Correlated insulator and Chern insulators in pentalayer rhombohedral-stacked graphene.

Rhombohedral-stacked multilayer graphene hosts a pair of flat bands touching at zero energy, which should give rise to correlated electron phenomena that can be tuned further by an electric field. Moreover, when electron correlation breaks the isospin symmetry, the valley-dependent Berry phase at zero energy may give rise to topologically non-trivial states. Here we measure electron transport through hexagonal boron nitride-encapsulated pentalayer graphene down to 100 mK. We observed a correlated insulating state with resistance at the megaohm level or greater at charge density n = 0 and displacement field D = 0. Tight-binding calculations predict a metallic ground state under these conditions. By increasing D, we observed a Chern insulator state with C = -5 and two other states with C = -3 at a magnetic field of around 1 T. At high D and n, we observed isospin-polarized quarter- and half-metals. Hence, rhombohedral pentalayer graphene exhibits two different types of Fermi-surface instability, one driven by a pair of flat bands touching at zero energy, and one induced by the Stoner mechanism in a single flat band. Our results establish rhombohedral multilayer graphene as a suitable system for exploring intertwined electron correlation and topology phenomena in natural graphitic materials without the need for moiré superlattice engineering.

Robust Higher-Order Hamiltonian Engineering for Quantum Sensing with Strongly Interacting Systems.

Dynamical decoupling techniques constitute an integral part of many quantum sensing platforms, often leading to orders-of-magnitude improvements in coherence time and sensitivity. Most ac sensing sequences involve a periodic echolike structure, in which the target signal is synchronized with the echo period. We show that for strongly interacting systems, this construction leads to a fundamental sensitivity limit associated with imperfect interaction decoupling. We present a simple physical picture demonstrating the origin of this limitation, and further formalize these considerations in terms of concise higher-order decoupling rules. We then show how these limitations can be surpassed by identifying a novel sequence building block, in which the signal period matches twice the echo period. Using these decoupling rules and the resulting sequence building block, we experimentally demonstrate significant improvements in dynamical decoupling timescales and magnetic field sensitivity, opening the door for new applications in quantum sensing and quantum many-body physics.

A semiconductor 96-microplate platform for electrical-imaging based high-throughput phenotypic screening.

High-content imaging for compound and genetic profiling is popular for drug discovery but limited to endpoint images of fixed cells. Conversely, electronic-based devices offer label-free, live cell functional information but suffer from limited spatial resolution or throughput. Here, we introduce a semiconductor 96-microplate platform for high-resolution, real-time impedance imaging. Each well features 4096 electrodes at 25 µm spatial resolution and a miniaturized data interface allows 8× parallel plate operation (768 total wells) for increased throughput. Electric field impedance measurements capture >20 parameter images including cell barrier, attachment, flatness, and motility every 15 min during experiments. We apply this technology to characterize 16 cell types, from primary epithelial to suspension cells, and quantify heterogeneity in mixed co-cultures. Screening 904 compounds across 13 semiconductor microplates reveals 25 distinct responses, demonstrating the platform's potential for mechanism of action profiling. The scalability and translatability of this semiconductor platform expands high-throughput mechanism of action profiling and phenotypic drug discovery applications.

Orbital multiferroicity in pentalayer rhombohedral graphene.

Ferroic orders describe spontaneous polarization of spin, charge and lattice degrees of freedom in materials. Materials exhibiting multiple ferroic orders, known as multiferroics, have important parts in multifunctional electrical and magnetic device applications1-4. Two-dimensional materials with honeycomb lattices offer opportunities to engineer unconventional multiferroicity, in which the ferroic orders are driven purely by the orbital degrees of freedom and not by electron spin. These include ferro-valleytricity corresponding to the electron valley5 and ferro-orbital-magnetism6 supported by quantum geometric effects. These orbital multiferroics could offer strong valley-magnetic couplings and large responses to external fields-enabling device applications such as multiple-state memory elements and electric control of the valley and magnetic states. Here we report orbital multiferroicity in pentalayer rhombohedral graphene using low-temperature magneto-transport measurements. We observed anomalous Hall signals Rxy with an exceptionally large Hall angle (tanΘH > 0.6) and orbital magnetic hysteresis at hole doping. There are four such states with different valley polarizations and orbital magnetizations, forming a valley-magnetic quartet. By sweeping the gate electric field E, we observed a butterfly-shaped hysteresis of Rxy connecting the quartet. This hysteresis indicates a ferro-valleytronic order that couples to the composite field E · B (where B is the magnetic field), but not to the individual fields. Tuning E would switch each ferroic order independently and achieve non-volatile switching of them together. Our observations demonstrate a previously unknown type of multiferroics and point to electrically tunable ultralow-power valleytronic and magnetic devices.

