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Implementing and tuning chirality is fundamental in physics, chemistry, and material science. Chiral charge density waves (CDWs), where chirality arises from correlated charge orders, are attracting intense interest due to their exotic transport and optical properties. However, a general framework for predicting chiral CDW materials is lacking, primarily because the underlying mechanisms remain elusive. Here, we address this challenge by developing the first comprehensive predictive framework, systematically identifying chiral CDW materials via first-principles calculations. The key lies in the previously overlooked phase difference of the CDW Q-vectors between layers, which is linked to opposite collective atomic displacements across different layers. This phase difference induces a spiral arrangement of the Q-vectors, ultimately giving rise to a chiral structure in real space. We validate our framework by applying it to the kagome lattice AV$_{3}$Sb$_{5}$ (A = K, Rb, Cs), successfully predicting emergent structural chirality. To demonstrate the generality of our approach, we extend it to predict chiral CDWs in the triangular-lattice NbSe$_{2}$. Beyond material predictions, our theory uncovers a universal and unprecedented Hall effect in chiral CDW materials, occurring without external magnetic fields or intrinsic magnetization. Our experiments on CsV$_{3}$Sb$_{5}$ confirm this prediction, observing a unique signature where the Hall conductivity's sign reverses when the input current is reversed, a phenomenon distinct from known Hall effects. Our findings elucidate the mechanisms behind chiral CDWs and open new avenues for discovering materials with unconventional quantum properties, with potential applications in next-generation electronic and spintronic devices.

In a PN junction, the separation between positive and negative charges leads to diode transport. In the past few years, the intrinsic diode transport in noncentrosymmetric polar conductors has attracted great interest, because it suggests novel nonlinear applications and provides a symmetry-sensitive probe of Fermi surface. Recently, such studies have been extended to noncentrosymmetric superconductors, realizing the superconducting diode effect. Here, we show that, even in a centrosymmetric crystal without directional charge separation, the spins of an antiferromagnet (AFM) can generate a spatial directionality, leading to an AFM diode effect. We observe large second-harmonic transport in a nonlinear electronic device enabled by the compensated AFM state of even-layered MnBi2Te4. We also report a novel electrical sum-frequency generation (SFG), which has been rarely explored in contrast to the well-known optical SFG in wide-gap insulators. We demonstrate that the AFM enables an in-plane field-effect transistor and harvesting of wireless electromagnetic energy. The electrical SFG establishes a powerful method to study nonlinear electronics built by quantum materials. The AFM diode effect paves the way for potential device concepts including AFM logic circuits, self-powered AFM spintronics, and other applications that potentially bridge nonlinear electronics with AFM spintronics., Comment: 33+8 pages, 14+2 figures. arXiv admin note: text overlap with arXiv:2306.09575

The convergence of topology and correlations represents a highly coveted realm in the pursuit of novel quantum states of matter. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order, not possible in quantum Hall and Chern insulator systems. However, the QSH insulator with quantized edge conductance remains rare, let alone that with significant correlations. In this work, we report a novel dual QSH insulator within the intrinsic monolayer crystal of TaIrTe4, arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe4 demonstrates the QSH insulator that aligns with single-particle band structure calculations, manifesting enhanced nonlocal transport and quantized helical edge conductance. Interestingly, upon introducing electrons from charge neutrality, TaIrTe4 only shows metallic behavior in a small range of charge densities but quickly goes into a new insulating state, entirely unexpected based on TaIrTe4's single-particle band structure. This insulating state could arise from a strong electronic instability near the van Hove singularities (VHS), likely leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state, marked by the revival of nonlocal transport and quantized helical edge conduction. Our observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands via CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism., Comment: 23 pages, 15 figures, submitted version

Topological materials are at the forefront of quantum materials research, offering tremendous potential for next-generation energy and information devices. However, current investigation of these materials remains largely focused on performance and often neglects the crucial aspect of sustainability. Recognizing the pivotal role of sustainability in addressing global pollution, carbon emissions, resource conservation, and ethical labor practices, we present a comprehensive evaluation of topological materials based on their sustainability and environmental impact. Our approach involves a hierarchical analysis encompassing cost, toxicity, energy demands, environmental impact, social implications, and resilience to imports. By applying this framework to over 16,000 topological materials, we establish a sustainable topological materials database. Our endeavor unveils environmental-friendly topological materials candidates which have been previously overlooked, providing insights into their environmental ramifications and feasibility for industrial scalability. The work represents a critical step toward industrial adoption of topological materials, offering the potential for significant technological advancements and broader societal benefits.

