High Electron Mobility, Quantum Hall Effect and Anomalous Optical Response in Atomically Thin InSe
D. A. Bandurin, A. V. Tyurnina, G. L. Yu, A. Mishchenko, V. Zolyomi, S. V. Morozov, R. Krishna Kumar, R. V. Gorbachev, Z. R. Kudrynskyi, S. Pezzini, Z. D. Koval… 展开作者
D. A. Bandurin, A. V. Tyurnina, G. L. Yu, A. Mishchenko, V. Zolyomi, S. V. Morozov, R. Krishna Kumar, R. V. Gorbachev, Z. R. Kudrynskyi, S. Pezzini, Z. D. Kovalyuk, U. Zeitler, K. S. Novoselov, A. Patane, L. Eaves, I. V. Grigorieva, V. I. Fal'ko, A. K. Geim, Y. Cao
A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 1,000 and 10,000 cm2/Vs at room and liquid-helium temperatures, respectively, allowing the observation of the fully-developed quantum Hall effect. The conduction electrons occupy a single 2D subband and have a small effective mass. Photoluminescence spectroscopy reveals that the bandgap increases by more than 0.5 eV with decreasing the thickness from bulk to bilayer InSe. The band-edge optical response vanishes in monolayer InSe, which is attributed to monolayer's mirror-plane symmetry. Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically-thin dichalcogenides and black phosphorus.
We propose atomic films of n-doped $γ$-InSe as a platform for intersubband optics in the infrared (IR) and far infrared (FIR) range, coupled to out-of-plane polarized light. Depending on the film thickness (number of layers) of the InSe film these transitions span from $\sim 0.7$ eV for bilayer to $\sim 0.05$ eV for 15-layer InSe. We use a hybrid $\mathbf{k} \cdot \mathbf{p}$ theory and tight-binding model, fully parametrized using density functional theory, to predict their oscillator strengths and thermal linewidths at room temperature.
We perform a $\mathbf{k \cdot p}$ theory analysis of the spectra of the lowest energy and excited states of the excitons in few-layer atomically thin films of InSe taking into account in-plane electric polarizability of the film and the influence of the encapsulation environment. For the thinner films, the lowest-energy state of the exciton is weakly indirect in momentum space, with its dispersion showing minima at a layer-number-dependent wave number, due to an inverted edge of a relatively flat topmost valence band branch of the InSe film spectrum and we compute the activation energy from th…
Atomically thin two-dimensional chalcogenides such as MoS2 monolayers are structurally ideal channel materials for the ultimate atomic electronics. However, a heavy thickness dependence of electrical performance is shown in these ultrathin materials, and the device performance normally degrades while exhibiting a low carrier mobility as compared with corresponding bulks, constituting a main hurdle for application in electronics. In this brief review, we summarize our recent work on electrode/channel contacts and carrier scattering mechanisms to address the origins of this adverse thickness dep…
The structure and mobility of dislocations in the layered semiconductor InSe is studied within a multiscale approach based on generalized Peierls--Nabarro model with material-specific parametrization derived from first principles. The plasticity of InSe turns out to be attributed to peculiarities of the generalized stacking fault relief for the interlayer dislocation slips such as existence of the stacking fault with a very low energy and low energy barriers. Our results give a consistent microscopic explanation of recently observed [Science {\bf 369}, 542 (2020)] exceptional plasticity of InS…
Van der Waals materials offer a wide range of atomic layers with unique properties that can be easily combined to engineer novel electronic and photonic devices. A missing ingredient of the van der Waals platform is a two-dimensional crystal with naturally occurring out-of-plane luminescent dipole orientation. Here we measure the far-field photoluminescence intensity distribution of bulk InSe and two-dimensional InSe, WSe$_2$ and MoSe$_2$. We demonstrate, with the support of ab-initio calculations, that layered InSe flakes sustain luminescent excitons with an intrinsic out-of-plane orientation…
High mobility two-dimensional hole system on hydrogen-terminated silicon (111) surfaces
我们实现了一个二维空穴系统（2DHS），其中2DHS是由施加在真空腔两端的负栅电压在原子级平坦的氢终止的Si（111）表面上诱导的。在70 mK时，空穴密度可达$7.5\times10^{11}$ cm $^{-2}$，峰值空穴迁移率约为$10^4$ cm $^2$ /Vs.观察到了量子霍尔效应。Shubnikov-de Haas振荡由于自旋轨道效应而显示出拍频模式，并且推测的零场自旋分裂可以通过栅极电压来调节。
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…
