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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.