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Keji Lai

Publications and source records attributed to Keji Lai.

At least 55 records · Page 3Linked to original sources

Tailoring Semiconductor Lateral Multi-junctions for Giant Photoconductivity Enhancement

Semiconductor heterostructures have played a critical role as the enabler for new science and technology. The emergence of transition metal dichalcogenides (TMDs) as atomically thin semiconductors has opened new frontiers in semiconductor heterostructures either by stacking different TMDs to form vertical heterojunctions or by stitching them laterally to form lateral heterojunctions via direct growth. In conventional semiconductor heterostructures, the design of multi-junctions is critical to achieve carrier confinement. Analogously, we report successful synthesis of monolayer WS2/WS2(1-x)Se2x/WS2 multi-junction lateral heterostructure via direct growth by chemical vapor deposition. The grown structures are characterized by Raman, photoluminescence, and annular dark-field scanning transmission electron microscopy to determine its lateral compositional profile. More importantly, using microwave impedance microscopy, we demonstrate that the local photoconductivity in the alloy region can be tailored and enhanced by 2 orders of magnitude over pure WS2. Finite element analysis confirms that this effect is due to the carrier diffusion and confinement into the alloy region. Our work exemplifies the technological potential of atomically thin lateral heterostructures in optoelectronic applications.

cond-mat.mtrl-sci↗

Out-of-plane Piezoelectricity and Ferroelectricity in Layered $α$-In2Se3 Nano-flakes

Piezoelectric and ferroelectric properties in the two dimensional (2D) limit are highly desired for nanoelectronic, electromechanical, and optoelectronic applications. Here we report the first experimental evidence of out-of-plane piezoelectricity and ferroelectricity in van der Waals layered $α$-In2Se3 nano-flakes. The non-centrosymmetric R3m symmetry of the $α$-In2Se3 samples is confirmed by scanning transmission electron microscopy, second-harmonic generation, and Raman spectroscopy measurements. Domains with opposite polarizations are visualized by piezo-response force microscopy. Single-point poling experiments suggest that the polarization is potentially switchable for $α$-In2Se3 nano-flakes with thicknesses down to ~ 10 nm. The piezotronic effect is demonstrated in two-terminal devices, where the Schottky barrier can be modulated by the strain-induced piezopotential. Our work on polar $α$-In2Se3, one of the model 2D piezoelectrics and ferroelectrics with simple crystal structures, shows its great potential in electronic and photonic applications.

cond-mat.mtrl-sci↗

Low-energy Structural Dynamics of Ferroelectric Domain Walls in Hexagonal Rare-earth Manganites

Domain walls (DWs) in ferroic materials, across which the order parameter abruptly changes its orientation, can host emergent properties that are absent in the bulk domains. Using a broadband ($10^6-10^{10}$ Hz) scanning impedance microscope, we show that the electrical response of the interlocked antiphase boundaries and ferroelectric domain walls in hexagonal rare-earth manganites ($h-RMnO_3$) is dominated by the bound-charge oscillation rather than free-carrier conduction at the DWs. As a measure of the rate of energy dissipation, the effective conductivity of DWs on the (001) surfaces of $h-RMnO_3$ at GHz frequencies is drastically higher than that at dc, while the effect is absent on surfaces with in-plane polarized domains. First-principles and model calculations indicate that the frequency range and selection rules are consistent with the periodic sliding of the DW around its equilibrium position. This acoustic-wave-like mode, which is associated with the synchronized oscillation of local polarization and apical oxygen atoms, is localized perpendicular to the DW but free to propagate along the DW plane. Our results break the ground to understand structural DW dynamics and exploit new interfacial phenomena for novel devices.

cond-mat.mes-hall↗

Impact of Grain Boundaries on Efficiency and Stability of Organic-Inorganic Trihalide Perovskites

Organic-inorganic perovskite solar cells have attracted tremendous attention because of their remarkably high power conversion efficiencies (PCEs). To further improve the device performance, however, it is imperative to obtain fundamental understandings on the photo-response and long-term stability down to the microscopic level. Here, we report the first quantitative nanoscale photoconductivity imaging on two methylammonium lead triiodide (MAPbI3) thin films with different PCEs by light-stimulated microwave impedance microscopy. The intrinsic photo-response is largely uniform across grains and grain boundaries, which is direct evidence on the inherently benign nature of microstructures in the perovskite thin films. In contrast, the carrier mobility and lifetime are strongly affected by bulk properties such as the sample crystallinity. As visualized by the spatial evolution of local photoconductivity, the degradation due to water diffusion through the capping layer begins with the disintegration of large grains rather than the nucleation and propagation from grain boundaries. Our findings provide new insights to improve the electro-optical properties of MAPbI3 thin films towards large-scale commercialization.

