A quantum ruler for orbital magnetism in moiré quantum matter.

For almost a century, magnetic oscillations have been a powerful "quantum ruler" for measuring Fermi surface topology. In this study, we used Landau-level spectroscopy to unravel the energy-resolved valley-contrasting orbital magnetism and large orbital magnetic susceptibility that contribute to the energies of Landau levels of twisted double-bilayer graphene. These orbital magnetism effects led to substantial deviations from the standard Onsager relation, which manifested as a breakdown in scaling of Landau-level orbits. These substantial magnetic responses emerged from the nontrivial quantum geometry of the electronic structure and the large length scale of the moiré lattice potential. Going beyond traditional measurements, Landau-level spectroscopy performed with a scanning tunneling microscope offers a complete quantum ruler that resolves the full energy dependence of orbital magnetic properties in moiré quantum matter.

Photocatalytic Activity of Ti-SBA-15/C3N4 for Degradation of 2,4-Dichlorophenoxyacetic Acid in Water under Visible Light.

In the present study, the photocatalytic activity of Ti-SBA-15/C3N4 catalysts was investigated to degrade 2,4-Dichlorophenoxyacetic acid (2,4-D) herbicides in water under visible light irradiation. The catalysts were synthesized via a simple hydrothermal method and characterized by various analytical techniques, including SAXS, N2 adsorption-desorption isotherms, Zeta potential, PL, FT-IR, XRF, TGA, and UV-DRS. Our study indicated that the 2.5Ti-SBA-15/C3N4 had higher efficiency in the degradation of 2,4-D than Ti-SBA-15 and C3N4. The decomposition of 2,4-D reached 60% under 180 minutes of visible light irradiation at room temperature on 2.5Ti-SBA-15/C3N4. Moreover, the degradation of 2,4-D on Ti-SBA-15/C3N4 was pseudo-first-order kinetics with the highest rate constant (0.00484 min-1), which was much higher than that obtained for other photocatalysts reported recently. Furthermore, the catalyst can be reused at least two times for photodegradation of 2,4-D solution under visible light irradiation within a slight decrease in catalytic activity.

Are 2D Interfaces Really Flat?

Two-dimensional (2D) van der Waals materials are subject to mechanical deformation and thus forming bubbles and wrinkles during exfoliation and transfer. A lack of interfacial "flatness" has implications for interface properties, such as those formed by metal contacts or insulating layers. Therefore, an understanding of the detailed properties of 2D interfaces, especially their flatness under different conditions, is of high importance. Here we use cross-sectional scanning transmission electron microscopy (STEM) to investigate various 2D interfaces (2D-2D and 3D-2D) under the effects of stacking, atomic layer deposition (ALD), and metallization. We characterize and compare the flatness of the hBN-2D and metal-2D interfaces down to angstrom resolution. It is observed that the dry transfer of hexagonal boron nitride (hBN) can dramatically alter the interface structure. When characterizing 3D metal-2D interfaces, we find that Ni-MoS2 interfaces are more uneven and have larger nanocavities compared to other metal-2D interfaces. The electrical characteristics of a MoS2-based field-effect transistor are correlated to the interfacial transformation in the contact and channel regions. The device transconductance is improved by 40% after the hBN encapsulation, likely due to the interface interactions at both the channel and contacts. Overall, these observations reveal the intricacy of 2D interfaces and their dependence on the fabrication processes.

Edge channels of broken-symmetry quantum Hall states in graphene visualized by atomic force microscopy.

The quantum Hall (QH) effect, a topologically non-trivial quantum phase, expanded the concept of topological order in physics bringing into focus the intimate relation between the "bulk" topology and the edge states. The QH effect in graphene is distinguished by its four-fold degenerate zero energy Landau level (zLL), where the symmetry is broken by electron interactions on top of lattice-scale potentials. However, the broken-symmetry edge states have eluded spatial measurements. In this article, we spatially map the quantum Hall broken-symmetry edge states comprising the graphene zLL at integer filling factors of [Formula: see text] across the quantum Hall edge boundary using high-resolution atomic force microscopy (AFM) and show a gapped ground state proceeding from the bulk through to the QH edge boundary. Measurements of the chemical potential resolve the energies of the four-fold degenerate zLL as a function of magnetic field and show the interplay of the moiré superlattice potential of the graphene/boron nitride system and spin/valley symmetry-breaking effects in large magnetic fields.

