Development of new, high quality functional materials has been at the forefront of condensed matter research. The recent advent of two-dimensional black phosphorus has greatly enriched the material base of two-dimensional electron systems. Significant progress has been made to achieve high mobility black phosphorus two-dimensional electron gas (2DEG) since the development of the first black phosphorus field-effect transistors (FETs)$^{1-4}$. Here, we reach a milestone in developing high quality black phosphorus 2DEG - the observation of integer quantum Hall (QH) effect. We achieve high quality by embedding the black phosphorus 2DEG in a van der Waals heterostructure close to a graphite back gate; the graphite gate screens the impurity potential in the 2DEG, and brings the carrier Hall mobility up to 6000 $cm^{2}V^{-1}s^{-1}$. The exceptional mobility enabled us, for the first time, to observe QH effect, and to gain important information on the energetics of the spin-split Landau levels in black phosphorus. Our results set the stage for further study on quantum transport and device application in the ultrahigh mobility regime.
The advent of black phosphorus field-effect transistors (FETs) has brought new possibilities in the study of two-dimensional (2D) electron systems. In a black phosphorus FET, the gate induces highly anisotropic 2D electron and hole gases. Although the 2D hole gas in black phosphorus has reached high carrier mobilities that led to the observation of the integer quantum Hall effect, the improvement in the sample quality of the 2D electron gas (2DEG) has however been only moderate; quantum Hall effect remained elusive. Here, we obtain high quality black phosphorus 2DEG by defining the 2DEG region…
We implement the molecular beam epitaxy method to embed the black-phosphorus-like bismuth nanosheets into the bulk ferromagnet Cr$_2$Te$_3$. As a typical surfactant, bismuth lowers the surface tensions and mediates the layer-by-layer growth of Cr$_2$Te$_3$. Meanwhile, the bismuth atoms precipitate into black-phosphorus-like nanosheets with the lateral size of several tens of nanometers. In Cr$_2$Te$_3$ embedded with Bi-nanosheets, we observe simultaneously a large topological Hall effect together with the magnetic susceptibility plateau and magnetoresistivity anomaly. As a control experiment, …
Quantum wells constitute one of the most important classes of devices in the study of 2D systems. In a double layer QW, the additional "which-layer" degree of freedom gives rise to celebrated phenomena such as Coulomb drag, Hall drag and exciton condensation. Here we demonstrate facile formation of wide QWs in few-layer black phosphorus devices that host double layers of charge carriers. In contrast to tradition QWs, each 2D layer is ambipolar, and can be tuned into n-doped, p-doped or intrinsic regimes. Fully spin-polarized quantum Hall states are observed on each layer, with enhanced Lande g…
We study the quantum Hall effect of 2D electron gas in black phosphorus in the presence of perpendicular electric and magnetic fields. In the absence of a bias voltage, the external magnetic field leads to a quantization of the energy spectrum into equidistant Landau levels, with different cyclotron frequencies for the electron and hole bands. The applied voltage reduces the band gap, and eventually a semiconductor to semimetal transition takes place. This nontrivial phase is characterized by the emergence of a pair of Dirac points in the spectrum. As a consequence, the Landau levels are not e…
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…
We realize p-p'-p junctions in few-layer black phosphorus (BP) devices, and use magneto-transport measurements to study the equilibration and transmission of edge states at the interfaces of regions with different charge densities. We observe both full equilibration, where all edge channels equilibrate and are equally partitioned at the interfaces, and partial equilibration, where only equilibration only takes place among modes of the same spin polarization. Furthermore, the inner p'-region with low-doping level in the junction can function as a filter for highly doped p-regions which demonstr…
Ultrafast nonlinear Hall effect in black phosphorus
Fritz Haber Institute of the Max Planck Society（马克斯·普朗克学会弗里茨·哈伯研究所）；KTH Royal Institute of Technology（皇家理工学院）；CNR-ISM, Division of Ultrafast Processes in Materials (FLASHit)（意大利国家研究委员会材料科学研究所超快过程部门（FLASHit））；CELIA, University of Bordeaux–CNRS–CEA（波尔多大学-法国国家科学研究中心-法国原子能和替代能源委员会联合实验室）；Beijing National Laboratory for Condensed Matter Physics, Chinese Academy of Sciences（中国科学院凝聚态物理国家实验室）；Institute for Optics and Atomic Physics, Technical University Berlin（柏林工业大学光学与原子物理研究所）；Department of Physics, Tor Vergata University of Rome（罗马托尔维尔加塔大学物理系）
The origin of phonon thermal Hall Effect (THE) observed in a variety of insulators is yet to be identified. Here, we report on the observation of a thermal Hall conductivity in a non-magnetic elemental insulator, with an amplitude exceeding what has been previously observed. In black phosphorus (BP), the longitudinal ($κ_{ii}$), and the transverse, $κ_{ij}$, thermal conductivities peak at the same temperature and at this peak temperature, the $κ_{ij}/κ_{jj}/B $ is $\approx 10^{-4}$-$10^{-3}$ T$^{-1}$. Both these features are shared by other insulators displaying THE, despite an absolute amplit…
