Angle-resolved transport non-reciprocity and spontaneous symmetry breaking in twisted trilayer graphene.

The identification and characterization of spontaneous symmetry breaking is central to our understanding of strongly correlated two-dimensional materials. In this work, we utilize the angle-resolved measurements of transport non-reciprocity to investigate spontaneous symmetry breaking in twisted trilayer graphene. By analysing the angular dependence of non-reciprocity in both longitudinal and transverse channels, we are able to identify the symmetry axis associated with the underlying electronic order. We report that a hysteretic rotation in the mirror axis can be induced by thermal cycles and a large current bias, supporting the spontaneous breaking of rotational symmetry. Moreover, the onset of non-reciprocity with decreasing temperature coincides with the emergence of orbital ferromagnetism. Combined with the angular dependence of the superconducting diode effect, our findings uncover a direct link between rotational and time-reversal symmetry breaking. These symmetry requirements point towards exchange-driven instabilities in momentum space as a possible origin for transport non-reciprocity in twisted trilayer graphene.

Recent Advances in 2D Material Theory, Synthesis, Properties, and Applications.

Two-dimensional (2D) material research is rapidly evolving to broaden the spectrum of emergent 2D systems. Here, we review recent advances in the theory, synthesis, characterization, device, and quantum physics of 2D materials and their heterostructures. First, we shed insight into modeling of defects and intercalants, focusing on their formation pathways and strategic functionalities. We also review machine learning for synthesis and sensing applications of 2D materials. In addition, we highlight important development in the synthesis, processing, and characterization of various 2D materials (e.g., MXnenes, magnetic compounds, epitaxial layers, low-symmetry crystals, etc.) and discuss oxidation and strain gradient engineering in 2D materials. Next, we discuss the optical and phonon properties of 2D materials controlled by material inhomogeneity and give examples of multidimensional imaging and biosensing equipped with machine learning analysis based on 2D platforms. We then provide updates on mix-dimensional heterostructures using 2D building blocks for next-generation logic/memory devices and the quantum anomalous Hall devices of high-quality magnetic topological insulators, followed by advances in small twist-angle homojunctions and their exciting quantum transport. Finally, we provide the perspectives and future work on several topics mentioned in this review.

Bridging the gap between atomically thin semiconductors and metal leads.

Electrically interfacing atomically thin transition metal dichalcogenide semiconductors (TMDSCs) with metal leads is challenging because of undesired interface barriers, which have drastically constrained the electrical performance of TMDSC devices for exploring their unconventional physical properties and realizing potential electronic applications. Here we demonstrate a strategy to achieve nearly barrier-free electrical contacts with few-layer TMDSCs by engineering interfacial bonding distortion. The carrier-injection efficiency of such electrical junction is substantially increased with robust ohmic behaviors from room to cryogenic temperatures. The performance enhancements of TMDSC field-effect transistors are well reflected by the low contact resistance (down to 90 Ωµm in MoS2, towards the quantum limit), the high field-effect mobility (up to 358,000 cm2V-1s-1 in WSe2), and the prominent transport characteristics at cryogenic temperatures. This method also offers possibilities of the local manipulation of atomic structures and electronic properties for TMDSC device design.

Spin-orbit-driven ferromagnetism at half moiré filling in magic-angle twisted bilayer graphene.

Strong electron correlation and spin-orbit coupling (SOC) can have a profound influence on the electronic properties of materials. We examine their combined influence on a 2-dimensional electronic system at the atomic interface between magic-angle twisted bilayer graphene and a tungsten diselenide crystal. Strong electron correlation within the moiré flatband stabilizes correlated insulating states at both quarter and half filling, and SOC transforms these Mott-like insulators into ferromagnets, evidenced by robust anomalous Hall effect with hysteretic switching behavior. The coupling between spin and valley degrees of freedom is demonstrated through the control of the magnetic order with an in-plane magnetic field, or a perpendicular electric field. Our findings establish an experimental knob to engineer topological properties of moiré bands in twisted bilayer graphene and related systems.

Interaction effects and superconductivity signatures in twisted double-bilayer WSe2.

Twisted bilayer graphene provides a new two-dimensional platform for studying electron interaction phenomena and flat band properties such as correlated insulator transition, superconductivity and ferromagnetism at certain magic angles. Here, we present experimental characterization of interaction effects and superconductivity signatures in p-type twisted double-bilayer WSe2. Enhanced interlayer interactions are observed when the twist angle decreases to a few degrees as reflected by the high-order satellites in the electron diffraction patterns taken from the reconstructed domains from a conventional moiré superlattice. In contrast to twisted bilayer graphene, there is no specific magic angle for twisted WSe2. Flat band properties are observable at twist angles ranging from 1 to 4 degrees. Our work has facilitated future study in the area of flat band related properties in twisted transition metal dichalcogenide layered structures.