Optimal field-effect transistor operation for high-resolution biochemical measurements.

Field-effect transistors (FETs) are powerful tools for sensitive measurements of numerous biomarkers (e.g., proteins, nucleic acids, and antigen) and gaseous species. Most research studies in this field focused on building discrete devices with high performance. We show that instrumentation that is commonly used in multiple areas of physics and engineering can greatly improve the performance of measurement systems that embed FET-based transducers for biological applications. We review the state-of-the-art instrumentation in the field as applied to sensing with FETs. We show how high-performance dual-gate 2D FETs that we recently developed, when operated using closed-loop proportional-integral-derivative control, can drastically improve both the sensitivity and resolution. We further show that this closed-loop control approach can be extended to commonly used single-gate silicon FETs. The generalizability of the results will allow their application to virtually any previously developed FET-based sensor. Finally, we provide insight into further optimization and performance benefits that can be extracted by using the closed-loop feedback approach for applications in biosensing.

Substrate-mediated hyperbolic phonon polaritons in MoO3.

Hyperbolic phonon polaritons (HPhPs) are hybrid excitations of light and coherent lattice vibrations that exist in strongly optically anisotropic media, including two-dimensional materials (e.g., MoO3). These polaritons propagate through the material's volume with long lifetimes, enabling novel mid-infrared nanophotonic applications by compressing light to sub-diffractional dimensions. Here, the dispersion relations and HPhP lifetimes (up to ≈12 ps) in single-crystalline α-MoO3 are determined by Fourier analysis of real-space, nanoscale-resolution polariton images obtained with the photothermal induced resonance (PTIR) technique. Measurements of MoO3 crystals deposited on periodic gratings show longer HPhPs propagation lengths and lifetimes (≈2×), and lower optical compressions, in suspended regions compared with regions in direct contact with the substrate. Additionally, PTIR data reveal MoO3 subsurface defects, which have a negligible effect on HPhP propagation, as well as polymeric contaminants localized under parts of the MoO3 crystals, which are derived from sample preparation. This work highlights the ability to engineer substrate-defined nanophotonic structures from layered anisotropic materials.

Achieving µeV tunneling resolution in an in-operando scanning tunneling microscopy, atomic force microscopy, and magnetotransport system for quantum materials research.

Research in new quantum materials requires multi-mode measurements spanning length scales, correlations of atomic-scale variables with a macroscopic function, and spectroscopic energy resolution obtainable only at millikelvin temperatures, typically in a dilution refrigerator. In this article, we describe a multi-mode instrument achieving a µeV tunneling resolution with in-operando measurement capabilities of scanning tunneling microscopy, atomic force microscopy, and magnetotransport inside a dilution refrigerator operating at 10 mK. We describe the system in detail including a new scanning probe microscope module design and sample and tip transport systems, along with wiring, radio-frequency filtering, and electronics. Extensive benchmarking measurements were performed using superconductor-insulator-superconductor tunnel junctions, with Josephson tunneling as a noise metering detector. After extensive testing and optimization, we have achieved less than 8 µeV instrument resolving capability for tunneling spectroscopy, which is 5-10 times better than previous instrument reports and comparable to the quantum and thermal limits set by the operating temperature at 10 mK.

Rapid, quantitative therapeutic screening for Alzheimer's enzymes enabled by optimal signal transduction with transistors.

We show that commercially sourced n-channel silicon field-effect transistors (nFETs) operating above their threshold voltage with closed loop feedback to maintain a constant channel current allow a pH readout resolution of (7.2 ± 0.3) × 10-3 at a bandwidth of 10 Hz, or ≈3-fold better than the open loop operation commonly employed by integrated ion-sensitive field-effect transistors (ISFETs). We leveraged the improved nFET performance to measure the change in solution pH arising from the activity of a pathological form of the kinase Cdk5, an enzyme implicated in Alzheimer's disease, and showed quantitative agreement with previous measurements. The improved pH resolution was realized while the devices were operated in a remote sensing configuration with the pH sensing element off-chip and connected electrically to the FET gate terminal. We compared these results with those measured by using a custom-built dual-gate 2D field-effect transistor (dg2DFET) fabricated with 2D semi-conducting MoS2 channels and a signal amplification of 8. Under identical solution conditions the nFET performance approached the dg2DFETs pH resolution of (3.9 ± 0.7) × 10-3. Finally, using the nFETs, we demonstrated the effectiveness of a custom polypeptide, p5, as a therapeutic agent in restoring the function of Cdk5. We expect that the straight-forward modifications to commercially sourced nFETs demonstrated here will lower the barrier to widespread adoption of these remote-gate devices and enable sensitive bioanalytical measurements for high throughput screening in drug discovery and precision medicine applications.