Graphene-like two-dimensional (2D) materials, not only are interesting for their exotic electronic structure and fundamental electronic transport or optical properties but also, hold promises for device miniaturization down to atomic thickness. As one material belonging to this category, InSe is not only a promising candidate for optoelectronic devices but also has potential for ultrathin field effect transistor (FET) with high mobility transport. In this work, various substrates such as PMMA, bare silicon oxide, passivated silicon oxide, and silicon nitride were used to fabricate multi-layer …
Understanding and optimizing the properties of photoactive two-dimensional (2D) Van der Waals solids are crucial for developing optoelectronics applications. Here we present a detailed investigation of layer dependent photoconductive behavior of InSe based field-effect transistors (FETs). InSe based FETs with five different channel thickness (t, 20 nm < t < 100 nm) were investigated with a continuous laser source of λ = 658 nm (1.88 eV) over a wide range of illumination power of 22.8 nW < P < 1.29 μW. All the devices studied, showed signatures of photogating, however, our investigations sugges…
Resistance in superconductors arises from the motion of vortices driven by flowing supercurrents or external electromagnetic fields and may be strongly affected by thermal or quantum fluctuations. The common expectation borne out in previous experiments is that as the temperature is lowered, vortex motion is suppressed, leading to a decreased resistance. A new generation of materials provides access to the previously inaccessible regime of clean-limit superconductivity in atomically thin superconducting layers. We show experimentally that for few-layer 2H-NbSe$_2$ the resistance below the supe…
The ability of spin-orbit interactions to convert charge current into spin current, most often in the bulk of heavy metal thin films, has been the hallmark of spintronics in the last decade. In this study, we demonstrate how the insertion of light metal element interface profoundly affects both the nature of spin-orbit torque and its efficiency in terms of damping-like ($H_{\text{DL}}$) and field-like ($H_{\text{FL}}$) effective fields in ultrathin Co ferromagnet. Indeed, we measure unexpectedly large $H_{\text{FL}}$/$H_{\text{DL}}$ ratio ($\sim$2.5) upon inserting a 1.4 nm thin Al layer in Pt…
Next-generation electronics calls for new materials beyond silicon for increased functionality, performance, and scaling in integrated circuits. Carbon nanotubes and semiconductor nanowires are at the forefront of these materials, but have challenges due to the complex fabrication techniques required for large-scale applications. Two-dimensional (2D) gapless graphene and semiconducting transition metal dichalcogenides (TMDCs) have emerged as promising electronic materials due to their atomic thickness, chemical stability and scalability. Difficulties in the assembly of 2D electronic structures…
Post-transition metal chalcogenides (PTMCs) such as GaSe, GaS, InSe, and InS have been proposed as promising thermoelectric materials due to low lattice conductivity, originating from the atomically layered structure, high Seebeck coefficient, and the anticipation that its figure-of-merit be improved when thinned to few-layers as the band structure turns into Mexican-hat valence band (MHVB). Here we show by ab initio calculations that the MHVB should be present even on thick films of InSe/GaSe type-II heterostructures, and a 50% enhancement on thermoelectric figure-of-merit zT at room-temperat…
The transfer of graphene grown by chemical vapor deposition (CVD) using amorphous polymers represents a widely implemented method for graphene-based electronic device fabrication. However, the most commonly used polymer, poly(methyl methacrylate) (PMMA), leaves a residue on the graphene that limits the mobility. Here we report a method for graphene transfer and patterning that employs a perfluoropolymer---Hyflon---as a transfer handle and to protect graphene against contamination from photoresists or other polymers. CVD-grown graphene transferred this way onto LaAlO$_3$/SrTiO$_3$ heterostructu…
The extraordinary properties of two dimensional (2D) materials, such as the extremely high carrier mobility in graphene and the large direct band gaps in transition metal dichalcogenides MX2 (M = Mo or W, X = S, Se) monolayers, highlight the crucial role quantum confinement can have in producing a wide spectrum of technologically important electronic properties. Currently one of the highest priorities in the field is to search for new 2D crystalline systems with structural and electronic properties that can be exploited for device development. In this letter, we report on the unusual quantum t…