Determining Interaction Enhanced Valley Susceptibility in Spin-Valley-Locked MoS2.

Two-dimensional transition metal dichalcogenides (TMDCs) are recently emerged electronic systems with various novel properties, such as spin-valley locking, circular dichroism, valley Hall effect, and superconductivity. The reduced dimensionality and large effective masses further produce unconventional many-body interaction effects. Here we reveal strong interaction effects in the conduction band of MoS2 by transport experiment. We study the massive Dirac electron Landau levels (LL) in high-quality MoS2 samples with field-effect mobilities of 24 000 cm2/(V·s) at 1.2 K. We identify the valley-resolved LLs and low-lying polarized LLs using the Lifshitz-Kosevitch formula. By further tracing the LL crossings in the Landau fan diagram, we unambiguously determine the density-dependent valley susceptibility and the interaction enhanced g-factor from 12.7 to 23.6. Near integer ratios of Zeeman-to-cyclotron energies, we discover LL anticrossings due to the formation of quantum Hall Ising ferromagnets, the valley polarizations of which appear to be reversible by tuning the density or an in-plane magnetic field. Our results provide evidence for many-body interaction effects in the conduction band of MoS2 and establish a fertile ground for exploring strongly correlated phenomena of massive Dirac electrons.

Intrinsic valley Hall transport in atomically thin MoS2.

Electrons hopping in two-dimensional honeycomb lattices possess a valley degree of freedom in addition to charge and spin. In the absence of inversion symmetry, these systems were predicted to exhibit opposite Hall effects for electrons from different valleys. Such valley Hall effects have been achieved only by extrinsic means, such as substrate coupling, dual gating, and light illuminating. Here we report the first observation of intrinsic valley Hall transport without any extrinsic symmetry breaking in the non-centrosymmetric monolayer and trilayer MoS2, evidenced by considerable nonlocal resistance that scales cubically with local resistance. Such a hallmark survives even at room temperature with a valley diffusion length at micron scale. By contrast, no valley Hall signal is observed in the centrosymmetric bilayer MoS2. Our work elucidates the topological origin of valley Hall effects and marks a significant step towards the purely electrical control of valley degree of freedom in topological valleytronics.

Gate-tunable strong-weak localization transition in few-layer black phosphorus.

Atomically-thin black phosphorus (BP) field-effect transistors show strong-weak localization transition, which is tunable through gate voltages. Hopping transports through charge impurity-induced localized states are observed at low carrier density regime. Variable-range hopping model is applied to simulate scattering behaviors of charge carriers. In the high carrier concentration regime, a negative magnetoresistance indicates weak localization effects. The extracted phase coherence length is power-law temperature-dependent [Formula: see text] and demonstrates inelastic electron-electron interactions and the 2D transport features in few-layer BP field-effect devices. The competition between localization and phase coherence lengths is investigated and analyzed based on observed gate-tunable strong-weak localization transition in few-layer BP.

Isolation and Characterization of Few-Layer Manganese Thiophosphite.

This work reports an experimental study on an antiferromagnetic honeycomb lattice of MnPS3 that couples the valley degree of freedom to a macroscopic antiferromagnetic order. The crystal structure of MnPS3 is identified by high-resolution scanning transmission electron microscopy. Layer-dependent angle-resolved polarized Raman fingerprints of the MnPS3 crystal are obtained, and the Raman peak at 383 cm-1 exhibits 100% polarity. Temperature dependences of anisotropic magnetic susceptibility of the MnPS3 crystal are measured in a superconducting quantum interference device. Anisotropic behaviors of the magnetic moment are explored on the basis of the mean field approximation model. Ambipolar electronic conducting channels in MnPS3 are realized by the liquid gating technique. The conducting channel of MnPS3 offers a platform for exploring the spin/valleytronics and magnetic orders in 2D limitation.

Odd-Integer Quantum Hall States and Giant Spin Susceptibility in p-Type Few-Layer WSe_{2}.

We fabricate high-mobility p-type few-layer WSe_{2} field-effect transistors and surprisingly observe a series of quantum Hall (QH) states following an unconventional sequence predominated by odd-integer states under a moderate strength magnetic field. By tilting the magnetic field, we discover Landau level crossing effects at ultralow coincident angles, revealing that the Zeeman energy is about 3 times as large as the cyclotron energy near the valence band top at the Γ valley. This result implies the significant roles played by the exchange interactions in p-type few-layer WSe_{2}, in which itinerant or QH ferromagnetism likely occurs. Evidently, the Γ valley of few-layer WSe_{2} offers a unique platform with unusually heavy hole carriers and a substantially enhanced g factor for exploring strongly correlated phenomena.

Achieving Ultrahigh Carrier Mobility in Two-Dimensional Hole Gas of Black Phosphorus.