Quantum capacitance-limited MoS2 biosensors enable remote label-free enzyme measurements.

We have demonstrated atomically thin, quantum capacitance-limited, field-effect transistors (FETs) that enable the detection of pH changes with 75-fold higher sensitivity (≈4.4 V per pH) over the Nernst value of 59 mV per pH at room temperature when used as a biosensor. The transistors, which are fabricated from monolayer films of MoS2, use a room temperature ionic liquid (RTIL) in place of a conventional oxide gate dielectric and exhibit very low intrinsic noise resulting in a pH resolution of 92 × 10-6 at 10 Hz. This high device performance, which is a function of the structure of our device, is achieved by remotely connecting the gate to a pH sensing element allowing the FETs to be reused. Because pH measurements are fundamentally important in biotechnology, the increased resolution demonstrated here will benefit numerous applications ranging from pharmaceutical manufacturing to clinical diagnostics. As an example, we experimentally quantified the function of the kinase Cdk5, an enzyme implicated in Alzheimer's disease, at concentrations that are 5-fold lower than physiological values, and with sufficient time-resolution to allow the estimation of both steady-state and kinetic parameters in a single experiment. The high sensitivity, increased resolution, and fast turnaround time of the measurements will allow the development of early diagnostic tools and novel therapeutics to detect and treat neurological conditions years before currently possible.

Reproducible Performance Improvements to Monolayer MoS2 Transistors through Exposed Material Forming Gas Annealing.

Metal-mediated exfoliation has been demonstrated as a promising approach for obtaining large-area flakes of two-dimensional (2D) materials to fabricate prototypical nanoelectronics. However, several processing challenges related to organic contamination at the interface of a 2D material and gate oxide must be overcome to realize robust devices with high yields. Here, we demonstrate an optimized process to realize high-performance field-effect transistor (FET) arrays from large-area (∼5000 µm2), monolayer MoS2 with a yield of 85%. A central element of this process is an exposed material forming gas anneal (EM-FGA) that results in uniform FET performance metrics (i.e., field-effect mobilities, threshold voltages, and contact performance). Complementary analytical measurements show that the EM-FGA process reduces deleterious channel doping effects by decreasing organic contamination while also reducing the prevalence of insulating molybdenum oxide, effectively improving the MoS2-gate oxide interface. The uniform FET performance metrics and high device yield achieved by applying the EM-FGA technique on large-area 2D material flakes will help advance the fabrication of complex 2D nanoelectronic devices and demonstrate the need for improved engineering of the 2D material-gate oxide interface.

Improved contacts to p-type MoS2 transistors by charge-transfer doping and contact engineering.

MoS2 is known to show stubborn n-type behavior due to its intrinsic band structure and Fermi level pinning. Here, we investigate the combined effects of molecular doping and contact engineering on the transport and contact properties of monolayer (ML) MoS2 devices. Significant p-type (hole-transport) behavior was only observed for chemically doped MoS2 devices with high work function palladium (Pd) contacts, while MoS2 devices with low work function metal contacts made from titanium showed ambipolar behavior with electron transport favored even after prolonged p-doping treatment. ML MoS2 transistors with Pd contacts exhibit effective hole mobilities of (2.3 ± 0.7) cm2 V-1 S-1 and an on/off ratio exceeding 106. We also show that p-doping can help to improve electrical contacts in p-type field-effect transistors: relatively low contact resistances of (482 ± 40) kΩ µm and a Schottky barrier height of ≈156 meV were obtained for ML MoS2 transistors. To demonstrate the potential application of 2D-based complementary electronic devices, a MoS2 inverter based on pristine (n-type) and p-doped monolayer MoS2 was fabricated. This work presents a simple and effective route for contact engineering, which enables the exploration and development of high-efficiency 2D-based semiconductor devices.

Contact and Noncontact Measurement of Electronic Transport in Individual 2D SnS Colloidal Semiconductor Nanocrystals.

