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When the Fermi level matches the Dirac point in graphene, the reduced charge screening can dramatically enhance electron-electron (e-e) scattering to produce a strongly interacting Dirac liquid. While the dominance of e-e scattering already leads to novel behaviors, such as electron hydrodynamic flow, further exotic phenomena have been predicted to arise specifically from the unique kinematics of e-e scattering in massless Dirac systems. Here, we use optoelectronic probes, which are highly sensitive to the kinematics of electron scattering, to uncover a giant intrinsic photocurrent response in pristine graphene. This photocurrent emerges exclusively at the charge neutrality point and vanishes abruptly at non-zero charge densities. Moreover, it is observed at places with broken reflection symmetry, and it is selectively enhanced at free graphene edges with sharp bends. Our findings reveal that the photocurrent relaxation is strongly suppressed by a drastic change of fast photocarrier kinematics in graphene when its Fermi level matches the Dirac point. The emergence of robust photocurrents in neutral Dirac materials promises new energy-harvesting functionalities and highlights intriguing electron dynamics in the optoelectronic response of Dirac fluids., Comment: Originally submitted version

The electrical Hall effect is the production of a transverse voltage under an out-of-plane magnetic field. Historically, studies of the Hall effect have led to major breakthroughs including the discoveries of Berry curvature and the topological Chern invariants. In magnets, the internal magnetization allows Hall conductivity in the absence of external magnetic field. This anomalous Hall effect (AHE) has become an important tool to study quantum magnets. In nonmagnetic materials without external magnetic fields, the electrical Hall effect is rarely explored because of the constraint by time-reversal symmetry. However, strictly speaking, only the Hall effect in the linear response regime, i.e., the Hall voltage linearly proportional to the external electric field, identically vanishes due to time-reversal symmetry. The Hall effect in the nonlinear response regime, on the other hand, may not be subject to such symmetry constraints. Here, we report the observation of the nonlinear Hall effect (NLHE) in the electrical transport of the nonmagnetic 2D quantum material, bilayer WTe2. Specifically, flowing an electrical current in bilayer WTe2 leads to a nonlinear Hall voltage in the absence of magnetic field. The NLHE exhibits unusual properties sharply distinct from the AHE in metals: The NLHE shows a quadratic I-V characteristic; It strongly dominates the nonlinear longitudinal response, leading to a Hall angle of about 90 degree. We further show that the NLHE directly measures the "dipole moment" of the Berry curvature, which arises from layer-polarized Dirac fermions in bilayer WTe2. Our results demonstrate a new Hall effect and provide a powerful methodology to detect Berry curvature in a wide range of nonmagnetic quantum materials in an energy-resolved way.

Imaging materials and inner structures with resolution below the diffraction limit has become of fundamental importance in recent years for a wide variety of applications. In this work, we report sub-diffractive internal structure diagnosis of hexagonal boron nitride by exciting and imaging hyperbolic phonon polaritons. Based on their unique propagation properties, we are able to accurately locate defects in the crystal interior with nanometer resolution. The precise location, size and geometry of the concealed defects is reconstructed by analyzing the polariton wavelength, reflection coefficient and their dispersion. We have also studied the evolution of polariton reflection, transmission and scattering as a function of defect size and photon frequency. The nondestructive high-precision polaritonic structure diagnosis technique introduced here can be also applied to other hyperbolic or waveguide systems, and may be deployed in the next-generation bio-medical imaging, sensing and fine structure analysis., Comment: 18 pages, 4 figures

Recent experimental evidence for the quantum spin Hall (QSH) state in monolayer WTe$_2$ has bridged two of the most active fields of condensed matter physics, 2D materials and topological physics. This 2D topological crystal also displays unconventional spin-torque and gate-tunable superconductivity. While the realization of QSH has demonstrated the nontrivial topology of the electron wavefunctions of monolayer WTe$_2$, the geometrical properties of the wavefunction, such as the Berry curvature, remain unstudied. On the other hand, it has been increasingly recognized that the Berry curvature plays an important role in multiple areas of condensed matter physics including nonreciprocal electron transport, enantioselective optical responses, chiral polaritons and even unconventional superconductivity. Here we utilize mid-infrared optoelectronic microscopy to investigate the Berry curvature in monolayer WTe$_2$. By optically exciting electrons across the inverted QSH gap, we observe an in-plane circular photogalvanic current even under normal incidence. The application of an out-of-plane displacement field further systematically controls the direction and magnitude of the photocurrent. Our observed photocurrent reveals a novel Berry curvature dipole that arises from the nontrivial wavefunctions near the inverted gap edge. These previously unrealized Berry curvature dipole and strong electric field effect are uniquely enabled by the inverted band structure and tilted crystal lattice of monolayer WTe$_2$. Such an electrically switchable Berry curvature dipole opens the door to the observation of a wide range of quantum geometrical phenomena, such as quantum nonlinear Hall, orbital-Edelstein and chiral polaritonic effects., Comment: Originally submitted version, main text combined with part of the SI

Topological crystalline insulators (TCI) are insulating electronic phases of matter with nontrivial topology originating from crystalline symmetries. Recent theoretical advances have provided powerful guidelines to search for TCIs in real materials. Using density functional theory, we identify a class of new TCI states in the tetragonal lattice of the Ca$_2$As material family. On both top and side surfaces, we observe topological surface states protected independently by rotational and mirror symmetries. We show that a particular lattice distortion can single out the newly proposed topological protection by the rotational symmetry. As a result, the Dirac points of the topological surface states are moved to generic locations in momentum space away from any high symmetry lines. Such topological surface states have not been seen before. Moreover, the other family members, including Ca$_2$Sb, Ca$_2$Bi and Sr$_2$Sb, feature different topological surface states due to their distinct topological invariants. We thus further propose topological phase transitions in the pseudo-binary systems such as (Ca$_{1-x}$Sr$_x$)$_2$As and Ca$_2$As$_x$Sb$_{1-x}$. Our work reveals rich and exotic TCI physics across the Ca$_2$As family of materials, and suggests the feasibility of materials database search methods to discover new TCIs., Comment: 5 pages, 4 figures