cond-mat.mtrl-sci↗

Uncovering edge states and electrical inhomogeneity in MoS2 field-effect transistors

The understanding of various types of disorders in atomically thin transition metal dichalcogenides (TMDs), including dangling bonds at the edges, chalcogen deficiencies in the bulk, and charges in the substrate, is of fundamental importance for their applications in electronics and photonics. Because of the imperfections, electrons moving on these two-dimensional (2D) crystals experience a spatially non-uniform Coulomb environment, whose effect on the charge transport has not been microscopically studied. Here, we report the mesoscopic conductance mapping in monolayer and few-layer MoS2 field-effect transistors (FETs) by microwave impedance microscopy (MIM). The spatial evolution of the insulator-to-metal transition is clearly resolved. Interestingly, as the transistors are gradually turned on, electrical conduction emerges initially at the edges before appearing in the bulk of MoS2 flakes, which can be explained by our first-principles calculations. The results unambiguously confirm that the contribution of edge states to the channel conductance is significant under the threshold voltage but negligible once the bulk of the TMD device becomes conductive. Strong conductance inhomogeneity, which is associated with the fluctuations of disorder potential in the 2D sheets, is also observed in the MIM images, providing a guideline for future improvement of the device performance.

cond-mat.mes-hall↗

Direct Imaging of Dynamic Glassy Behavior in a Strained Manganite Film

Complex many-body interaction in perovskite manganites gives rise to a strong competition between ferromagnetic metallic and charge ordered phases with nanoscale electronic inhomogeneity and glassy behaviors. Investigating this glassy state requires high resolution imaging techniques with sufficient sensitivity and stability. Here, we present the results of a near-field microwave microscope imaging on the strain driven glassy state in a manganite film. The high contrast between the two electrically distinct phases allows direct visualization of the phase separation. The low temperature microscopic configurations differ upon cooling with different thermal histories. At sufficiently high temperatures, we observe switching between the two phases in either direction. The dynamic switching, however, stops below the glass transition temperature. Compared with the magnetization data, the phase separation was microscopically frozen, while spin relaxation was found in a short period of time.

cond-mat.mes-hall↗

Thickness-dependent Dielectric Constant of Few-layer In2Se3 Nano-flakes

The dielectric constant or relative permittivity of a dielectric material, which describes how the net electric field in the medium is reduced with respect to the external field, is a parameter of critical importance for charging and screening in electronic devices. Such a fundamental material property is intimately related to not only the polarizability of individual atoms, but also the specific atomic arrangement in the crystal lattice. In this letter, we present both experimental and theoretical investigations on the dielectric constant of few-layer In2Se3 nano-flakes grown on mica substrates by van der Waals epitaxy. A nondestructive microwave impedance microscope is employed to simultaneously quantify the number of layers and local electrical properties. The measured dielectric constant increases monotonically as a function of the thickness and saturates to the bulk value at around 6 ~ 8 quintuple layers. The same trend of layer-dependent dielectric constant is also revealed by first-principle calculations. Our results of the dielectric response, being ubiquitously applicable to layered 2D semiconductors, are expected to be significant for this vibrant research field.

cond-mat.mes-hall↗

Thermal Oxidation of WSe2 Nano-sheets Adhered on SiO2/Si Substrates

Due to the drastically different intralayer versus interlayer bonding strengths, the mechanical, thermal, and electrical properties of two-dimensional (2D) materials are highly anisotropic between the in-plane and out-of-plane directions. The structural anisotropy may also play a role in chemical reactions, such as oxidation, reduction, and etching. Here, the composition, structure, and electrical properties of mechanically exfoliated WSe2 nano- sheets on SiO2/Si substrates were studied as a function of the extent of thermal oxidation. A major component of the oxidation, as indicated from optical and Raman data, starts from the nano-sheet edges and propagates laterally towards the center. Partial oxidation also occurs in certain areas at the surface of the flakes, which are shown to be highly conductive by microwave impedance microscopy. Using secondary ion mass spectroscopy, we also observed extensive oxidation at the WSe2/SiO2 interface. The combination of multiple microcopy methods can thus provide vital information on the spatial evolution of chemical reactions on 2D materials and the nanoscale electrical properties of the reaction products.

cond-mat.mtrl-sci↗

Direct Imaging of Nanoscale Conductance Evolution in Ion-Gel-Gated Oxide Transistors