Diode effects are of great interest for both fundamental physics and modern technologies. Electrical diode effects (nonreciprocal transport) have been observed in Weyl systems. Optical diode effects arising from the Weyl fermions have been theoretically considered but not probed experimentally. Here, we report the observation of a nonlinear optical diode effect (NODE) in the magnetic Weyl semimetal CeAlSi, where the magnetization introduces a pronounced directionality in the nonlinear optical second-harmonic generation (SHG). We show demonstrate a six-fold change of the measured SHG intensity between opposite propagation directions over a bandwidth exceeding 250 meV. Supported by density-functional theory, we establish the linearly dispersive bands emerging from Weyl nodes as the origin of this broadband effect. We further demonstrate current-induced magnetization switching and thus electrical control of the NODE. Our results advance ongoing research to identify novel nonlinear optical/transport phenomena in magnetic topological materials and further opens new pathways for the unidirectional manipulation of light., Comment: 20 pages, 4 figures, SI included

Quantum geometry - the geometry of electron Bloch wavefunctions - is central to modern condensed matter physics. Due to the quantum nature, quantum geometry has two parts, the real part quantum metric and the imaginary part Berry curvature. The studies of Berry curvature have led to countless breakthroughs, ranging from the quantum Hall effect in 2DEGs to the anomalous Hall effect (AHE) in ferromagnets. However, in contrast to Berry curvature, the quantum metric has rarely been explored. Here, we report a new nonlinear Hall effect induced by quantum metric by interfacing even-layered MnBi2Te4 (a PT-symmetric antiferromagnet (AFM)) with black phosphorus. This novel nonlinear Hall effect switches direction upon reversing the AFM spins and exhibits distinct scaling that suggests a non-dissipative nature. Like the AHE brought Berry curvature under the spotlight, our results open the door to discovering quantum metric responses. Moreover, we demonstrate that the AFM can harvest wireless electromagnetic energy via the new nonlinear Hall effect, therefore enabling intriguing applications that bridges nonlinear electronics with AFM spintronics., Comment: 19 pages, 4 figures and a Supplementary Materials with 66 pages, 4 figures and 3 tables. Originally submitted to Science on Oct. 5, 2022

Electronic ferroelectricity represents a new paradigm where spontaneous symmetry breaking driven by electronic correlations, in contrast to traditional lattice-driven ferroelectricity, leads to the formation of electric dipoles. Despite the potential application advantages arising from its electronic nature, switchable electronic ferroelectricity remains exceedingly rare. Here, we report the discovery of an electronic ratchet effect that manifests itself as switchable electronic ferroelectricity in a layer-contrasting graphene-boron nitride moir\'e heterostructure. Our engineered layer-asymmetric moir\'e potential landscapes result in layer-polarized localized and itinerant electronic subsystems. At particular fillings of the localized subsystem, we find a ratcheting injection of itinerant carriers in a non-volatile manner, leading to a highly unusual ferroelectric response. Strikingly, the remnant polarization can be stabilized at multiple (quasi-continuous) states with behavior markedly distinct from known ferroelectrics. Our experimental observations, simulations, and theoretical analysis suggest that dipolar excitons are the driving force and elementary ferroelectric units in our system. This signifies a new type of electronic ferroelectricity where the formation of dipolar excitons with aligned moments generates a macroscopic polarization and leads to an electronically-driven ferroelectric response, which we term excitonic ferroelectricity. Such new ferroelectrics, driven by quantum objects like dipolar excitons, could pave the way to innovative quantum analog memory and synaptic devices.

