Highly anisotropic spin transport in ultrathin black phosphorus.

In anisotropic crystals, the direction-dependent effective mass of carriers can have a profound impact on spin transport dynamics. The puckered crystal structure of black phosphorus leads to direction-dependent charge transport and optical response, suggesting that it is an ideal system for studying anisotropic spin transport. To this end, we fabricate and characterize high-mobility encapsulated ultrathin black-phosphorus-based spin valves in a four-terminal geometry. Our measurements show that in-plane spin lifetimes are strongly gate tunable and exceed one nanosecond. Through high out-of-plane magnetic fields, we observe a fivefold enhancement in the out-of-plane spin signal case compared to in-plane and estimate a colossal spin-lifetime anisotropy of ∼6. This finding is further confirmed by oblique Hanle measurements. Additionally, we estimate an in-plane spin-lifetime anisotropy ratio of up to 1.8. Our observation of strongly anisotropic spin transport along three orthogonal axes in this pristine material could be exploited to realize directionally tunable spin transport.

Strong Moiré Excitons in High-Angle Twisted Transition Metal Dichalcogenide Homobilayers with Robust Commensuration.

The burgeoning field of twistronics, which concerns how changing the relative twist angles between two materials creates new optoelectronic properties, offers a novel platform for studying twist-angle dependent excitonic physics. Herein, by surveying a range of hexagonal phase transition metal dichalcogenides (TMD) twisted homobilayers, we find that 21.8 ± 1.0°-twisted (7a×7a) and 27.8 ± 1.0°-twisted (13a×13a) bilayers account for nearly 20% of the total population of twisted bilayers in solution-phase restacked bilayers and can be found also in chemical vapor deposition (CVD) samples. Examining the optical properties associated with these twisted angles, we found that 21.8 ± 1.0° twisted MoS2 bilayers exhibit an intense moiré exciton peak in the photoluminescence (PL) spectra, originating from the refolded Brillouin zones. Our work suggests that commensurately twisted TMD homobilayers with short commensurate wavelengths can have interesting optoelectronic properties that are different from the small twist angle counterparts.

Electron Doping of Ultrathin Black Phosphorus with Cu Adatoms.

Few-layer black phosphorus is a monatomic two-dimensional crystal with a direct band gap that has high carrier mobility for both holes and electrons. Similarly to other layered atomic crystals, like graphene or layered transition metal dichalcogenides, the transport behavior of few-layer black phosphorus is sensitive to surface impurities, adsorbates, and adatoms. Here we study the effect of Cu adatoms onto few-layer black phosphorus by characterizing few-layer black phosphorus field effect devices and by performing first-principles calculations. We find that the addition of Cu adatoms can be used to controllably n-dope few layer black phosphorus, thereby lowering the threshold voltage for n-type conduction without degrading the transport properties. We demonstrate a scalable 2D material-based complementary inverter which utilizes a boron nitride gate dielectric, a graphite gate, and a single bP crystal for both the p- and n-channels. The inverter operates at matched input and output voltages, exhibits a gain of 46, and does not require different contact metals or local electrostatic gating.

Van der Waals force: a dominant factor for reactivity of graphene.

Reactivity control of graphene is an important issue because chemical functionalization can modulate graphene's unique mechanical, optical, and electronic properties. Using systematic optical studies, we demonstrate that van der Waals interaction is the dominant factor for the chemical reactivity of graphene on two-dimensional (2D) heterostructures. A significant enhancement in the chemical stability of graphene is achieved by replacing the common SiO2 substrate with 2D crystals such as an additional graphene layer, WS2, MoS2, or h-BN. Our theoretical and experimental results show that its origin is a strong van der Waals interaction between the graphene layer and the 2D substrate. This results in a high resistive force on graphene toward geometric lattice deformation. We also demonstrate that the chemical reactivity of graphene can be controlled by the relative lattice orientation with respect to the substrates and thus can be used for a wide range of applications including hydrogen storage.

Tuning and Persistent Switching of Graphene Plasmons on a Ferroelectric Substrate.

We characterized plasmon propagation in graphene on thin films of the high-κ dielectric PbZr0.3Ti0.7O3 (PZT). Significant modulation (up to ±75%) of the plasmon wavelength was achieved with application of ultrasmall voltages (< ±1 V) across PZT. Analysis of the observed plasmonic fringes at the graphene edge indicates that carriers in graphene on PZT behave as noninteracting Dirac Fermions approximated by a semiclassical Drude response, which may be attributed to strong dielectric screening at the graphene/PZT interface. Additionally, significant plasmon scattering occurs at the grain boundaries of PZT from topographic and/or polarization induced graphene conductivity variation in the interior of graphene, reducing the overall plasmon propagation length. Lastly, through application of 2 V across PZT, we demonstrate the capability to persistently modify the plasmonic response of graphene through transient voltage application.

Nanometer thick elastic graphene engine.