Two-dimensional electron gases (2DEG) have been an important source of experimental discovery and conceptual development in condensed matter physics for decades. When combined with the unique electronic properties of two-dimensional (2D) crystals, rich new physical phenomena can be probed at the quantum level. Here, we create a new 2DEG in black phosphorus, a recent member of the two-dimensional atomic crystal family, using a gate electric field. We achieve high carrier mobility in black phosphorus 2DEG by placing it on a hexagonal boron nitride substrate (h-BN). This allows us, for the first …
Newly fabricated monolayer phosphorene and its few-layer structures are expected to be promising for electronic and optical applications because of their finite direct band gaps and sizable but anisotropic electronic mobility. By first-principles simulations, we show that this unique anisotropic conductance can be controlled by using simple strain conditions. With the appropriate biaxial or uniaxial strain, we can rotate the preferred conducting direction by 90 degrees. This will be of useful for exploring quantum Hall effects, and exotic electronic and mechanical applications based on phospho…
We have conducted a comprehensive investigation into the magneto-transport properties of few-layer black phosphorus in terms of phase coherence length, phase coherence time, and mobility via weak localization measurement and Hall-effect measurement. We present magnetoresistance data showing the weak localization effect in bare p-type few-layer black phosphorus and reveal its strong dependence on temperature and carrier concentration. The measured weak localization agrees well with the Hikami-Larkin-Nagaoka model and the extracted phase coherence length of 104 nm at 350 mK, decreasing as ~T^-0.…
Phosphorene is a novel two-dimensional material that can be isolated through mechanical exfoliation from layered black phosphorus, but unlike graphene and silicene, monolayer phosphorene has a large band gap. It was thus unsuspected to exhibit band inversion and the ensuing topological insulator behavior. It has recently attracted interest because of its proposed application as field effect transistors. Using first-principles calculations with applied perpendicular electric field F we predict a continuous transition from the normal insulator to a topological insulator and eventually to a metal…
We report electrically detected magnetic resonance of phosphorus donors in a silicon field-effect transistor. An on-chip transmission line is used to generate the oscillating magnetic field allowing broadband operation. At milli-kelvin temperatures, continuous wave spectra were obtained up to 40 GHz, using both magnetic field and microwave frequency modulation. The spectra reveal the hyperfine-split electron spin resonances characteristic for Si:P and a central feature which displays the fingerprint of spin-spin scattering in the two-dimensional electron gas.
We report on the electronic transport properties of black phosphorus and analyze them using a two-carrier model in a wide range of pressure up to 2.5 GPa. In semiconducting state at 0.29 GPa, the remarkable non-linear behavior in the Hall resistance is reasonably reproduced by assuming the coexistence of two kinds of hole with different densities and mobilities. On the other hand, two-carrier analyses of the magnetotransport properties above 1.01 GPa suggest the coexistence of high mobility electron and hole carriers that have almost the same densities, i.e., nearly compensated semimetallic na…
Few layer black phosphorus is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of stability severely limits our ability to synthesise and process this material. Here we demonstrate that high-quality, few-layer black phosphorus nanosheets can be produced in large quantities by liquid phase exfoliation in the solvent N-cyclohexyl-2-pyrrolidone (CHP). We can control nanosheet dimensions and have developed metrics to estimate both nanosheet size and thickness spectroscopically. When exfoliated in CHP, the nanosheets are remarkably…
Ultrathin black phosphorus, or phosphorene, is the second known elementary two-dimensional material that can be exfoliated from a bulk van der Waals crystal. Unlike graphene it is a semiconductor with a sizeable band gap and its excellent electronic properties make it attractive for applications in transistor, logic, and optoelectronic devices. However, it is also the first widely investigated two dimensional electronic material to undergo degradation upon exposure to ambient air. Therefore a passivation method is required to study the intrinsic material properties, understand how oxidation af…