Using circularly-polarized light to control quantum matter is a highly intriguing topic in physics, chemistry and biology. Previous studies have demonstrated helicity-dependent optical control of spatial chirality and magnetization $M$. The former is central for asymmetric synthesis in chemistry and homochirality in bio-molecules, while the latter is of great interest for ferromagnetic spintronics. In this paper, we report the surprising observation of helicity-dependent optical control of fully-compensated antiferromagnetic (AFM) order in 2D even-layered MnBi$_2$Te$_4$, a topological Axion insulator with neither chirality nor $M$. We further demonstrate helicity-dependent optical creation of AFM domain walls by double induction beams and the direct reversal of AFM domains by ultrafast pulses. The control and reversal of AFM domains and domain walls by light helicity have never been achieved in any fully-compensated AFM. To understand this optical control, we study a novel type of circular dichroism (CD) proportional to the AFM order, which only appears in reflection but is absent in transmission. We show that the optical control and CD both arise from the optical Axion electrodynamics, which can be visualized as a Berry curvature real space dipole. Our Axion induction provides the possibility to optically control a family of $\mathcal{PT}$-symmetric AFMs such as Cr$_2$O$_3$, CrI$_3$ and possibly novel states in cuprates. In MnBi$_2$Te$_4$, this further opens the door for optical writing of dissipationless circuit formed by topological edge states.

The bulk-boundary correspondence is a key concept in topological quantum materials. For instance, a quantum spin Hall insulator features a bulk insulating gap with gapless helical boundary states protected by the underlying Z2 topology. However, the bulk-boundary dichotomy and distinction are rarely explored in optical experiments, which can provide unique information about topological charge carriers beyond transport and electronic spectroscopy techniques. Here, we utilize mid-infrared absorption micro-spectroscopy and pump-probe micro-spectroscopy to elucidate the bulk-boundary optical responses of Bi4Br4, a recently discovered room-temperature quantum spin Hall insulator. Benefiting from the low energy of infrared photons and the high spatial resolution, we unambiguously resolve a strong absorption from the boundary states while the bulk absorption is suppressed by its insulating gap. Moreover, the boundary absorption exhibits a strong polarization anisotropy, consistent with the one-dimensional nature of the topological boundary states. Our infrared pump-probe microscopy further measures a substantially increased carrier lifetime for the boundary states, which reaches one nanosecond scale. The nanosecond lifetime is about one to two orders longer than that of most topological materials and can be attributed to the linear dispersion nature of the helical boundary states. Our findings demonstrate the optical bulk-boundary dichotomy in a topological material and provide a proof-of-principal methodology for studying topological optoelectronics., Comment: 26 pages, 4 figures

Nonlinear optical responses of quantum materials have recently undergone dramatic developments to unveil nontrivial geometry and topology. A remarkable example is the quantized longitudinal circular photogalvanic effect (CPGE) associated with the Chern number of Weyl fermions, while the physics of transverse CPGE in Weyl semimetals remains exclusive. Here, we show that the transverse CPGE of Lorentz invariant Weyl fermions is forced to be zero. We find that the transverse photocurrents of Weyl fermions are associated not only with the Chern numbers but also with the degree of Lorentz-symmetry breaking in condensed matter systems. Based on the generic two-band model analysis, we provide a new powerful equation to calculate the transverse CPGE based on the tilting and warping terms of Weyl fermions. Our results are more capable in designing large transverse CPGE of Weyl semimetals in experiments and are applied to more than tens of Weyl materials to estimate their photocurrents. Our method paves the way to study the CPGE of massless or massive quasiparticles to design next-generation quantum optoelectronics.

The photoexcitation life-cycle from incident photon (and creation of photoexcited electron hole pair) to ultimate extraction of electrical current is a complex multi-physics process spanning across a range of spatio-temporal scales of quantum materials. While often viewed through a device-technology lens, photocurrent is a key observable of the life-cycle that is sensitive to a myriad of physical processes across these scales. As a result, photocurrent is emerging as a versatile probe of electronic states, Bloch band quantum geometry, quantum kinetic processes, and device characteristics of quantum materials. This review outlines the key multi-physics principles of photocurrent diagnostics. In particular, we describe how the fundamental link between light-matter interaction and quantum geometry renders photocurrent a wavefunction-sensitive probe capable of resolving bandstructure and characterizing topological materials. We further highlight the sensitivity of the photoexcitation life-cycle to relaxational processes which in turn enables photocurrent to disentangle distinct types of carrier scattering that can range from femtosecond to nanosecond timescales. We survey the intrinsically nonlocal character of photocurrent collection that allows new types remote sensing protocols and photocurrent nanoscopy. These distinctive features underscore photocurrent diagnostics as a novel multi-physics probe for a growing class of quantum materials with properties governed by physics spanning multiple spatio-temporal scales., Comment: original submitted version