Atomically thin, two-dimensional (2D) indium selenide (InSe) has attracted considerable attention due to large tunability in the band gap (from 1.4 to 2.6 eV) and high carrier mobility. The intriguingly high dependence of band gap on layer thickness may lead to novel device applications, although its origin remains poorly understood, and generally attributed to quantum confinement effect. In this work, we demonstrate via first-principles calculations that strong interlayer coupling may be mainly responsible for this phenomenon, especially in the fewer-layer region, and it could also be an esse…
Van der Waals heterostructures formed by stacking different types of 2D materials are attracting increasing attention due to new emergent physical properties such as interlayer excitons. Recently synthesized atomically thin indium selenide (InSe) and antimony (Sb) individually exhibit interesting electronic properties such as high electron mobility in the former and high hole mobility in the latter. In this work, we present a first-principles investigation on the stability and electronic properties of ultrathin bilayer heterostructures composed of InSe and Sb single layers. The calculated elec…
Electrolyte gating is a powerful technique for accumulating large carrier densities in surface two-dimensional electron systems (2DES). Yet this approach suffers from significant sources of disorder: electrochemical reactions can damage or alter the surface of interest, and the ions of the electrolyte and various dissolved contaminants sit Angstroms from the 2DES. Accordingly, electrolyte gating is well-suited to studies of superconductivity and other phenomena robust to disorder, but of limited use when reactions or disorder must be avoided. Here we demonstrate that these limitations can be o…
Two-dimensional semiconductors are excellent candidates for next-generation electronics and optoelec-tronics thanks to their electrical properties and strong light-matter interaction. To fabricate devices with optimal electrical properties, it is crucial to have both high-quality semiconducting crystals and ideal con-tacts at metal-semiconductor interfaces. Thanks to the mechanical exfoliation of van der Waals crystals, atomically-thin high-quality single-crystals can easily be obtained in a laboratory. However, conventional metal deposition techniques can introduce chemical disorder and metal…
Atomically-thin 2D semiconducting materials integrated into van der Waals heterostructures have enabled architectures that hold great promise for next generation nanoelectronics. However, challenges still remain to enable their full acceptance as compliant materials for integration in logic devices. Two key-components to master are the barriers at metal/semiconductor interfaces and the mobility of the semiconducting channel, which endow the building-blocks of ${pn}$ diode and field effect transistor. Here, we have devised a reverted stacking technique to intercalate a wrinkle-free h-BN tunnel …
Optical and transport properties of doped monolayer semiconductors are dominated by trions, which are three-particle compounds formed by two electrons and one hole or vice versa. In this work, we investigate the trion-phonon interaction on a microscopic footing and apply our model to the exemplary case of a molybdenum diselenide (MoSe2) monolayer. We determine the trion series of states and their internal quantum structure by solving the trion Schrödinger equation. Transforming the system into a trion basis and solving equations of motion, including the trion-phonon interaction within the seco…
The discovery of archetypal two-dimensional (2D) materials provides enormous opportunities in both fundamental breakthroughs and device applications, as evident by the research booming in graphene, atomically thin transition-metal chalcogenides, and few-layer black phosphorous in the past decade. Here, we report a new, large family of semiconducting dialkali-metal monochalcogenides (DMMCs) with an inherent A$_{2}$X monolayer structure, in which two alkali sub-monolayers form hexagonal close packing and sandwich the triangular chalcogen atomic plane. Such unique lattice structure leads to extra…
The field of two-dimensional materials has been developing at an impressive pace, with atomically thin crystals of an increasing number of different compounds that have become available, together with techniques enabling their assembly into functional heterostructures. The strategy to detect these atomically thin crystals has however remained unchanged since the discovery of graphene. Such an absence of evolution is starting to pose problems because for many of the 2D materials of current interest the optical contrast provided by the commonly used detection procedure is insufficient to identif…