Significant progress has been made in the construction and theoretical understanding of molecular motors because of their potential use. Here, we have demonstrated fabrication of a simple but powerful 1 nm thick graphene engine. The engine comprises a high elastic membrane-piston made of graphene and weakly chemisorbed ClF3 molecules as the high power volume changeable actuator, while a 532 nm LASER acts as the ignition plug. Rapid volume expansion of the ClF3 molecules leads to graphene blisters. The size of the blister is controllable by changing the ignition parameters. The estimated internal pressure per expansion cycle of the engine is about ∼10(6) Pa. The graphene engine presented here shows exceptional reliability, showing no degradation after 10,000 cycles.

Third-order nonlinear Hall effect in a quantum Hall system.

In two-dimensional systems, perpendicular magnetic fields can induce a bulk band gap and chiral edge states, which gives rise to the quantum Hall effect. The quantum Hall effect is characterized by zero longitudinal resistance (Rxx) and Hall resistance (Rxy) plateaus quantized to h/(υe2) in the linear response regime, where υ is the Landau level filling factor, e is the elementary charge and h is Planck's constant. Here we explore the nonlinear response of monolayer graphene when tuned to a quantum Hall state. We observe a third-order Hall effect that exhibits a nonzero voltage plateau scaling cubically with the probe current. By contrast, the third-order longitudinal voltage remains zero. The magnitude of the third-order response is insensitive to variations in magnetic field (down to ~5 T) and in temperature (up to ~60 K). Moreover, the third-order response emerges in graphene devices with a variety of geometries, different substrates and stacking configurations. We term the effect third-order nonlinear response of the quantum Hall state and propose that electron-electron interaction between the quantum Hall edge states is the origin of the nonlinear response of the quantum Hall state.

Graphene moiré superlattices with giant quantum nonlinearity of chiral Bloch electrons.

Graphene-based samples have shown a plethora of exotic characteristics and these properties may help the realization of a new generation of fast electronic devices. However, graphene's centrosymmetry prohibits second-order electronic transport. Here, we show giant second-order nonlinear transports in graphene moiré superlattices at zero magnetic field, both longitudinal and transverse to the applied current direction. High carrier mobility and inversion symmetry breaking by hexagonal boron nitride lead to nonlinear conductivities five orders of magnitude larger than those in WTe2. The nonlinear conductivity strongly depends on the gate voltage as well as on the stacking configuration, with a giant enhancement originating from the moiré bands. Longitudinal nonlinear conductivity cannot originate from Berry curvature dipoles. Our theoretical modelling highlights skew scattering of chiral Bloch electrons as the physical origin. With these results, we demonstrate nonlinear charge transport due to valley-contrasting chirality, which constitutes an alternative means to induce second-order transports in van der Waals heterostructures. Our approach is promising for applications in frequency-doubling and energy harvesting via rectification.

Conductance oscillations induced by ballistic snake states in a graphene heterojunction.

The realization of p-n junctions in graphene, combined with the gapless and chiral nature of its massless Dirac fermions has led to the observation of many intriguing phenomena such as the quantum Hall effect in the bipolar regime, Klein tunnelling and Fabry-Pérot interferences, all of which involve electronic transport across p-n junctions. Ballistic snake states propagating along the p-n junctions have been predicted to induce conductance oscillations, manifesting their twisting nature. However, transport studies along p-n junctions have so far only been performed in low mobility devices. Here, we report the observation of conductance oscillations due to ballistic snake states along a p-n interface in high-quality graphene encapsulated by hexagonal boron nitride. These snake states are exceptionally robust as they can propagate over 12 µm, limited only by the size of our sample, and survive up to at least 120 K. The ability to guide carriers over a long distance provide a crucial building block for graphene-based electron optics.

Air-stable transport in graphene-contacted, fully encapsulated ultrathin black phosphorus-based field-effect transistors.

The presence of direct bandgap and high mobility in semiconductor few-layer black phosphorus offers an attractive prospect for using this material in future two-dimensional electronic devices. However, creation of barrier-free contacts which is necessary to achieve high performance in black phosphorus-based devices is challenging and currently limits their potential for applications. Here, we characterize fully encapsulated ultrathin (down to bilayer) black phosphorus field effect transistors fabricated under inert gas conditions by utilizing graphene as source-drain electrodes and boron nitride as an encapsulation layer. The observation of a linear ISD-VSD behavior with negligible temperature dependence shows that graphene electrodes lead to barrier-free contacts, solving the issue of Schottky barrier limited transport in the technologically relevant two-terminal field-effect transistor geometry. Such one-atom-thick conformal source-drain electrodes also enable the black phosphorus surface to be sealed, to avoid rapid degradation, with the inert boron nitride encapsulating layer. This architecture, generally applicable for other sensitive two-dimensional crystals, results in air-stable, hysteresis-free transport characteristics.