Junmo Kang

Investigation of Band-Offsets at Monolayer–Multilayer MoS2 Junctions by Scanning Photocurrent Microscopy

The thickness-dependent band structure of MoS2 implies that discontinuities in energy bands exist at the interface of monolayer (1L) and multilayer (ML) thin films. The characteristics of such heterojunctions are analyzed here using current versus voltage measurements, scanning photocurrent microscopy, and finite element simulations of charge carrier transport. Rectifying I-V curves are consistently observed between contacts on opposite sides of 1L/ML junctions, and a strong bias-dependent photocurrent is observed at the junction. Finite element device simulations with varying carrier concentrations and electron affinities show that a type II band alignment at single layer/multilayer junctions reproduces both the rectifying electrical characteristics and the photocurrent response under bias. However, the zero-bias junction photocurrent and its energy dependence are not explained by conventional photovoltaic and photothermoelectric mechanisms, indicating the contributions of hot carriers.

Probing Out-of-Plane Charge Transport in Black Phosphorus with Graphene-Contacted Vertical Field-Effect Transistors

Black phosphorus (BP) has recently emerged as a promising narrow band gap layered semiconductor with optoelectronic properties that bridge the gap between semimetallic graphene and wide band gap transition metal dichalcogenides such as MoS2. To date, BP field-effect transistors have utilized a lateral geometry with in-plane transport dominating device characteristics. In contrast, we present here a vertical field-effect transistor geometry based on a graphene/BP van der Waals heterostructure. The resulting device characteristics include high on-state current densities (>1600 A/cm(2)) and current on/off ratios exceeding 800 at low temperature. Two distinct charge transport mechanisms are identified, which are dominant for different regimes of temperature and gate voltage. In particular, the Schottky barrier between graphene and BP determines charge transport at high temperatures and positive gate voltages, whereas tunneling dominates at low temperatures and negative gate voltages. These results elucidate out-of-plane electronic transport in BP and thus have implications for the design and operation of BP-based van der Waals heterostructures.

Low-Voltage Complementary Electronics from Ion-Gel-Gated Vertical Van der Waals Heterostructures

Low-voltage complementary circuits comprising n-type and p-type van der Waals heterojunction vertical field-effect transistors (VFETs) are demonstrated. The resulting VFETs possess high on-state current densities (>3000 A cm(-2) ) and on/off current ratios (>10(4) ) in a narrow voltage window (<3 V).

Solution-Processed Dielectrics Based on Thickness-Sorted Two-Dimensional Hexagonal Boron Nitride Nanosheets

Gate dielectrics directly affect the mobility, hysteresis, power consumption, and other critical device metrics in high-performance nanoelectronics. With atomically flat and dangling bond-free surfaces, hexagonal boron nitride (h-BN) has emerged as an ideal dielectric for graphene and related two-dimensional semiconductors. While high-quality, atomically thin h-BN has been realized via micromechanical cleavage and chemical vapor deposition, existing liquid exfoliation methods lack sufficient control over h-BN thickness and large-area film quality, thus limiting its use in solution-processed electronics. Here, we employ isopycnic density gradient ultracentrifugation for the preparation of monodisperse, thickness-sorted h-BN inks, which are subsequently layer-by-layer assembled into ultrathin dielectrics with low leakage currents of 3 × 10(-9) A/cm(2) at 2 MV/cm and high capacitances of 245 nF/cm(2). The resulting solution-processed h-BN dielectric films enable the fabrication of graphene field-effect transistors with negligible hysteresis and high mobilities up to 7100 cm(2) V(-1) s(-1) at room temperature. These h-BN inks can also be used as coatings on conventional dielectrics to minimize the effects of underlying traps, resulting in improvements in overall device performance. Overall, this approach for producing and assembling h-BN dielectric inks holds significant promise for translating the superlative performance of two-dimensional heterostructure devices to large-area, solution-processed nanoelectronics.

Self-Aligned van der Waals Heterojunction Diodes and Transistors

A general self-aligned fabrication scheme is reported here for a diverse class of electronic devices based on van der Waals materials and heterojunctions. In particular, self-alignment enables the fabrication of source-gated transistors in monolayer MoS2 with near-ideal current saturation characteristics and channel lengths down to 135 nm. Furthermore, self-alignment of van der Waals p-n heterojunction diodes achieves complete electrostatic control of both the p-type and n-type constituent semiconductors in a dual-gated geometry, resulting in gate-tunable mean and variance of antiambipolar Gaussian characteristics. Through finite-element device simulations, the operating principles of source-gated transistors and dual-gated antiambipolar devices are elucidated, thus providing design rules for additional devices that employ self-aligned geometries. For example, the versatility of this scheme is demonstrated via contact-doped MoS2 homojunction diodes and mixed-dimensional heterojunctions based on organic semiconductors. The scalability of this approach is also shown by fabricating self-aligned short-channel transistors with subdiffraction channel lengths in the range of 150-800 nm using photolithography on large-area MoS2 films grown by chemical vapor deposition. Overall, this self-aligned fabrication method represents an important step toward the scalable integration of van der Waals heterojunction devices into more sophisticated circuits and systems.

Inorganic “Conductive Glass” Approach to Rendering Mesoporous Metal–Organic Frameworks Electronically Conductive and Chemically Responsive

A representative mesoporous metal-organic-framework (MOF) material, NU-1000, has been rendered electronically conductive via a robust inorganic approach that permits retention of MOF crystallinity and porosity. The approach is based on condensed-phase grafting of molecular tin species onto the MOF nodes via irreversible reaction with hydroxyl and aqua ligands presented at the node surface, a self-limiting process termed solvothermal installation (of metal ions) in MOFs (SIM, a solution-phase analog of atomic layer deposition in MOFs). Treatment of the modified MOF with aerated steam at 120 °C converts the grafted tin molecules to tetratin(IV)oxy clusters, with the clusters being sited between insulating pairs of zirconia-like nodes (the zirconium component being key to endowing the parent material with requisite chemical and thermal stability). By introducing new O-H presenting ligands on the modified-MOF node, the high-temperature steam step additionally serves to reset the material to reactive form, thus enabling a second self-limiting tin-grafting step to be run (and after further steam treatment, enabling a third). Difference-envelop-density (DED) analyses of synchrotron-derived X-ray scattering data, with and without installed tin species, show that the clusters formed after one cycle are spatially isolated, but that repetitive SIM cycling adds metal and oxygen ions in a way that enshrouds nodes, links clusters, and yields continuous one-dimensional strands of oxy-tin(IV), oriented exclusively along the c axis of the MOF. Two-probe conductivity measurements show that the parent MOF and the version containing isolated oxy-tin(IV) clusters are electrically insulating, but that the versions featuring continuous strands show an electrical conductivity of 1.8 × 10-7 S/cm after three Sn-SIM cycles. When combined with interdigitated microelectrodes, the solvent-free and conductive-glass-modified material (three Sn-SIM cycles) displays a substantial and persistent increase in electrical conductivity during exposure to 5% H2, indicating a role for dissociated H2 as an electronic dopant. The increase can be repetitively reversed by alternating H2 with air, illustrating the ability of the conductive MOF to function as a resistive sensor for H2 and suggesting further potential applications that may capitalize on the combination of high volumetric surface area, high mesoporosity, high chemical and thermal stability, and significant electrical conductivity.

A hybrid silicon-phosphorene nanolaser

We show evidence of lasing from a hybrid nanostructure composed of a silicon optical resonator and a two-dimensional phosphorene film. The ~1555 nm emission wavelength opens possibilities for optically-active devices for integrated silicon photonics.