Quantum Logic Enhanced Sensing in Solid-State Spin Ensembles.

We demonstrate quantum logic enhanced sensitivity for a macroscopic ensemble of solid-state, hybrid two-qubit sensors. We achieve over a factor of 30 improvement in the single-shot signal-to-noise ratio, translating to an ac magnetic field sensitivity enhancement exceeding an order of magnitude for time-averaged measurements. Using the electronic spins of nitrogen vacancy (NV) centers in diamond as sensors, we leverage the on-site nitrogen nuclear spins of the NV centers as memory qubits, in combination with homogeneous and stable bias and control fields, ensuring that all of the ∼10^{9} two-qubit sensors are sufficiently identical to permit global control of the NV ensemble spin states. We find quantum logic sensitivity enhancement for multiple measurement protocols with varying optimal sensing intervals, including XY8 and DROID-60 dynamical decoupling, as well as correlation spectroscopy, using an applied ac magnetic field signal. The results are independent of the nature of the target signal and broadly applicable to measurements using NV centers and other solid-state spin ensembles. This work provides a benchmark for macroscopic ensembles of quantum sensors that employ quantum logic or quantum error correction algorithms for enhanced sensitivity.

An Inverse-Designed Nanophotonic Interface for Excitons in Atomically Thin Materials.

Efficient nanophotonic devices are essential for applications in quantum networking, optical information processing, sensing, and nonlinear optics. Extensive research efforts have focused on integrating two-dimensional (2D) materials into photonic structures, but this integration is often limited by size and material quality. Here, we use hexagonal boron nitride (hBN), a benchmark choice for encapsulating atomically thin materials, as a waveguiding layer while simultaneously improving the optical quality of the embedded films. When combined with a photonic inverse design, it becomes a complete nanophotonic platform to interface with optically active 2D materials. Grating couplers and low-loss waveguides provide optical interfacing and routing, tunable cavities provide a large exciton-photon coupling to transition metal dichalcogenide (TMD) monolayers through Purcell enhancement, and metasurfaces enable the efficient detection of TMD dark excitons. This work paves the way for advanced 2D-material nanophotonic structures for classical and quantum nonlinear optics.

Controlling Local Thermalization Dynamics in a Floquet-Engineered Dipolar Ensemble.

Understanding the microscopic mechanisms of thermalization in closed quantum systems is among the key challenges in modern quantum many-body physics. We demonstrate a method to probe local thermalization in a large-scale many-body system by exploiting its inherent disorder and use this to uncover the thermalization mechanisms in a three-dimensional, dipolar-interacting spin system with tunable interactions. Utilizing advanced Hamiltonian engineering techniques to explore a range of spin Hamiltonians, we observe a striking change in the characteristic shape and timescale of local correlation decay as we vary the engineered exchange anisotropy. We show that these observations originate from the system's intrinsic many-body dynamics and reveal the signatures of conservation laws within localized clusters of spins, which do not readily manifest using global probes. Our method provides an exquisite lens into the tunable nature of local thermalization dynamics and enables detailed studies of scrambling, thermalization, and hydrodynamics in strongly interacting quantum systems.

A semiconductor 96-microplate platform for electrical-imaging based high-throughput phenotypic screening.