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to inter-particle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

A Weyl semimetal (WSM) is a novel topological phase of matter, in which Weyl fermions (WFs) arise as pseudo-magnetic monopoles in its momentum space. The chirality of the WFs, given by the sign of the monopole charge, is central to the Weyl physics, since it directly serves as the sign of the topological number and gives rise to exotic properties such as Fermi arcs and the chiral anomaly. Despite being the defining property of a WSM, the chirality of the WFs has never been experimentally measured. Here, we directly detect the chirality of the WFs by measuring the photocurrent in response to circularly polarized mid-infrared light. The resulting photocurrent is determined by both the chirality of WFs and that of the photons. Our results pave the way for realizing a wide range of theoretical proposals for studying and controlling the WFs and their associated quantum anomalies by optical and electrical means. More broadly, the two chiralities, analogous to the two valleys in 2D materials, lead to a new degree of freedom in a 3D crystal with potential novel pathways to store and carry information., Comment: Accepted to Nature Physics. Version of original submission

We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field microscope is itself an efficient polariton launcher. Our analysis reveals that the scanning tips are superior to other types of emitters we have investigated. Furthermore, the study of polariton emission and emission efficiency may provide insights for development of polaritonic devices and for fundamental studies of collective modes in other van der Waals materials., Comment: 19 pages, 3 figures

Ultrafast electron thermalization - the process leading to Auger recombination, carrier multiplication via impact ionization and hot carrier luminescence - occurs when optically excited electrons in a material undergo rapid electron-electron scattering to redistribute excess energy and reach electronic thermal equilibrium. Due to extremely short time and length scales, the measurement and manipulation of electron thermalization in nanoscale devices remains challenging even with the most advanced ultrafast laser techniques. Here, we overcome this challenge by leveraging the atomic thinness of two-dimensional van der Waals (vdW) materials in order to introduce a highly tunable electron transfer pathway that directly competes with electron thermalization. We realize this scheme in a graphene-boron nitride-graphene (G-BN-G) vdW heterostructure, through which optically excited carriers are transported from one graphene layer to the other. By applying an interlayer bias voltage or varying the excitation photon energy, interlayer carrier transport can be controlled to occur faster or slower than the intralayer scattering events, thus effectively tuning the electron thermalization pathways in graphene. Our findings, which demonstrate a novel means to probe and directly modulate electron energy transport in nanoscale materials, represent an important step toward designing and implementing novel optoelectronic and energy-harvesting devices with tailored microscopic properties., Comment: Accepted to Nature Physics

Diverse parallel stitched two-dimensional heterostructures are synthesized, including metal-semiconductor (graphene-MoS2), semiconductor-semiconductor (WS2-MoS2), and insulator-semiconductor (hBN-MoS2), directly through selective sowing of aromatic molecules as the seeds in chemical vapor deposition (CVD) method. Our methodology enables the large-scale fabrication of lateral heterostructures with arbitrary patterns, and clean and precisely aligned interfaces, which offers tremendous potential for its application in integrated circuits., Comment: 30 pages, 4 figures, Accepted by Advanced Materials

Opto-electronic devices utilizing graphene have already demonstrated unique capabilities, which are much more difficult to realize with conventional technologies. However, the requirements in terms of material quality and uniformity are very demanding. A major roadblock towards high-performance devices are the nanoscale variations of graphene properties, which strongly impact the macroscopic device behaviour. Here, we present and apply opto-electronic nanoscopy to measure locally both the optical and electronic properties of graphene devices. This is achieved by combining scanning near-field infrared nanoscopy with electrical device read-out, allowing infrared photocurrent mapping at length scales of tens of nanometers. We apply this technique to study the impact of edges and grain boundaries on spatial carrier density profiles and local thermoelectric properties. Moreover, we show that the technique can also be applied to encapsulated graphene/hexagonal boron nitride (h-BN) devices, where we observe strong charge build-up near the edges, and also address a device solution to this problem. The technique enables nanoscale characterization for a broad range of common graphene devices without the need of special device architectures or invasive graphene treatment.

Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies addressed the general operation of graphene-based photo-thermoelectric devices, and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster time scale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 femtoseconds. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 femtosecond laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity between 500 and 1500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications., Comment: 6 pages, 4 figures

We report on temperature dependent photocurrent measurements of high-quality dual-gated monolayer graphene (MLG) p-n junction devices. A photothermoelectric (PTE) effect governs the photocurrent response in our devices, allowing us to track the hot electron temperature and probe hot electron cooling channels over a wide temperature range (4 K to 300 K). At high temperatures ($T > T^*$), we found that both the peak photocurrent and the hot spot size decreased with temperature, while at low temperatures ($T < T^*$), we found the opposite, namely that the peak photocurrent and the hot spot size increased with temperature. This non-monotonic temperature dependence can be understood as resulting from the competition between two hot electron cooling pathways: (a) (intrinsic) momentum-conserving normal collisions (NC) that dominates at low temperatures and (b) (extrinsic) disorder-assisted supercollisions (SC) that dominates at high temperatures. Gate control in our high quality samples allows us to resolve the two processes in the same device for the first time. The peak temperature $T^*$ depends on carrier density and disorder concentration, thus allowing for an unprecedented way of controlling graphene's photoresponse., Comment: 5 pages, 4 figures