We use electron transport to characterize monolayer graphene - multilayer MoS2 heterostructures. Our samples show ambipolar characteristics and conductivity saturation on the electron branch which signals the onset of MoS2 conduction band population. Surprisingly, the carrier density in graphene decreases with gate bias once MoS2 is populated, demonstrating negative compressibility in MoS2. We are able to interpret our measurements quantitatively by accounting for disorder and using the random phase approximation (RPA) for the exchange and correlation energies of both Dirac and parabolic-band two-dimensional electron gases. This interpretation allows us to extract the energetic offset between the conduction band edge of MoS2 and the Dirac point of graphene.
Negative compressibility generated by many-body effects in 2D electronic systems can enhance gate capacitance. We observe capacitance enhancement in a newly emerged 2D layered material, atomically thin black phosphorus (BP). The encapsulation of BP by hexagonal boron nitride sheets with few-layer graphene as a terminal ensures ultraclean heterostructure interfaces, allowing us to observe negative compressibility at low hole carrier concentrations. We explained the negative compressibility based on the Coulomb correlation among in-plane charges and their image charges in a gate electrode in the…
A series of (Ga,In)As/GaAs/Ga(As,Sb) multi-quantum well heterostructures is analyzed using temperature- and power-dependent photoluminescence (PL) spectroscopy. Pronounced PL variations with sample temperature are observed and analyzed using microscopic many-body theory and band structure calculations based on the k$\cdot$p method. This theory-experiment comparison reveals an unusual, temperature dependent variation of the band alignment between the (Ga,In)As and Ga(As,Sb) quantum wells.
Oxide heterostructures with polar films display special electronic properties, such as the electronic reconstruction at their internal interfaces with the formation of two-dimensional metallic states. Moreover, the electrical field from the polar layers is inversion-symmetry breaking and generates a Rashba spin-orbit coupling (RSOC) in the interfacial electronic system. We investigate the quantum capacitance of a heterostructure in which a sizeable RSOC at a metallic interface is controlled by the electric field of a surface electrode. Such a structure is, for example, given by a LaAlO_3 film …
Utilizing three-terminal tunnel emission of ballistic electrons and holes, we have developed a method to self-consistently measure the bandgap of semiconductors and band discontinuities at semiconductor heterojunctions without any prerequisite material parameter. Measurements are performed on lattice-matched GaAs/AlxGa1-xAs and GaAs/(AlxGa1-x)0.51In0.49P single-barrier heterostructures. The bandgaps of AlGaAs and AlGaInP are measured with a resolution of several meV at 4.2 K. For the GaAs/AlGaAs interface, the measured Gamma band offset ratio is 60.4:39.6 (+/-2%). For the GaAs/AlGaInP interfac…
Epitaxially-grown semiconductor heterostructures give the possibility to tailor the potential landscape for the carriers in a very controlled way. In planar lattice-matched heterostructures, the potential has indeed a very simple and easily predictable behavior: it is constant everywhere except at the interfaces where there is a step (discontinuity) which only depends on the composition of the semiconductors in contact. In this paper, we show that this universally accepted picture can be invalid in nanoscale heterostructures (e.g., quantum dots, rods, nanowires) which can be presently fabricat…
Anharmonicity of the inter-atomic potential is taken into account for the quantitative simulation of the conduction and valence band offsets for highly-strained semiconductor heterostructures. The anharmonicity leads to a weaker compressive hydrostatic strain than that obtained with the commonly used quasi-harmonic approximation of the Keating model. Inclusion of the anharmonicity in the simulation of strained InAs/GaAs nanostructures results in an improvement of the electron band offset computed on an atomistic level by up to 100 meV compared to experiment.