Few-layer InSe draws tremendous research interests owing to the superior electronic and optical properties. It exhibits high carrier mobility up to more than 1000 cm2/Vs at room temperature. The strongly layer-tunable band gap spans a large spectral range from near-infrared to the visible. In this perspective, we systematically review the optical properties of few-layer InSe. Firstly, the intrinsic optical and electronic properties are introduced. Compared to other two-dimensional (2D) materials, the light-matter interaction of few-layer InSe is unusual. The band gap transition is inactive or …
The 2D electrons trapped in vacuum near the atomically thin dielectric (ATD, mono- or $N$-layer film of $h$-BN or transition metal dichalcogenide) are considered. ATD is suspended above the back gate and forms the capacitor which is controlled by the biased voltage determining 2D concentration, $n_{2D}$. It is found that the leakage current through ATD is negligible and effect of the polarizability of ATD is weak if $N\leq 5$. At temperatures $T=0.1÷$15 K and $n_{2D}=5\times 10^8÷10^{10}$ cm$^{-2}$, one deals with the Boltzmann liquid of the macroscopic thickness $\sim$100 A. Due to bending of…
As a high mobility two-dimensional semiconductor with strong structural and electronic anisotropy, atomically thin black phosphorus (BP) provides a new playground for investigating the quantum Hall (QH) effect, including outstanding questions such as the functional dependence of Landau level (LL) gaps on magnetic field B, and possible anisotropic fractional QH states. Using encapsulating few-layer BP transistors with mobility up to 55,000 cm2/Vs, we extract LL gaps over an exceptionally wide range of B for QH states at filling factors ν=-1 to -4, which are determined to be linear in B, thus re…
Spin-orbit coupling (SOC) is a relativistic effect, where an electron moving in an electric field experiences an effective magnetic field in its rest frame. In crystals without inversion symmetry, it lifts the spin degeneracy and leads to many magnetic, spintronic and topological phenomena and applications. In bulk materials, SOC strength is a constant that cannot be modified. Here we demonstrate SOC and intrinsic spin-splitting in atomically thin InSe, which can be modified over an unprecedentedly large range. From quantum oscillations, we establish that the SOC parameter αis thickness-depend…
The electrical contact to two-dimensional (2D)-semiconductor materials are decisive to the electronic performance of 2D-semiconductor field-effect devices (FEDs). The presence of a Schottky barrier often leads to a large contact resistance, which seriously limits the channel conductance and carrier mobility measured in a two-terminal geometry. In contrast, ohmic contact is desirable and can be achieved by the presence of a nonrectifying or tunneling barrier. Here, we demonstrate that an nonrectifying barrier can be realized by contacting indium (In), a low work function metal, with layered InS…
InSe, a member of the layered materials family, is a superior electronic and optical material which retains a direct bandgap feature from the bulk to atomically thin few-layers and high electronic mobility down to a single layer limit. We, for the first time, exploit strain to drastically modify the bandgap of two-dimensional (2D) InSe nanoflakes. We demonstrated that we could decrease the bandgap of a few-layer InSe flake by 160 meV through applying an in-plane uniaxial tensile strain to 1.06% and increase the bandgap by 79 meV through applying an in-plane uniaxial compressive strain to 0.62%…
Two-dimensional semiconductors - atomic layers of materials with covalent intra-layer bonding and weak (van der Waals or quadrupole) coupling between the layers - are a new class of materials with great potential for optoelectronic applications. Among those, a special position is now being taken by post-transition metal chalcogenides (PTMC), InSe and GaSe. It has recently been found that the band gap in 2D crystals of InSe more than doubles in the monolayer compared to thick multilayer crystals, while the high mobility of conduction band electrons is promoted by their light in-plane mass. Here…
Atomically thin black phosphorus (BP) is a promising two-dimensional material for fabricating electronic and optoelectronic nano-devices with high mobility and tunable bandgap structures. However, the charge-carrier mobility in few-layer phosphorene (monolayer BP) is mainly limited by the presence of impurity and disorders. In this study, we demonstrate that vertical BP heterostructure devices offer great advantages in probing the electron states of monolayer and few-layer phosphorene at temperatures down to 2 K through capacitance spectroscopy. Electronic states in the conduction and valence …