Profiling compounds and genetic perturbations via high-content imaging has become increasingly popular for drug discovery, but the technique is limited to endpoint images of fixed cells. In contrast, electronic-based devices offer label-free, functional information of live cells, yet current approaches suffer from low-spatial resolution or single-well throughput. Here, we report a semiconductor 96-microplate platform designed for high-resolution real-time impedance "imaging" at scale. Each well features 4,096 electrodes at 25 µm spatial resolution while a miniaturized data interface allows 8× parallel plate operation (768 total wells) within each incubator for enhanced throughputs. New electric field-based, multi-frequency measurement techniques capture >20 parameter images including tissue barrier, cell-surface attachment, cell flatness, and motility every 15 min throughout experiments. Using these real-time readouts, we characterized 16 cell types, ranging from primary epithelial to suspension, and quantified heterogeneity in mixed epithelial and mesenchymal co-cultures. A proof-of-concept screen of 904 diverse compounds using 13 semiconductor microplates demonstrates the platform's capability for mechanism of action (MOA) profiling with 25 distinct responses identified. The scalability of the semiconductor platform combined with the translatability of the high dimensional live-cell functional parameters expands high-throughput MOA profiling and phenotypic drug discovery applications.

Operando electron microscopy investigation of polar domain dynamics in twisted van der Waals homobilayers.

Conventional antiferroelectric materials with atomic-scale anti-aligned dipoles undergo a transition to a ferroelectric (FE) phase under strong electric fields. The moiré superlattice formed in the twisted stacks of van der Waals crystals exhibits polar domains alternating in moiré length with anti-aligned dipoles. In this moiré domain antiferroelectic (MDAF) arrangement, the distribution of electric dipoles is distinguished from that of two-dimensional FEs, suggesting dissimilar domain dynamics. Here we performed an operando transmission electron microscopy investigation on twisted bilayer WSe2 to observe the polar domain dynamics in real time. We find that the topological protection, provided by the domain wall network, prevents the MDAF-to-FE transition. As one decreases the twist angle, however, this transition occurs as the domain wall network disappears. Exploiting stroboscopic operando transmission electron microscopy on the FE phase, we measure a maximum domain wall velocity of 300 µm s-1. Domain wall pinnings by various disorders limit the domain wall velocity and cause Barkhausen noises in the polarization hysteresis loop. Atomic-scale analysis of the pinning disorders provides structural insight on how to improve the switching speed of van der Waals FEs.

Quantum sensors for biomedical applications.

Quantum sensors are finding their way from laboratories to the real world, as witnessed by the increasing number of start-ups in this field. The atomic length scale of quantum sensors and their coherence properties enable unprecedented spatial resolution and sensitivity. Biomedical applications could benefit from these quantum technologies, but it is often difficult to evaluate the potential impact of the techniques. This Review sheds light on these questions, presenting the status of quantum sensing applications and discussing their path towards commercialization. The focus is on two promising quantum sensing platforms: optically pumped atomic magnetometers, and nitrogen-vacancy centres in diamond. The broad spectrum of biomedical applications is highlighted by four case studies ranging from brain imaging to single-cell spectroscopy.

Electrically switchable anisotropic polariton propagation in a ferroelectric van der Waals semiconductor.

Tailoring of the propagation dynamics of exciton-polaritons in two-dimensional quantum materials has shown extraordinary promise to enable nanoscale control of electromagnetic fields. Varying permittivities along crystal directions within layers of material systems, can lead to an in-plane anisotropic dispersion of polaritons. Exploiting this physics as a control strategy for manipulating the directional propagation of the polaritons is desired and remains elusive. Here we explore the in-plane anisotropic exciton-polariton propagation in SnSe, a group-IV monochalcogenide semiconductor that forms ferroelectric domains and shows room-temperature excitonic behaviour. Exciton-polaritons are launched in SnSe multilayer plates, and their propagation dynamics and dispersion are studied. This propagation of exciton-polaritons allows for nanoscale imaging of the in-plane ferroelectric domains. Finally, we demonstrate the electric switching of the exciton-polaritons in the ferroelectric domains of this complex van der Waals system. The study suggests that systems such as group-IV monochalcogenides could serve as excellent ferroic platforms for actively reconfigurable polaritonic optical devices.

Modulation Doping of Single-Layer Semiconductors for Improved Contact at Metal Interfaces.