The interface between topological and normal insulators hosts metallic states that appear due to the change in band topology. While these topological states at a surface, i.e., a topological insulator-air/vacuum interface, have been studied intensely, topological states at a solid-solid interface have been less explored. Here we combine experiment and theory to study such \textit{embedded} topological states (ETSs) in heterostructures of GeTe (normal insulator) and Sb$_2$Te$_3$ (topological insulator). We analyse their dependence on the interface and their confinement characteristics. To chara…
The emergence of transition metal dichalcogenides (TMDs) as 2D electronic materials has stimulated proposals of novel electronic and photonic devices based on TMD heterostructures. Here we report the determination of band offsets in TMD heterostructures by using microbeam X-ray photoelectron spectroscopy (μ-XPS) and scanning tunneling microscopy/spectroscopy (STM/S). We determine a type-II alignment between $\textrm{MoS}_2$ and $\textrm{WSe}_2$ with a valence band offset (VBO) value of 0.83 eV and a conduction band offset (CBO) of 0.76 eV. First-principles calculations show that in this hetero…
We performed density functional theory calculations on heterostructures of single layers of hexagonal BN and MoS$_2$ to assess the effect of doping in the BN sheet and of interstitial Na atoms on the electronic properties of the adjacent MoS$_2$ layer. Our calculations predict that $n$-doping of the boron nitride subsystem by oxygen, carbon and sulfur impurities causes noticeable charge transfer into the conduction band of the MoS$_2$ sheet, while $p$-doping by beryllium and carbon leaves the molybdenum disulphide layer largely unaffected. Intercalated sodium atoms lead to a significant increa…
Semiconductor coupled quantum dots provide a unique opportunity of tuning bandgaps by tailoring band offsets, making them ideal for photovoltaic and other applications. Here, we have studied stability, trends in the band gap, band offsets, and optical properties for a series of coupled quantum dots comprised of II-VI semiconductor using a hybrid functional method. We have shown how the quantum confinement and interfacial strain considerably affect the band gap and band offsets for these heterostructures at the nanoscale. We show that the trend in band offsets obtained from our first-principles…
The spin Hall effect in a heavy metal thin film allows to probe the magnetic properties of an adjacent magnetic insulator via magnetotransport measurements. Here, we investigate the magnetoresistive response of yttrium iron garnet/platinum heterostructures from room temperature to beyond the Curie temperature $T_\mathrm{C, YIG} \approx 560\,\mathrm{K}$ of the ferrimagnetic insulator. We find that the amplitude of the (local) spin Hall magnetoresistance decreases monotonically from $300\,\mathrm{K}$ towards $T_\mathrm{C}$, mimicking the evolution of the saturation magnetization of yttrium iron …
Two-dimensional heterostructure of WSe2/MoS2 atomic layers has unique piezoelectric characteristics which depends on the number of atomic layer, stacking type, and interlayer interaction size. The van der Waals heterostructure of p- and n-type TMDC atomic layers with different work functions forms a staggered gap alignment. The large band offset of conduction band minimum and valence band maximum between p-type WSe2 and n-type MoS2 atomic layers leads to the large electric polarization and piezoelectricity. The output voltages for a MoS2/WSe2 partial vertical heterostructure with a size of 3.0…
The electronic structure of bulk fcc GaAs, fcc and tetragonal CrAs, and CrAs/GaAs supercells, computed within LMTO local spin-density functional theory, is used to extract the band alignment (band offset) for the [1,0,0] GaAs/CrAs interface in dependence of the spin orientation. With the lateral lattice constant fixed to the experimental bulk GaAs value, a local energy minimum is found for a tetragonal CrAs unit cell with a slightly ($\approx$ 2%) reduced longitudinal ([1,0,0]) lattice constant. Due to the identified spin-dependent band alignment, half-metallicity of CrAs no longer is a key re…
We have studied the effects of Mn concentration on the ballistic spin-polarized transport through diluted magnetic semiconductor heterostructures with a single paramagnetic layer. Using a fitted function for zero-field conduction band offset based on the experimental data, we found that the spin current densities strongly depend on the Mn concentration. The magnitude as well as the sign of the electron-spin polarization and the tunnel magnetoresistance can be tuned by varying the Mn concentration, the width of the paramagnetic layer, and the external magnetic field. By an appropriate choice of…
