective masses. Here, we experimentally show strain-enhanced electron mobility in monolayer MoS2 transistors with uniaxial tensile strain, on flexible substrates. The on-state current and mobility are nearly doubled with tensile strain up to 0.7%,…
Two-dimensional (2D) transition metal dichalcogenides (TMDs) exhibit novel electrical and optical properties and are emerging as a new platform for exploring 2D semiconductor physics. Reduced screening in 2D results in dramatically enhanced electron-electron interactions, which have been predicted to generate giant bandgap renormalization and excitonic effects. Currently, however, there is little direct experimental confirmation of such many-body effects in these materials. Here we present an experimental observation of extraordinarily large exciton binding energy in a 2D semiconducting TMD. W…
Defects in conventional semiconductors substantially lower the photoluminescence (PL) quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional (2D) transition metal dichalcogenides (TMDCs), such as monolayer MoS2, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic by electrostatic doping, without any chemical passivation. Surprisingly, neutra…
Optically generated excitons dictate the absorption and emission spectrum of doped semiconductor transition metal dichalcogenide monolayers. We show that upon increasing the electron density, the elementary optical excitations develop a roton-like dispersion, evidenced by a shift of the lowest energy state to a finite momentum on the order of the Fermi momentum. This effect emerges due to Pauli exclusion between excitons and the electron Fermi sea, but the robustness of the roton minimum in these systems is a direct consequence of the long-range nature of the Coulomb interaction and the nonloc…
We demonstrate superconducting vertical interconnect access (VIA) contacts to a monolayer of molybdenum disulfide (MoS$_2$), a layered semiconductor with highly relevant electronic and optical properties. As a contact material we use MoRe, a superconductor with a high critical magnetic field and high critical temperature. The electron transport is mostly dominated by a single superconductor/normal conductor junction with a clear superconductor gap. In addition, we find MoS$_2$ regions that are strongly coupled to the superconductor, resulting in resonant Andreev tunneling and junction dependen…
Three-dimensional confinement allows semiconductor quantum dots (QDs) to exhibit size-tunable electronic and optical properties that enable a wide range of opto-electronic applications from displays, solar cells and bio-medical imaging to single-electron devices. Additional modalities such as spin and valley properties can provide further degrees of freedom requisite for quantum information and spintronics. When seeking to combine these material features into QD structures, however, confinement can cause hybridization that inhibits the robustness of these emergent properties for insertion into…
Atomically thin (two-dimensional, 2D) semiconductors have shown great potential as the fundamental building blocks for next-generation electronics. However, all the 2D semiconductors that have been experimentally made so far have room-temperature electron mobility lower than that of bulk silicon, which is not understood. Here, by using first-principles calculations and reformulating the transport equations to isolate and quantify contributions of different mobility-determining factors, we show that the universally low mobility of 2D semiconductors originates from the high 'density of scatterin…
In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial --tens of teslas or more-- due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS$_2$, MoSe$_2$, MoTe$_2$, and WS$_2$ in very high magnetic fields to 91~T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton's $1s$ ground state but also …
The carrier mobility of anisotropic two-dimensional (2D) semiconductors under longitudinal acoustic (LA) phonon scattering was theoretically studied with the deformation potential theory. Based on Boltzmann equation with relaxation time approximation, an analytic formula of intrinsic anisotropic mobility was deduced, which shows that the influence of effective mass to the mobility anisotropy is larger than that of deformation potential constant and elastic modulus. Parameters were collected for various anisotropic 2D materials (black phosphorus, Hittorf's phosphorus, BC$_2$N, MXene, TiS$_3$, G…
We study the magnetotransport properties of high mobility holes in monolayer and bilayer WSe$_2$, which display well defined Shubnikov-de Haas (SdH) oscillations, and quantum Hall states (QHSs) in high magnetic fields. In both mono and bilayer WSe$_2$, the SdH oscillations and the QHSs occur predominantly at even filling factors, evincing a two-fold Landau level degeneracy. The Fourier transform analysis of the SdH oscillations in bilayer WSe$_2$ reveal the presence of two subbands localized in the top or the bottom layer, as well as negative compressibility. From the temperature dependence of…
Two-dimensional (2D) semiconductors are promising material candidates for next-generation nanoelectronics. However, there are fundamental challenges related to their metal-semiconductor (MS) contacts which limit the performance potential for practical device applications. In this work, we exploit 2D monolayer hexagonal boron nitride (h-BN) as an ultrathin decorating layer to form a metal-insulator-semiconductor (MIS) contact, and demonstrate a novel diode-like selective enhancement of the carrier transport through it. Compared to the conventional MS contact, the MIS contact dominated by both t…
We report magneto-absorption spectroscopy of gated WSe$_2$ monolayers in high magnetic fields up to 60~T. When doped with a 2D Fermi sea of mobile holes, well-resolved sequences of optical transitions are observed in both $σ^\pm$ circular polarizations, which unambiguously and separately indicate the number of filled Landau levels (LLs) in both $K$ and $K'$ valleys. This reveals the interaction-enhanced valley Zeeman energy, which is found to be highly tunable with hole density $p$. We exploit this tunability to align the LLs in $K$ and $K'$, and find that the 2D hole gas becomes unstable agai…
Using a spatially-resolved optical pump-probe experiment, we measure the lateral transport of spin/valley polarized electrons over very long distances (tens of micrometers) in a single WSe2 monolayer. By locally pumping the Fermi sea of 2D electrons to a high degree of spin/valley polarization (up to 75%) using circularly-polarized light, the lateral diffusion of the electron polarization can be mapped out via the photoluminescence induced by a spatially-separated and linearly-polarized probe laser. Up to 25% spin-valley polarization is observed at pump-probe separations up to 20 microns. Char…
Using time-resolved optical Kerr rotation, we measure the low temperature valley dynamics of resident electrons and holes in exfoliated WSe$_2$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically-gated WSe$_2$ monolayers having different dielectric environments. In a fully-encapsulated structure (hBN/WSe$_2$/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to…