Single crystals of orthorhombic black phosphorus can be grown by a short way transport reaction from red phosphorus and Sn/SnI4 as mineralization additive. Sizes of several millimeters can be realized with high crystal quality and purity, making a large area preparation of single or multilayer phosphorene possible. An in situ neutron diffraction study has been performed addressing the formation of black phosphorus. Black phosphorus is formed directly via gas phase without the occurrence of any other intermediate phase. Crystal growth was initiated after cooling the starting materials down from…
We report ambipolar transport properties in black phosphorus using an electric-double-layer transistor (EDLT) configuration. The transfer curve clearly exhibits ambipolar transistor behavior with an ON-OFF ratio of 5*10^3. The band gap was determined as = 0.35 eV from the transfer curve, and Hall-effect measurements revealed that the hole mobility was ~ 190 cm^2/Vs at 170 K, which is one order of magnitude larger than the electron mobility. By inducing an ultra-high carrier density of ~ 10^14 cm^-2, an electric-field-induced transition from the insulating state to the metallic state was realiz…
We examine the electronic properties of 2D electron gas in black phosphorus multilayers in the presence of a perpendicular magnetic field, highlighting the role of in-plane anisotropy on various experimental quantities such as ac magneto-conductivity, screening, and magneto-plasmons. We find that resonant structures in the ac conductivity exhibits a red-shift with increasing doping due to inter-band coupling, $γ$. This arises from an extra correction term in the Landau energy spectrum proportional to $n^2γ^2$ ($n$ is Landau index), up to second order in $γ$. We found also that Coulomb interact…
The travel of heat in insulators is commonly pictured as a flow of phonons scattered along their individual trajectory. In rare circumstances, momentum-conserving collision events dominate, and thermal transport becomes hydrodynamic. One of these cases, dubbed the Poiseuille flow of phonons, can occur in a temperature window just below the peak temperature of thermal conductivity. We report on a study of heat flow in bulk black phosphorus between 0.1 and 80 K. We find a thermal conductivity showing a faster than cubic temperature dependence between 5 and 12 K. Consequently, the effective phono…
Black phosphorus (bP) is the second known elemental allotrope with a layered crystal structure that can be mechanically exfoliated down to atomic layer thickness. We have fabricated bP naked quantum wells in a back-gated field effect transistor geometry with bP thicknesses ranging from $6\pm1$ nm to $47\pm1$ nm. Using an encapsulating polymer superstrate, we have suppressed bP oxidation and have observed field effect mobilities up to 600 cm$^2$/Vs and on/off current ratios exceeding $10^5$. Importantly, Shubnikov-de Haas (SdH) oscillations observed in magnetotransport measurements up to 35 T r…
We are reporting a new synthetic strategy to grow large size black phosphorus (Black-P) crystals through a ternary clathrate Sn$_{24}$P$_{22-x}$I$_8$, under lower synthetic temperature and pressure. The Black-P crystals are found grown in situ at the site where the solid clathrate originally resides, which suggests chemical vapor mineralizer does not play a critical role for the Black-P formation. More detailed systematical studies has indicated the P vacancies in the framework of ternary clathrate Sn$_{24}$P$_{22-x}$I$_8$ is important for the subsequent Black-P from phosphorus vapors, and a l…
Anisotropy refers to the property of a material exhibiting directionally dependent features. In this paper, we introduce black phosphorous (BP), the most stable allotrope of phosphorus in layered orthorhombic structure with a bandgap of 0.3 eV in bulk, as a unique 2D material in which electrons, phonons and their interactions with photons behave in a highly anisotropic manner within the plane of the layers. The unique anisotropic nature of BP thin films is revealed using angle-resolved Raman and infrared spectroscopies, together with angle-resolved transport study. For 15 nm thick BP, we measu…
Artificial lattices have been employed in many two-dimensional systems, including those of electrons, atoms and photons, in a quest for massless Dirac particles with flexibility and controllability. Periodically patterned molecule assembly and electrostatic gating as well as moiré pattern induced by substrate, have produced electronic states with linear dispersions from isotropic two-dimensional electron gas (2DEG). Here we demonstrate that massless Dirac fermions with tunable anisotropic characteristics can, in general, be generated in highly anisotropic 2DEG under slowly varying external per…
This paper describes a simple microwave apparatus to measure the Hall effect in semiconductor wafers. The advantage of this technique is that it does not require contacts on the sample or the use of a resonant cavity. Our method consists of placing the semiconductor wafer into a slot cut in an X-band (8 - 12 GHz) waveguide series tee, injecting microwave power into the two opposite arms of the tee, and measuring the microwave output at the third arm. A magnetic field applied perpendicular to the wafer gives a microwave Hall signal that is linear in the magnetic field and which reverses phase w…