Electrostatic modification of functional materials by electrolytic gating has demonstrated a remarkably wide range of density modulation, a condition crucial for developing novel electronic phases in systems ranging from complex oxides to layered chalcogenides. Yet little is known microscopically when carriers are modulated in electrolyte-gated electric double-layer transistors (EDLTs) due to the technical challenge of imaging the buried electrolyte-semiconductor interface. Here, we demonstrate the real-space mapping of the channel conductance in ZnO EDLTs using a cryogenic microwave impedance microscope. A spin-coated ionic gel layer with typical thicknesses below 50 nm allows us to perform high resolution (on the order of 100 nm) sub-surface imaging, while maintaining the capability of inducing the metal-insulator transition under a gate bias. The microwave images vividly show the spatial evolution of channel conductance and its local fluctuations through the transition, as well as the uneven conductance distribution established by a large source-drain bias. The unique combination of ultra-thin ion-gel gating and microwave imaging offers a new opportunity to study the local transport and mesoscopic electronic properties in EDLTs.

cond-mat.mes-hall↗

Unexpected edge conduction in HgTe quantum wells under broken time reversal symmetry

The realization of quantum spin Hall (QSH) effect in HgTe quantum wells (QWs) is considered a milestone in the discovery of topological insulators. The QSH edge states are predicted to allow current to flow at the edges of an insulating bulk, as demonstrated in various experiments. A key prediction of QSH theory that remains to be experimentally verified is the breakdown of the edge conduction under broken time reversal symmetry (TRS). Here we first establish a rigorous framework for understanding the magnetic field dependence of electrostatically gated QSH devices. We then report unexpected edge conduction under broken TRS, using a unique cryogenic microwave impedance microscopy (MIM), on a 7.5 nm HgTe QW device with an inverted band structure. At zero magnetic field and low carrier densities, clear edge conduction is observed in the local conductivity profile of this device but not in the 5.5 nm control device whose band structure is trivial. Surprisingly, the edge conduction in the 7.5 nm device persists up to 9 T with little effect from the magnetic field. This indicates physics beyond simple QSH models, possibly associated with material- specific properties, other symmetry protection and/or electron-electron interactions.

cond-mat.mes-hall↗

Toward Air-Stable Multilayer Phosphorene Thin-Films and Transistors

Few-layer black phosphorus (BP), also known as phosphorene, is poised to be the most attractive graphene analogue owing to its high mobility approaching that of graphene, and its thickness- tunable band gap that can be as large as that of molybdenum disulfide. In essence, phosphorene represents the much sought after high-mobility, large direct band gap two-dimensional layered crystal that is ideal for optoelectronics and flexible devices. However, its instability in air is of paramount concern for practical applications. Here, we demonstrate air-stable BP devices with dielectric and hydrophobic encapsulation. Microscopy, spectroscopy, and transport techniques were employed to elucidate the aging mechanism, which can initiate from the BP surface for bare samples, or edges for samples with thin dielectric coating highlighting the ineffectiveness of conventional scaled dielectrics. Our pioneering months-long studies indicate that a double layer of Al2O3 and hydrophobic fluoropolymer affords BP devices and transistors with indefinite air-stability for the first time, overcoming a critical material challenge for applied research and development.

cond-mat.mtrl-sci↗

Mesoscale Imperfections in MoS2 Atomic Layers Grown by Vapor Transport Technique

The success of isolating small flakes of atomically thin layers through mechanical exfoliation has triggered enormous research interest in graphene and other two-dimensional materials. For device applications, however, controlled large-area synthesis of highly crystalline monolayers with a low density of electronically active defects is imperative. Here, we demonstrate the electrical imaging of dendritic ad-layers and grain boundaries in monolayer molybdenum disulfide (MoS2) grown by vapor transport technique using microwave impedance microscopy. The micrometer-sized precipitates in our films, which appear as a second layer of MoS2 in conventional height and optical measurements, show 2 orders of magnitude higher conductivity than that of the single layer. The zigzag grain boundaries, on the other hand, are shown to be more resistive than the crystalline grains, consistent with previous studies. Our ability to map the local electrical properties in a rapid and nondestructive manner is highly desirable for optimizing the growth process of large-scale MoS2 atomic layers.

cond-mat.mtrl-sci↗

Batch-fabricated cantilever probes with electrical shielding for nanoscale dielectric and conductivity imaging