Colloidal-based solution syntheses offer a scalable and cost-efficient means of producing 2D nanomaterials in high yield. While much progress has been made toward the controlled and tailorable synthesis of semiconductor nanocrystals in solution, it remains a substantial challenge to fully characterize the products' inherent electronic transport properties. This is often due to their irregular morphology or small dimensions, which demand the formation of colloidal assemblies or films as a prerequisite to performing electrical measurements. Here, we report the synthesis of nearly monodisperse 2D colloidal nanocrystals of semiconductor SnS and a thorough investigation of the intrinsic electronic transport properties of single crystals. We utilize a combination of multipoint contact probe measurements and ultrafast terahertz spectroscopy to determine the carrier concentration, carrier mobility, conductivity/resistivity, and majority carrier type of individual colloidal semiconductor nanocrystals. Employing this metrological approach, we compare the electronic properties extracted for distinct morphologies of 2D SnS and relate them to literature values. Our results indicate that the electronic transport of colloidal semiconductors may be tuned through prudent selection of the synthetic conditions. We find that these properties compare favorably to SnS grown using vapor deposition techniques, illustrating that colloidal solution synthesis is a promising route to scalable production of nanoscale 2D materials.

Contacts to solution-synthesized SnS nanoribbons: dependence of barrier height on metal work function.

Tin(ii) monosulfide (SnS) is a layered, anisotropic material that is of interest as a two-dimensional semiconductor for opto-electronic, thermoelectric, and piezoelectric applications. In this study, the effect of work function on contact behavior was investigated. Ni/Au, Pd/Au, Cr/Au, and Ti/Au contacts were fabricated onto individual, solution-synthesized, p-type SnS nanoribbons. The lower work function metals (Cr and Ti) formed Schottky contacts, whereas the higher work function metals (Ni and Pd) formed ohmic or semi-ohmic contacts. Of the ohmic contacts, Ni was found to have a lower contact resistance (∼10-4 Ω cm2 or lower) than Pd (∼10-3 Ω cm2 or lower). Both the calculated Schottky barriers (0.39 and 0.50 eV) for Cr and Ti, respectively, and the ohmic behavior for Ni and Pd agree with behavior predicted by Schottky-Mott theory. The results indicate that high work function metals should be considered to form low resistance contacts to SnS multilayers.

Simpplified extended Kalman filter phase noise estimation for CO-OFDM transmissions.

We propose a flexible simplified extended Kalman filter (S-EKF) scheme that can be applied in both pilot-aided and blind modes for phase noise compensation in 16-QAM CO-OFDM transmission systems employing a small-to-moderate number of subcarriers. The performance of the proposed algorithm is evaluated and compared with conventional pilot-aided (PA) and blind phase search (BPS) methods via extensive an Monte Carlo simulation in a back-to-back configuration and with a dual polarization fiber transmission. For 64 subcarrier 32 Gbaud 16-QAM CO-OFDM systems with 200 kHz combined laser linewidths, an optical signal-to-noise ratio penalty as low as 1 dB can be achieved with the proposed S-EKF scheme using only 2 pilots in the pilot-aided mode and just 4 inputs in the blind mode, resulting in a spectrally efficient enhancement by a factor of 3 and a computational effort reduction by a factor of more than 50 in comparison with the conventional PA and the BPS methods, respectively.

Interacting nanoscale magnetic superatom cluster arrays in molybdenum oxide bronzes.

In this study, we examine several reduced ternary molybdates in the family of yellow rare earth molybdenum bronzes produced by electrochemical synthesis with composition LnMo16O44. These compounds contain an array of electrically isolated but magnetically interacting multi-atom clusters with composition Mo8O36. These arrayed superatom clusters support a single hole shared among the eight molybdenum atoms in the unit, corresponding to a net spin moment of 1µB, and exhibit magnetic exchange between the units via the MoO4 tetrahedra (containing Mo6+ ions) and the LnO8 cubes (containing Ln3+ ions). The findings presented here expand on the physics of the unusual collective properties of multi-atom clusters and extend the discussion of such assemblages to the rich structural chemistry of molybdenum bronzes.

Comparison of DSP-based nonlinear equalizers for intra-channel nonlinearity compensation in coherent optical OFDM.