Direct visualizations of spin accumulation due to the enhanced spin Hall effect (SHE) in bismuth (Bi) - doped silicon (Si) at room temperature are realized by using helicity-dependent photovoltage (HDP) measurements. Under application of a dc current to the Bi-doped Si, clear helicity-dependent photovoltages are detected at the edges of the Si channel, indicating a perpendicular spin accumulation due to the SHE. In contrast, the HDP signals are negligibly small for phosphorus-doped Si. Compared to a platinum channel, which has a large spin Hall angle, more than two-orders of magnitude larger H…
The quantum anomalous Hall effect has recently been observed experimentally in thin films of Cr doped (Bi,Sb)$_2$Te$_3$ at a low temperature ($\sim$ 30mK). In this work, we propose realizing the quantum anomalous Hall effect in more conventional diluted magnetic semiconductors with doped InAs/GaSb type II quantum wells. Based on a four band model, we find an enhancement of the Curie temperature of ferromagnetism due to band edge singularities in the inverted regime of InAs/GaSb quantum wells. Below the Curie temperature, the quantum anomalous Hall effect is confirmed by the direct calculation …
Two-dimensional (2D) materials, such as graphene and transition metal dichalcogenides have attracted great attention because of the rich physics and potential applications in next-generation nano-sized electronic devices. Recently, atomically thin black phosphorus (BP) has become a new member of the 2D materials family with high theoretical mobility and tunable bandgap structure. However, degradation of properties under atmospheric conditions and high-density charge traps in BP have largely limited its mobility (~400 cm2/Vs at room temperature) and thus restricted its future applications. Here…
A nonequilibrium Green's functions approach to spin-Hall effect is developed in a diffusive two-dimensional electron system with Rashba spin-orbit interaction. In the presence of long-range impurities, the coupled quantum kinetic equations are solved analytically in the self-consistent Born approximation. It is shown that the intrinsic spin-Hall effect stems from the dc-field-induced perturbation of the density of states. In addition, there is an additional disorder-mediated process, which involves the transition of nonequilibrium electrons between two spin-orbit-coupled bands. It results in a…
We propose a nonequilibrium Green's function approach to study the spin-Hall effect in a two-dimensional electron system with both the Rashba and Dresselhaus spin-orbit couplings. By taking into account the long-range electron-impurity scattering, the derived kinetic equations are solved numerically. It is found the vanishing of the total zero-temperature dissipationless spin-Hall effect, contributing from the intrinsic and disorder-mediated processes. This result has been examined in the wide ranges of spin-orbit coupling constants and electron density.
We propose that a quantum anomalous Hall insulator (QAHI) can be realized in a nanopatterned two-dimensional electron gas (2DEG) with a small in-plane magnetic field and a high carrier density. The Berry curvatures originating from the in-plane magnetic field and Rashba and Dresselhaus spin-orbit coupling, in combination with a nanoscale honeycomb lattice potential modulation, lead to topologically nontrivial insulating states in the 2DEG without Landau levels. In the bulk insulating gaps, the anomalous Hall conductivity is quantized $-e^{2}/h$, corresponding to a finite Chern number -1. There…
The spin Hall effect is investigated in a high mobility two dimensional electron system with the spin-orbital coupling of both the Rashba and the Dresselhaus types. A spin current perpendicular to the electric field is generated by either the Rashba or the Dresselhaus coupling. The spin Hall conductance is independent of the stength of the coupling, but its sign is determined by the relative ratio of the two couplings. The direction of spin current is controllable by tuning the magnitude of the surface electric field perpendicular to the two dimensional plane via adjusting the Rashba coupling.…
We develop the microscopic theory of the extrinsic spin Hall conductivity of a two-dimensional electron gas, including skew-scattering, side-jump, and Coulomb interaction effects. We find that while the spin-Hall conductivity connected with the side-jump is independent of the strength of electron-electron interactions, the skew-scattering term is reduced by the spin-Coulomb drag, so the total spin current and the total spin-Hall conductivity are reduced for typical experimental mobilities. Further, we predict that in paramagnetic systems the spin-Coulomb drag reduces the spin accumulations in …
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…