The application of ultrathin two-dimensional (2D) perovskites in near-infrared and visible-range optoelectronics has been limited owing to their inherent wide bandgaps, large excitonic binding energies and low optical absorption at higher wavelengths. Here, we show that by tailoring interfacial band alignments via conjugation with low-dimensional materials like monolayer transition metal dichalcogenides (TMD), the functionalities of 2D perovskites can be extended to diverse, visible-range photophysical applications. Based on the choice of individual constituents in the 2D perovskite/TMD hetero…
We have calculated electronic and optical properties of Si/BeSe$_{0.41}$Te$_{0.59}$ heterostructures by a semiempirical $sp^{3}s^{*}$ tight-binding method. Tight-binding parameters and band bowing of BeSe$_{0.41}$Te$_{0.59}$ are considered through a recent model for highly mismatched semiconductor alloys. The band bowing and the measurements of conduction band offset lead to a type II heterostucture for Si/BeSe$_{0.41}$Te$_{0.59}$ with conduction band minimum in the Si layer and valence band maximum in the BeSe$_{0.41}$Te$_{0.59}$ layer. The electronic structure and optical properties of vario…
A novel method for the direct correlation at the nanoscale of structural and optical properties of single GaAs nanowires is reported. Nanowires consisting of 100% wurtzite and nanowires presenting zinc-blende/wurtzite polytypism are investigated by photoluminescence spectroscopy and transmission electron microscopy. The photoluminescence of wurtzite GaAs is consistent with a band gap of 1.5 eV. In the polytypic nanowires, it is shown that the regions that are predominantly composed of either zinc-blende or wurtzite phase show photoluminescence emission close to the bulk GaAs band gap, while re…
Combining monolayers of different two-dimensional (2D) semiconductors into heterostructures opens up a wealth of possibilities for novel electronic and optical functionalities. Exploiting them hinges on accurate measurements of the band parameters and orbital hybridization in separate and stacked monolayers, many of which are only available as small samples. The recently introduced technique of angle-resolved photoemission spectroscopy with submicron spatial resolution (μ-ARPES) offers the capability to measure small samples, but the energy resolution obtained for such exfoliated samples to da…
Bilayer graphene has a unique electronic structure influenced by a complex interplay between various degrees of freedom. We probe its chemical potential using double bilayer graphene heterostructures, separated by a hexagonal boron nitride dielectric. The chemical potential has a non-linear carrier density dependence, and bears signatures of electron-electron interactions. The data allow a direct measurement of the electric field-induced bandgap at zero magnetic field, the orbital Landau level (LLs) energies, and the broken symmetry quantum Hall state gaps at high magnetic fields. We observe s…
The evolution of transverse-momentum-dependent effective band offset ($V_{\mathrm{eff}}$) profile for heavy (\emph{hh})- and light-holes (\emph{lh}), is detailed studied. Several new features in the metamorphosis of the standardized fixed-height $V_{\mathrm{eff}}$ profile for holes, in the presence of gradually increasing valence-band mixing and pseudomorphic strain, are presented. In some $III-V$ unstrained semiconducting layered heterostructures a fixed-height potential, is not longer valid for \emph{lh}. Indeed, we found ---as predicted for electrons---, permutations of the $V_{\mathrm{eff}…
Composition and Surface Termination Control Band Alignments in P3HT/Perovskite Heterostructures
Faculty of Engineering and Natural Sciences, Sabanci University（萨班哲大学工程与自然科学学院）；Materials Science and Nano Engineering Program, Sabanci University（萨班哲大学材料科学与纳米工程项目）
Ferromagnetism is most common in transition metal compounds but may also arise in low-density two-dimensional electron systems, with signatures observed in silicon, III-V semiconductor systems, and graphene moiré heterostructures. Here we show that gate-tuned van Hove singularities in rhombohedral trilayer graphene drive the spontaneous ferromagnetic polarization of the electron system into one or more spin- and valley flavors. Using capacitance measurements on graphite-gated van der Waals heterostructures, we find a cascade of density- and electronic displacement field tuned phase transitions…