A novel versatile digital signal processing (DSP)-based equalizer using support vector machine regression (SVR) is proposed for 16-quadrature amplitude modulated (16-QAM) coherent optical orthogonal frequency-division multiplexing (CO-OFDM) and experimentally compared to traditional DSP-based deterministic fiber-induced nonlinearity equalizers (NLEs), namely the full-field digital back-propagation (DBP) and the inverse Volterra series transfer function-based NLE (V-NLE). For a 40 Gb/s 16-QAM CO-OFDM at 2000 km, SVR-NLE extends the optimum launched optical power (LOP) by 4 dB compared to V-NLE by means of reduction of fiber nonlinearity. In comparison to full-field DBP at a LOP of 6 dBm, SVR-NLE outperforms by ∼1 dB in Q-factor. In addition, SVR-NLE is the most computational efficient DSP-NLE.

Advanced Experimental Methods for Low-temperature Magnetotransport Measurement of Novel Materials.

Novel electronic materials are often produced for the first time by synthesis processes that yield bulk crystals (in contrast to single crystal thin film synthesis) for the purpose of exploratory materials research. Certain materials pose a challenge wherein the traditional bulk Hall bar device fabrication method is insufficient to produce a measureable device for sample transport measurement, principally because the single crystal size is too small to attach wire leads to the sample in a Hall bar configuration. This can be, for example, because the first batch of a new material synthesized yields very small single crystals or because flakes of samples of one to very few monolayers are desired. In order to enable rapid characterization of materials that may be carried out in parallel with improvements to their growth methodology, a method of device fabrication for very small samples has been devised to permit the characterization of novel materials as soon as a preliminary batch has been produced. A slight variation of this methodology is applicable to producing devices using exfoliated samples of two-dimensional materials such as graphene, hexagonal boron nitride (hBN), and transition metal dichalcogenides (TMDs), as well as multilayer heterostructures of such materials. Here we present detailed protocols for the experimental device fabrication of fragments and flakes of novel materials with micron-sized dimensions onto substrate and subsequent measurement in a commercial superconducting magnet, dry helium close-cycle cryostat magnetotransport system at temperatures down to 0.300 K and magnetic fields up to 12 T.

Fiber nonlinearity-induced penalty reduction in CO-OFDM by ANN-based nonlinear equalization.

We experimentally demonstrate ∼2 dB quality (Q)-factor enhancement in terms of fiber nonlinearity compensation of 40 Gb/s 16 quadrature amplitude modulation coherent optical orthogonal frequency-division multiplexing at 2000 km, using a nonlinear equalizer (NLE) based on artificial neural networks (ANN). Nonlinearity alleviation depends on escalation of the ANN training overhead and the signal bit rate, reporting ∼4 dBQ-factor enhancement at 70 Gb/s, whereas a reduction of the number of ANN neurons annihilates the NLE performance. An enhanced performance by up to ∼2 dB in Q-factor compared to the inverse Volterra-series transfer function NLE leads to a breakthrough in the efficiency of ANN.

10 Mb/s visible light transmission system using a polymer light-emitting diode with orthogonal frequency division multiplexing.

We present a newly designed polymer light-emitting diode with a bandwidth of ~350 kHz for high-speed visible light communications. Using this new polymer light-emitting diode as a transmitter, we have achieved a record transmission speed of 10 Mb/s for a polymer light-emitting diode-based optical communication system with an orthogonal frequency division multiplexing technique, matching the performance of single carrier formats using multitap equalization. For achieving such a high data-rate, a power pre-emphasis technique was adopted.

Axial SiGe heteronanowire tunneling field-effect transistors.

We present silicon-compatible trigated p-Ge/i-Si/n-Si axial heteronanowire tunneling field-effect transistors (TFETs), where on-state tunneling occurs in the Ge drain section, while off-state leakage is dominated by the Si junction in the source. Our TFETs have high I(ON) ~ 2 µA/µm, fully suppressed ambipolarity, and a subthreshold slope SS ~ 140 mV/decade over 4 decades of current with lowest SS ~ 50 mV/decade. Device operation in the tunneling mode is confirmed by three-dimensional TCAD simulation. Interestingly, in addition to the TFET mode, our devices work as standard nanowire FETs with a good I(ON)/I(OFF) ratio when the source-drain junction is forward-biased. The improved transport in both biasing modes confirms the benefits of utilizing bandgap engineered axial nanowires for enhancing device performance.