We have investigated the complex two-dimensional electron system with unequal Rashba and Dresselhaus spin-orbit interactions in the presence of a perpendicular magnetic field. The spin polarizations are obtained in a wide range of magnetic fields. It is shown that such a system is hard to be magnetized. We also find that the resonant charge and spin Hall conductances occurs simultaneously at a certain magnetic field, at which two (nearly) degenerate Landau levels are filled partly. The resonant Hall effects are universal in this type of semiconductor materials, and could have potential applica…
The Kubo formula is used to calculate the spin-Hall conductivity in a spin-polarized two-dimensional electron system with Rashba-type spin-orbit interaction. As in the case of the unpolarized electron system, spin Hall conductivity is entirely determined by states at the Fermi level, a property that persists in the presence of magnetic impurities. In the clean limit, the spin-Hall conductivity decreases monotonically with the Zeeman splitting, a result of the ordering effect on the electron spins produced by the magnetic field. In the presence of magnetic impurities, the spin-dependent scatter…
The mid-infrared (MIR) spectral range is of immense use for civilian and military applications. The large number of vibrational absorption bands in this range can be used for gas sensing, process control and spectroscopy. In addition, there exists transparency windows in the atmosphere such as that between 3.6-3.8 $μ$m, which are ideal for free-space optical communication, range finding and thermal imaging. A number of different semiconductor platforms have been used for MIR light-emission. This includes InAsSb/InAs quantum wells, InSb/AlInSb, GaInAsSbP pentanary alloys, and intersubband trans…
Hall effect is detected in organic field-effect transistors, using appropriately shaped rubrene (C42H28) single crystals. It turned out that inverse Hall coefficient, having a positive sign, is close to the amount of electric-field induced charge upon the hole accumulation. The presence of the normal Hall effect means that the electromagnetic character of the surface charge is not of hopping carriers but resembles that of a two-dimensional hole-gas system.
The spintronic properties of a palladium thin film have been investigated in the presence of hydrogen gas in cobalt/palladium bilayers. Measurements of the inverse spin Hall Effect (ISHE) using cavity ferromagnetic resonance allow estimations of the spin Hall conductivity and spin diffusion length in both nitrogen and hydrogen gas atmospheres. Unwanted spin rectification effects are removed using a simple method of inverting the spin current direction with respect to the measurement setup. Absorption of hydrogen gas in the Pd layer at just 3% concentration results in a reduced ISHE voltage amp…
The anomalous Hall effect in a magnetic two-dimensional electron gas with Rashba spin-orbit coupling is studied within the Kubo-Streda formalism in the presence of pointlike potential impurities. We find that all contributions to the anomalous Hall conductivity vanish to leading order in disorder strength when both chiral subbands are occupied. In the situation that only the majority subband is occupied, all terms are finite in the weak scattering limit and the total anomalous Hall conductivity is dominated by skew scattering. We compare our results to previous treatments and resolve some of t…
We discuss the mechanism of anomalous Hall effect related to the contribution of electron states below the Fermi surface (induced by the Berry phase in momentum space). Our main calculations are made within a model of two-dimensional electron gas with spin-orbit interaction of the Rashba type, taking into account the scattering from impurities. We demonstrate that such an "intrinsic" mechanism can dominate but there is a competition with the impurity-scattering mechanism, related to the contribution of states in the vicinity of Fermi surface. We also show that the contribution to the Hall cond…
Magnetic impurities play an important role in many spintronics-related materials. Motivated by this fact, we study the anomalous Hall effect in the presence of magnetic impurities, focusing on two-dimensional electron systems with Rashba spin-orbit coupling. We find a highly nonlinear dependence on the impurity polarization, including possible sign changes. At small impurity magnetizations, this is a consequence of the remarkable result that the linear term is independent of the spin-orbit coupling strength. Near saturation of the impurity spins, the anomalous Hall conductivity can be resonant…
We present the concept of magnetic gas detection by the Extraordinary Hall effect (EHE). The technique is compatible with the existing conductometric gas detection technologies and allows simultaneous measurement of two independent parameters: resistivity and magnetization affected by the target gas. Feasibility of the approach is demonstrated by detecting low concentration hydrogen using thin CoPd films as the sensor material. The Hall effect sensitivity of the optimized samples exceeds 240% per 104 ppm at hydrogen concentrations below 0.5% in the hydrogen/nitrogen atmosphere, which is more t…