This paper presents the design and fabrication of batch-processed cantilever probes with electrical shielding for scanning microwave impedance microscopy. The diameter of the tip apex, which defines the electrical resolution, is less than 50 nm. The width of the stripline and the thicknesses of the insulation dielectrics are optimized for a small series resistance (< 5 W) and a small background capacitance (~ 1 pF), both critical for high sensitivity imaging on various samples. The coaxial shielding ensures that only the probe tip interacts with the sample. The structure of the cantilever is designed to be symmetric to balance the stresses and thermal expansions of different layers so that the cantilever remains straight under variable temperatures. Such shielded cantilever probes produced in the wafer scale will facilitate enormous applications on nanoscale dielectric and conductivity imaging.

physics.ins-det↗

Imaging of the Coulomb driven quantum Hall edge states

The edges of a two-dimensional electron gas (2DEG) in the quantum Hall effect (QHE) regime are divided into alternating metallic and insulating strips, with their widths determined by the energy gaps of the QHE states and the electrostatic Coulomb interaction. Local probing of these submicrometer features, however, is challenging due to the buried 2DEG structures. Using a newly developed microwave impedance microscope, we demonstrate the real-space conductivity mapping of the edge and bulk states. The sizes, positions, and field dependence of the edge strips around the sample perimeter agree quantitatively with the self-consistent electrostatic picture. The evolution of microwave images as a function of magnetic fields provides rich microscopic information around the ν= 2 QHE state.

cond-mat.mes-hall↗

Ambipolar Field Effect in Topological Insulator Nanoplates of (BixSb1-x)2Te3

Topological insulators represent a new state of quantum matter attractive to both fundamental physics and technological applications such as spintronics and quantum information processing. In a topological insulator, the bulk energy gap is traversed by spin-momentum locked surface states forming an odd number of surface bands that possesses unique electronic properties. However, transport measurements have often been dominated by residual bulk carriers from crystal defects or environmental doping which mask the topological surface contribution. Here we demonstrate (BixSb1-x)2Te3 as a tunable topological insulator system to manipulate bulk conductivity by varying the Bi/Sb composition ratio. (BixSb1-x)2Te3 ternary compounds are confirmed as topological insulators for the entire composition range by angle resolved photoemission spectroscopy (ARPES) measurements and ab initio calculations. Additionally, we observe a clear ambipolar gating effect similar to that observed in graphene using nanoplates of (BixSb1-x)2Te3 in field-effect-transistor (FET) devices. The manipulation of carrier type and concentration in topological insulator nanostructures demonstrated in this study paves the way for implementation of topological insulators in nanoelectronics and spintronics.

cond-mat.str-el↗

Cryogenic Microwave Imaging of Metal-Insulator Transition in Doped Silicon

We report the instrumentation and experimental results of a cryogenic scanning microwave impedance microscope. The microwave probe and the scanning stage are located inside the variable temperature insert of a helium cryostat. Microwave signals in the distance modulation mode are used for monitoring the tip-sample distance and adjusting the phase of the two output channels. The ability to spatially resolve the metal-insulator transition in a doped silicon sample is demonstrated. The data agree with a semi-quantitative finite-element simulation. Effects of the thermal energy and electric fields on local charge carriers can be seen in the images taken at different temperatures and DC biases.

cond-mat.mes-hall↗

Rapid Surface Oxidation as a Source of Surface Degradation Factor for Bi2Se3

Bi2Se3 is a topological insulator with metallic surface states residing in a large bulk bandgap. It is believed that Bi2Se3 gets additional n-type doping after exposure to atmosphere, thereby reducing the relative contribution of surface states in total conductivity. In this letter, transport measurements on Bi2Se3 nanoribbons provide additional evidence of such environmental doping process. Systematic surface composition analyses by X-ray photoelectron spectroscopy reveal fast formation and continuous growth of native oxide on Bi2Se3 under ambient conditions. In addition to n-type doping at the surface, such surface oxidation is likely the material origin of the degradation of topological surface states. Appropriate surface passivation or encapsulation may be required to probe topological surface states of Bi2Se3 by transport measurements.

cond-mat.mtrl-sci↗

Microwave imaging of mesoscopic percolating network in a manganite thin film

Many unusual behaviors in complex oxides are deeply associated with the spontaneous emergence of microscopic phase separation. Depending on the underlying mechanism, the competing phases can form ordered or random patterns at vastly different length scales. Using a microwave impedance microscope, we observed an orientation-ordered percolating network in strained Nd0.5Sr0.5MnO3 thin films with a large period of 100 nm. The filamentary metallic domains align preferentially along certain crystal axes of the substrate, suggesting the anisotropic elastic strain as the key interaction in this system. The local impedance maps provide microscopic electrical information of the hysteretic behavior in strained thin film manganites, suggesting close connection between the glassy order and the colossal magnetoresistance effects at low temperatures.

cond-mat.mes-hall↗