The recently observed unconventional ferroelectricity in AB bilayer graphene sandwiched by hexagonal Boron Nitride (hBN) presents a new platform to manipulate correlated phases in multilayered van der Waals heterostructures. We present a low-energy continuum model for AB bilayer graphene encapsulated by the top and bottom layers of either hBN or graphene, with two independent twist angles. For the graphene/hBN heterostructures, we show that twist angle asymmetry leads to a layer polarization of the valence and conduction bands. We also show that an out-of-plane displacement field not only tunes the layer polarization but also flattens the low-energy bands. We extend the model to show that the electronic structures of quadrilayer graphene heterostructure consisting of AB bilayer graphene encapsulated by the top and bottom graphene layers can similarly be tuned by an external electric field.

Emergent phenomena arising from the collective behavior of electrons is generally expected when Coulomb interactions dominate over the kinetic energy, as in delocalized quasiparticles in highly degenerate flat bands. Bernal-stacked bilayer graphene intrinsically supports a pair of flat bands predicted to host a variety of spontaneous broken-symmetry states arising from van Hove singularities and a four-fold spin-valley (isospin) degeneracy. Here, we show that ultra-clean samples of bilayer graphene display a cascade of symmetry-broken states with spontaneous and spin and valley ordering at zero magnetic field. Using capacitive sensing in a dual-gated geometry, we tune the carrier density and electric displacement field independently to explore the phase space of transitions and probe the character of the isospin order. Itinerant ferromagnetic states emerge near the conduction and valence band edges with complete spin and valley polarization and a high degree of displacement field tunability. At larger hole densities, two-fold degenerate quantum oscillations manifest in an additional broken symmetry state that is enhanced by the application of an in-plane magnetic field. Both types of symmetry-broken states display enhanced layer polarization at low temperatures, suggesting a coupling to the layer pseudospin degree of freedom in the electronic wavefunctions. Notably, the zero-field spontaneous symmetry breaking reported here emerges in the absence of a moir\'e superlattice and is intrinsic to natural graphene bilayers. Thus, we demonstrate that the tunable bands of bilayer graphene represent a related, but distinct approach to produce flat band collective behavior, complementary to engineered moir\'e structures.

While ferromagnets have been known and exploited for millennia, antiferromagnets (AFMs) were only discovered in the 1930s. The elusive nature indicates AFMs' unique properties: At large scale, due to the absence of global magnetization, AFMs may appear to behave like any non-magnetic material; However, such a seemingly mundane macroscopic magnetic property is highly nontrivial at microscopic level, where opposite spin alignment within the AFM unit cell forms a rich internal structure. In topological AFMs, such an internal structure leads to a new possibility, where topology and Berry phase can acquire distinct spatial textures. Here, we study this exciting possibility in an AFM Axion insulator, even-layered MnBi$_2$Te$_4$ flakes, where spatial degrees of freedom correspond to different layers. Remarkably, we report the observation of a new type of Hall effect, the layer Hall effect, where electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under no net electric field, even-layered MnBi$_2$Te$_4$ shows no anomalous Hall effect (AHE); However, applying an electric field isolates the response from one layer and leads to the surprising emergence of a large layer-polarized AHE (~50%$\frac{e^2}{h}$). Such a layer Hall effect uncovers a highly rare layer-locked Berry curvature, which serves as a unique character of the space-time $\mathcal{PT}$-symmetric AFM topological insulator state. Moreover, we found that the layer-locked Berry curvature can be manipulated by the Axion field, E$\cdot$B, which drives the system between the opposite AFM states. Our results achieve previously unavailable pathways to detect and manipulate the rich internal spatial structure of fully-compensated topological AFMs. The layer-locked Berry curvature represents a first step towards spatial engineering of Berry phase, such as through layer-specific moir\'e potential., Comment: A revised version of this article is published in Nature

For many materials, a precise knowledge of their dispersion spectra is insufficient to predict their ordered phases and physical responses. Instead, these materials are classified by the geometrical and topological properties of their wavefunctions. A key challenge is to identify and implement experiments that probe or control these quantum properties. In this review, we describe recent progress in this direction, focusing on nonlinear electromagnetic responses that arise directly from quantum geometry and topology. We give an overview of the field by discussing new theoretical ideas, groundbreaking experiments, and the novel materials that drive them. We conclude by discussing how these techniques can be combined with new device architectures to uncover, probe, and ultimately control novel quantum phases with emergent topological and correlated properties., Comment: Nature Materials (In Press)