Atomically transparent vertically aligned ZnO-based van der Waals material have been developed by surface passivation and encapsulation with atomic layers of MgO using materials by design; the physical properties investigated. The passivation and encapsulation led to a remarkable improvement in optical and electronic properties. The valence-band offset $ΔE_v$ between MgO and ZnO, ZnO and MgO/ZnO, and ZnO and MgO/ZnO/MgO heterointerfaces are determined to be 0.37 $\pm$0.02, -0.05$\pm$0.02, and -0.11$\pm$0.02 eV, respectively; the conduction-band offset $ΔE_c$ is deduced to be 0.97$\pm$0.02, 0.4…
Electrons in quantum materials exhibiting coexistence of dispersionless (flat) bands piercing dispersive (steep) bands can give rise to strongly correlated phenomena, and are associated with unconventional superconductivity. It is known that in twisted trilayer graphene steep Dirac cones can coexist with band flattening, but the phenomenon is not stable under layer misalignments. Here we show that such a twisted sandwiched graphene (TSWG) -- a three-layer van der Waals heterostructure with a twisted middle layer -- can have very stable flat bands coexisting with Dirac cones near the Fermi ener…
We present a detailed study of the electronic and spin-orbit properties of single and bilayer graphene in proximity to the topological insulator Bi$_2$Se$_3$. Our approach is based on first-principles calculations, combined with symmetry derived model Hamiltonians that capture the low-energy band properties. We consider single and bilayer graphene on 1--3 quintuple layers of Bi$_2$Se$_3$ and extract orbital and proximity induced spin-orbit coupling (SOC) parameters. We find that graphene gets significantly hole doped (350 meV), but the linear dispersion is preserved. The proximity induced SOC …
Van der Waals heterostuctures, made from stacks of two-dimensional materials, exhibit unique light-matter interactions and are promising for novel optoelectronic devices. The performance of such devices is governed by near-field coupling through, e.g., interlayer charge and/or energy transfer. New concepts and experimental methodologies are needed to properly describe two-dimensional heterointerfaces. Here, we report on interlayer charge and energy transfer in atomically thin metal (graphene)/semiconductor (transition metal dichalcogenide (TMD, here MoSe$_2$)) heterostructures using a combinat…
The ability to create high-quality lateral p-n junctions at nanometer length scales is essential for the next generation of two-dimensional (2D) electronic and plasmonic devices. Using a charge-transfer heterostructure consisting of graphene on $α$-RuCl$_3$, we conduct a proof-of-concept study demonstrating the existence of intrinsic nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multi-pronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy ($\textit{s}$-SNOM) …
We have studied the electronic structure of CdS/ZnSe coupled quantum dot, a novel heterostructure at the nano-scale. Our calculations reveal CdS/ZnSe coupled quantum dots to be of type-II in nature where the anion-p states play an important role in deciding the band offset for the highest occupied molecular orbitals (HOMO). We show that the offsets of HOMO as well as the lowest unoccupied molecular orbitals (LUMO) can be tuned by changing the sizes of the components of the coupled quantum dot, thereby providing an additional control parameter to tune the band gap and the optical properties. Ou…
Group-IV monochalcogenides are emerging as a new class of layered materials beyond graphene, transition metal dichalcogenides (TMDCs), and black phosphorus (BP). In this paper, we report experimental and theoretical investigations of the band structure and transport properties of GeSe and its heterostructures. We find that GeSe exhibits a markedly anisotropic electronic transport, with maximum conductance along the armchair direction. Density functional theory calculations reveal that the effective mass is 2.7 times larger along the zigzag direction than the armchair direction; this mass aniso…
Spin orbit coupling (SOC) is the key to realizing time-reversal invariant topological phases of matter. Famously, SOC was predicted by Kane and Mele to stabilize a quantum spin Hall insulator; however, the weak intrinsic SOC in monolayer graphene has precluded experimental observation. Here, we exploit a layer-selective proximity effect---achieved via van der Waals contact to a semiconducting transition metal dichalcogenide--to engineer Kane-Mele SOC in ultra-clean \textit{bilayer} graphene. Using high-resolution capacitance measurements to probe the bulk electronic compressibility, we find th…