We show that hole states in recently discovered single-layer InSe are strongly renormalized by the coupling with acoustic phonons. The coupling is enhanced significantly at moderate hole doping ($\sim$10$^{13}$ cm$^{-2}$) due to hexagonal warping of the Fermi surface. While the system remains dynamically stable, its electron-phonon spectral function exhibits sharp low-energy resonances, leading to the formation of satellite quasiparticle states near the Fermi energy. Such many-body renormalization is predicted to have two important consequences. First, it significantly suppresses charge carrie…
Indium selenide, a post-transition metal chalcogenide, is a novel two-dimensional (2D) semiconductor with interesting electronic properties. Its tunable band gap and high electron mobility have already attracted considerable research interest. Here we demonstrate strong quantum confinement and manipulation of single electrons in devices made from few-layer crystals of InSe using electrostatic gating. We report on gate-controlled quantum dots in the Coulomb blockade regime as well as one-dimensional quantization in point contacts, revealing multiple plateaus. The work represents an important mi…
The two-dimensional (2D) semiconductor indium selenide (InSe) has attracted significant interest due its unique electronic band structure, high electron mobility and wide tunability of its band gap energy achieved by varying the layer thickness. All these features make 2D InSe a potential candidate for advanced electronic and optoelectronic applications. Here, we report on the discovery of new polymorphs of InSe with enhanced electronic properties. Using a global structure search that combines artificial swarm intelligence with first-principles energetic calculations, we identify polymorphs th…
We demonstrate that encapsulation of atomically thin black phosphorus (BP) by hexagonal boron nitride (h-BN) sheets is very effective for minimizing the interface impurities induced during fabrication of BP channel material for quantum transport nanodevices. Highly stable BP nanodevices with ultrahigh mobility and controllable types are realized through depositing appropriate metal electrodes after conducting a selective etching to the BP encapsulation structure. Chromium and titanium are suitable metal electrodes for BP channels to control the transition from a p-type unipolar property to amb…
We report ab initio calculations of the spin splitting of the uppermost valence band (UVB) and the lowermost conduction band (LCB) in bulk and atomically thin GaS, GaSe, GaTe, and InSe. These layered monochalcogenides appear in four major polytypes depending on the stacking order, except for the monoclinic GaTe. Bulk and few-layer $ε$- and $γ$-type, and odd-number $β$-type GaS, GaSe, and InSe crystals are noncentrosymmetric. The spin splittings of the UVB and the LCB near the $Γ$-point in the Brillouin zone are finite, but still smaller than those in a zinc-blende semiconductor such as GaAs. O…
In the last six years, Indium selenide (InSe) has appeared as a new van der Waals heterostructure platform which has been extensively studied due to its unique electronic and optical properties. Such as transition metal dichalcogenides (TMDCs), the considerable bandgap and high electron mobility can provide a potential optoelectronic application. Here we present low-temperature transport measurements on a few-layer InSe van der Waals heterostructure with graphene-gated contacts. For high magnetic fields, we observe magnetoresistance minima at even filling factors related to two-fold spin degen…
The singular density of states and the two Fermi wavevectors resulting from a ring-shaped or "Mexican hat" valence band give rise to unique trends in the charged impurity scattering rates and charged impurity limited mobilities. Ring shaped valence bands are common features of many monolayer and few-layer two-dimensional materials including the III-VI materials GaS, GaSe, InS, and InSe. The wavevector dependence of the screening, calculated within the random phase approximation, is so strong that it is the dominant factor determining the overall trends of the scattering rates and mobilities wi…
How atoms acquire three-dimensional bulk character is one of the fundamental questions in materials science. Before addressing this question, how atomic layers become a bulk crystal might give a hint to the answer. While atomically thin films have been studied in a limited range of materials, a recent discovery showing how to mechanically exfoliate bulk crystals has opened up the field to study the atomic layers of various materials. Here, we show systematic variation in the band structure of high mobility graphene with one to seven layers by measuring the quantum oscillation of magnetoresista…