The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels. Examples range from parity violation in the subatomic weak force to the homochirality in essential biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order, where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal $1T$-TiSe$_2$. We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe$_2$. Such chiral induction provides a new way of optical control over novel orders in quantum materials., Comment: 22 pages, 5 figures

Advanced microscopy and/or spectroscopy tools play indispensable role in nanoscience and nanotechnology research, as it provides rich information about the growth mechanism, chemical compositions, crystallography, and other important physical and chemical properties. However, the interpretation of imaging data heavily relies on the "intuition" of experienced researchers. As a result, many of the deep graphical features obtained through these tools are often unused because of difficulties in processing the data and finding the correlations. Such challenges can be well addressed by deep learning. In this work, we use the optical characterization of two-dimensional (2D) materials as a case study, and demonstrate a neural-network-based algorithm for the material and thickness identification of exfoliated 2D materials with high prediction accuracy and real-time processing capability. Further analysis shows that the trained network can extract deep graphical features such as contrast, color, edges, shapes, segment sizes and their distributions, based on which we develop an ensemble approach topredict the most relevant physical properties of 2D materials. Finally, a transfer learning technique is applied to adapt the pretrained network to other applications such as identifying layer numbers of a new 2D material, or materials produced by a different synthetic approach. Our artificial-intelligence-based material characterization approach is a powerful tool that would speed up the preparation, initial characterization of 2D materials and other nanomaterials and potentially accelerate new material discoveries.

Recent theoretical advances have proposed a new class of topological crystalline insulator (TCI) phases protected by rotational symmetries. Distinct from topological insulators (TIs), rotational symmetry-protected TCIs are expected to show unique topologically protected boundary modes: First, the surface normal to the rotational axis features unpinned Dirac surface states whose Dirac points are located at generic k points. Second, due to the higher-order bulk boundary correspondence, a 3D TCI also supports 1D helical edge states. Despite the unique topological electronic properties, to date, purely rotational symmetry-protected TCIs remain elusive in real materials. Using first-principles band calculations and theoretical modeling, we identify the van der Waals material $\alpha$-Bi4Br4 as a TCI purely protected by rotation symmetry. We show that the Bi4Br4's (010) surface exhibits a pair of unpinned topological Dirac fermions protected by the two-fold rotational axis. These unpinned Dirac fermions show an exotic spin texture highly favorable for spin transport and a band structure consisting of van Hove singularities due to Lifshitz transition. We also identify 1D topological hinge states along the edges of an $\alpha$-Bi4Br4 rod. We further discuss how the proposed topological electronic properties in $\alpha$-Bi4Br4 can be observed by various experimental techniques.

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

Graphene is a new material showing high promise in optoelectronics, photonics, and energy-harvesting applications. However, the underlying physical mechanism of optoelectronic response has not been established. Here, we report on the intrinsic optoelectronic response of high-quality dual-gated monolayer and bilayer graphene p-n junction devices. Local laser excitation at the p-n interface leads to striking six-fold photovoltage patterns as a function of bottom- and top-gate voltages. These patterns, together with the measured spatial and density dependence of the photoresponse, provide strong evidence that non-local hot-carrier transport, rather than the photovoltaic effect, dominates the intrinsic photoresponse in graphene. This novel regime, which features a long-lived and spatially distributed hot carrier population, may open the doorway for optoelectronic technologies exploiting efficient energy transport at the nanoscale., Comment: 19 pages, 4 figures

We study the conductance spectrum of graphene quantum dots, both single and multiple cases. The single electron tunneling phenomenon is investigated and the periodicity, amplitude and line shape of the Coulomb blockade oscillations at low temperatures are obtained. Further, we discuss the transport behavior when multiple dots are assembled in array and find a phase transition of conductance spectra from individual Coulomb blockade to collective Coulomb blockade., Comment: 7 pages, 6 figures

We propose a new method to use gapped graphene as barrier to confine electrons in gapless graphene and form a good quantum dot, which can be realized on an oxygen-terminated $SiO_{2}$ substrate partly H-passivated. In particular, we use ferromagnetic insulators deposited on top of barrier which give rise to a spin related energy spectrum and transport properties. Compared to the complexity of etched quantum dots in graphene, the setup suggested here is a promising candidate for practical applications.