We demonstrate that a field-effect transistor (FET) made of few-layer black phosphorus (BP) encapsulated in hexagonal boron nitride (h-BN) in vacuum exhibits a room-temperature hole mobility of 5200 cm2/(Vs), being limited just by the phonon scattering. At cryogenic temperatures, the FET mobility increases up to 45 000 cm2/(Vs), which is five times higher compared to the mobility obtained in earlier reports. The unprecedentedly clean h-BN-BP-h-BN heterostructure exhibits Shubnikov-de Haas oscillations and a quantum Hall effect with Landau level (LL) filling factors down to v = 2 in conventional laboratory magnetic fields. Moreover, carrier density independent effective mass of m* = 0.26 m0 is measured, and a Landé g-factor of g = 2.47 is reported. Furthermore, an indication for a distinct hole transport behavior with up- and down-spin orientations is found.

Even-odd layer-dependent magnetotransport of high-mobility Q-valley electrons in transition metal disulfides.

In few-layer transition metal dichalcogenides (TMDCs), the conduction bands along the ΓK directions shift downward energetically in the presence of interlayer interactions, forming six Q valleys related by threefold rotational symmetry and time reversal symmetry. In even layers, the extra inversion symmetry requires all states to be Kramers degenerate; whereas in odd layers, the intrinsic inversion asymmetry dictates the Q valleys to be spin-valley coupled. Here we report the transport characterization of prominent Shubnikov-de Hass (SdH) oscillations and the observation of the onset of quantum Hall plateaus for the Q-valley electrons in few-layer TMDCs. Universally in the SdH oscillations, we observe a valley Zeeman effect in all odd-layer TMDC devices and a spin Zeeman effect in all even-layer TMDC devices, which provide a crucial information for understanding the unique properties of multi-valley band structures of few-layer TMDCs.

A fast transfer-free synthesis of high-quality monolayer graphene on insulating substrates by a simple rapid thermal treatment.

The transfer-free synthesis of high-quality, large-area graphene on a given dielectric substrate, which is highly desirable for device applications, remains a significant challenge. In this paper, we report on a simple rapid thermal treatment (RTT) method for the fast and direct growth of high-quality, large-scale monolayer graphene on a SiO2/Si substrate from solid carbon sources. The stack structure of a solid carbon layer/copper film/SiO2 is adopted in the RTT process. The inserted copper film does not only act as an active catalyst for the carbon precursor but also serves as a "filter" that prevents premature carbon dissolution, and thus, contributes to graphene growth on SiO2/Si. The produced graphene exhibits a high carrier mobility of up to 3000 cm(2) V(-1) s(-1) at room temperature and standard half-integer quantum oscillations. Our work provides a promising simple transfer-free approach using solid carbon sources to obtain high-quality graphene for practical applications.

van der Waals epitaxial growth of atomically thin Bi2Se3 and thickness-dependent topological phase transition.

Two-dimensional (2D) atomic-layered heterostructures stacked by van der Waals interactions recently introduced new research fields, which revealed novel phenomena and provided promising applications for electronic, optical, and optoelectronic devices. In this study, we report the van der Waals epitaxial growth of high-quality atomically thin Bi2Se3 on single crystalline hexagonal boron nitride (h-BN) by chemical vapor deposition. Although the in-plane lattice mismatch between Bi2Se3 and h-BN is approximately 65%, our transmission electron microscopy analysis revealed that Bi2Se3 single crystals epitaxially grew on h-BN with two commensurate states; that is, the (1̅21̅0) plane of Bi2Se3 was preferably parallel to the (1̅100) or (1̅21̅0) plane of h-BN. In the case of the Bi2Se3 (2̅110) ∥ h-BN (11̅00) state, the Moiré pattern wavelength in the Bi2Se3/h-BN superlattice can reach 5.47 nm. These naturally formed thin crystals facilitated the direct assembly of h-BN/Bi2Se3/h-BN sandwiched heterostructures without introducing any impurity at the interfaces for electronic property characterization. Our quantum capacitance (QC) measurements showed a compelling phenomenon of thickness-dependent topological phase transition, which was attributed to the coupling effects of two surface states from Dirac Fermions at/or above six quintuple layers (QLs) to gapped Dirac Fermions below six QLs. Moreover, in ultrathin Bi2Se3 (e.g., 3 QLs), we observed the midgap states induced by intrinsic defects at cryogenic temperatures. Our results demonstrated that QC measurements based on h-BN/Bi2Se3/h-BN sandwiched structures provided rich information regarding the density of states of Bi2Se3, such as quantum well states and Landau quantization. Our approach in fabricating h-BN/Bi2Se3/h-BN sandwiched device structures through the combination of bottom-up growth and top-down dry transferring techniques can be extended to other two-dimensional layered heterostructures.