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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.

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., Just appeared in Science. 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 moiré heterostructure. Our engineered layer-asymmetric moiré 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.

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., original submitted version

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 $��$-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 $��$-Bi4Br4 rod. We further discuss how the proposed topological electronic properties in $��$-Bi4Br4 can be observed by various experimental techniques.

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

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., 19 pages, 3 figures

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., 30 pages, 4 figures, Accepted by Advanced Materials

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.

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

Ultrafast electron thermalization—the process leading to 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. Owing 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 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 means to probe and directly modulate electron energy transport in nanoscale materials, represent a step towards designing and implementing optoelectronic and energy-harvesting devices with tailored microscopic properties., United States. Air Force Office of Scientific Research (FA9550-11-1-0225), National Science Foundation (U.S.) (DMR-1231319)

Hexagonal boron nitride (h-BN) is a natural hyperbolic material, for which the dielectric constants are the same in the basal plane (epsilon^t = epsilon^x = epsilon^y) but have opposite signs (epsilon^t*epsilon^z < 0) from that in the normal plane (epsilon^z). Due to this property, finite-thickness slabs of h-BN act as multimode waveguides for propagation of hyperbolic phonon polaritons - collective modes that originate from the coupling between photons and electric dipoles in phonons. However, control of these hyperbolic phonon polaritons modes has remained challenging, mostly because their electrodynamic properties are dictated by the crystal lattice of h-BN. Here we show by direct nano-infrared imaging that these hyperbolic polaritons can be effectively modulated in a van der Waals heterostructure composed of monolayer graphene on h-BN. Tunability originates from the hybridization of surface plasmon polaritons in graphene with hyperbolic phonon polaritons in h-BN, so that the eigenmodes of the graphene/h-BN heterostructure are hyperbolic plasmon-phonon polaritons. Remarkably, the hyperbolic plasmon-phonon polaritons in graphene/h-BN suffer little from ohmic losses, making their propagation length 1.5-2.0 times greater than that of hyperbolic phonon polaritons in h-BN. The hyperbolic plasmon-phonon polaritons possess the combined virtues of surface plasmon polaritons in graphene and hyperbolic phonon polaritons in h-BN. Therefore, graphene/h-BN structures can be classified as electromagnetic metamaterials since the resulting properties of these devices are not present in its constituent elements alone., 20 pages, 3 figures in Nature Nanotechnology 2015

et al., Optoelectronic devices utilizing graphene have demonstrated unique capabilities and performances beyond state-of-the-art technologies. However, requirements in terms of device quality and uniformity are demanding. A major roadblock towards high-performance devices are nanoscale variations of the graphene device properties, impacting their macroscopic behaviour. Here we present and apply non-invasive optoelectronic nanoscopy to measure the optical and electronic properties of graphene devices locally. This is achieved by combining scanning near-field infrared nanoscopy with electrical read-out, allowing infrared photocurrent mapping at length scales of tens of nanometres. Using this technique, we study the impact of edges and grain boundaries on the spatial carrier density profiles and local thermoelectric properties. Moreover, we show that the technique can readily be applied to encapsulated graphene devices. We observe charge build-up near the edges and demonstrate a solution to this issue., F.H.L.K. acknowledges financial support from the Spanish Ministry of Economy and Competitiveness, through the ‘Severo Ochoa’ Programme for Centres of Excellence in R&D (SEV-2015-0522), support by Fundacio Cellex Barcelona, the ERC Career integration grant (294056, GRANOP), the ERC starting grant (307806, CarbonLight), the Government of Catalonia trough the SGR grant (2014-SGR-1535), the Mineco grants Ramón y Cajal (RYC-2012-12281) and Plan Nacional (FIS2013-47161-P), and project GRASP (FP7-ICT-2013-613024-GRASP). F.H.L.K. and R.H. acknowledge support by the E.C. (European Commission) under Graphene Flagship (contract no. CNECT-ICT604391). D.J. acknowledges support from the Ramón y Cajal Fellowship Program. Y.G. and J.H. acknowledge support from the US Office of Naval Research N00014-13-1-0662. We acknowledge financial support from the Spanish Ministry of Economy and Competitiveness and ‘Fondo Europeo de Desarrollo Regional’ through Grant TEC2013-46168-R. Q.M. and P.J.-H. have been supported by AFOSR Grant No. FA9550-11-1-0225 and the Packard Fellowship program. This work made use of the Materials Research Science and Engineering Center Shared Experimental Facilities supported by the National Science Foundation (NSF) (Grant No. DMR-0819762) and of Harvard’s Center for Nanoscale Systems, supported by the NSF (Grant No. ECS-0335765). S.R. acknowledges the Spanish Ministry of Economy and Competitiveness for funding (MAT2012-33911), the Secretaria de Universidades e Investigacion del Departamento de Economia y Conocimiento de la Generalidad de Catalunya and the Severo Ochoa Program (MINECO SEV-2013-0295). J.E.B.-V. acknowledges support from SECITI (Mexico, D.F.).

Uniaxial materials whose axial and tangential permittivities have opposite signs are referred to as indefinite or hyperbolic media. In such materials, light propagation is unusual leading to novel and often non-intuitive optical phenomena. Here we report infrared nano-imaging experiments demonstrating that crystals of hexagonal boron nitride, a natural mid-infrared hyperbolic material, can act as a ‘hyper-focusing lens’ and as a multi-mode waveguide. The lensing is manifested by subdiffractional focusing of phonon–polaritons launched by metallic disks underneath the hexagonal boron nitride crystal. The waveguiding is revealed through the modal analysis of the periodic patterns observed around such launchers and near the sample edges. Our work opens new opportunities for anisotropic layered insulators in infrared nanophotonics complementing and potentially surpassing concurrent artificial hyperbolic materials with lower losses and higher optical localization., United States. Air Force Office of Scientific Research (Grant FA9550-11-1-0225)

Photoexcitation of graphene leads to an interesting sequence of phenomena, some of which can be exploited in optoelectronic devices based on graphene. In particular, the efficient and ultrafast generation of an electron distribution with an elevated electron temperature and the concomitant generation of a photo-thermoelectric voltage at symmetry-breaking interfaces is of interest for photosensing and light harvesting. Here, we experimentally study the generated photocurrent at the graphene–metal interface, focusing on the time-resolved photocurrent, the effects of photon energy, Fermi energy and light polarization. We show that a single framework based on photo-thermoelectric photocurrent generation explains all experimental results., United States. Air Force Office of Scientific Research (Grant FA9550-11-1-0225), David & Lucile Packard Foundation (Fellowship)

Controlling the energy flow processes and the associated energy relaxation rates of a light emitter is of high fundamental interest, and has many applications in the fields of quantum optics, photovoltaics, photodetection, biosensing and light emission. While advanced dielectric and metallic systems have been developed to tailor the interaction between an emitter and its environment, active control of the energy flow has remained challenging. Here, we demonstrate in-situ electrical control of the relaxation pathways of excited erbium ions, which emit light at the technologically relevant telecommunication wavelength of 1.5 $\mu$m. By placing the erbium at a few nanometres distance from graphene, we modify the relaxation rate by more than a factor of three, and control whether the emitter decays into either electron-hole pairs, emitted photons or graphene near-infrared plasmons, confined to $, Comment: 9 pages, 4 figures