Single layers of two-dimensional (2D) materials hold the promise for further miniaturization of semiconductor electronic devices. However, the metal-semiconductor contact resistance limits device performance. To mitigate this problem, we propose modulation doping, specifically a doping layer placed on the opposite side of a metal-semiconductor interface. Using first-principles calculations to obtain the band alignment, we show that the Schottky barrier height and, consequently, the contact resistance at the metal-semiconductor interface can be reduced by modulation doping. We demonstrate the feasibility of this approach for a single-layer tungsten diselenide (WSe2) channel and 2D MXene modulation doping layers, interfaced with several different metal contacts. Our results indicate that the Fermi level of the metal can be shifted across the entire band gap. This approach can be straight-forwardly generalized for other 2D semiconductors and a wide variety of doping layers.

CMOS electrochemical pH localizer-imager.

pH controls a large repertoire of chemical and biochemical processes in water. Densely arrayed pH microenvironments would parallelize these processes, enabling their high-throughput studies and applications. However, pH localization, let alone its arrayed realization, remains challenging because of fast diffusion of protons in water. Here, we demonstrate arrayed localizations of picoliter-scale aqueous acids, using a 256-electrochemical cell array defined on and operated by a complementary metal oxide semiconductor (CMOS)-integrated circuit. Each cell, comprising a concentric pair of cathode and anode with their current injections controlled with a sub-nanoampere resolution by the CMOS electronics, creates a local pH environment, or a pH "voxel," via confined electrochemistry. The system also monitors the spatiotemporal pH profile across the array in real time for precision pH control. We highlight the utility of this CMOS pH localizer-imager for high-throughput tasks by parallelizing pH-gated molecular state encoding and pH-regulated enzymatic DNA elongation at any selected set of cells.

Beam steering at the nanosecond time scale with an atomically thin reflector.

Techniques to mold the flow of light on subwavelength scales enable fundamentally new optical systems and device applications. The realization of programmable, active optical systems with fast, tunable components is among the outstanding challenges in the field. Here, we experimentally demonstrate a few-pixel beam steering device based on electrostatic gate control of excitons in an atomically thin semiconductor with strong light-matter interactions. By combining the high reflectivity of a MoSe2 monolayer with a graphene split-gate geometry, we shape the wavefront phase profile to achieve continuously tunable beam deflection with a range of 10°, two-dimensional beam steering, and switching times down to 1.6 nanoseconds. Our approach opens the door for a new class of atomically thin optical systems, such as rapidly switchable beam arrays and quantum metasurfaces operating at their fundamental thickness limit.

Multi-parametric functional imaging of cell cultures and tissues with a CMOS microelectrode array.

Electrode-based impedance and electrochemical measurements can provide cell-biology information that is difficult to obtain using optical-microscopy techniques. Such electrical methods are non-invasive, label-free, and continuous, eliminating the need for fluorescence reporters and overcoming optical imaging's throughput/temporal resolution limitations. Nonetheless, electrode-based techniques have not been heavily employed because devices typically contain few electrodes per well, resulting in noisy aggregate readouts. Complementary metal-oxide-semiconductor (CMOS) microelectrode arrays (MEAs) have sometimes been used for electrophysiological measurements with thousands of electrodes per well at sub-cellular pitches, but only basic impedance mappings of cell attachment have been performed outside of electrophysiology. Here, we report on new field-based impedance mapping and electrochemical mapping/patterning techniques to expand CMOS-MEA cell-biology applications. The methods enable accurate measurement of cell attachment, growth/wound healing, cell-cell adhesion, metabolic state, and redox properties with single-cell spatial resolution (20 µm electrode pitch). These measurements allow the quantification of adhesion and metabolic differences of cells expressing oncogenes versus wild-type controls. The multi-parametric, cell-population statistics captured by the chip-scale integrated device opens up new avenues for fully electronic high-throughput live-cell assays for phenotypic screening and drug discovery applications.

Probing dark exciton navigation through a local strain landscape in a WSe2 monolayer.

In WSe2 monolayers, strain has been used to control the energy of excitons, induce funneling, and realize single-photon sources. Here, we developed a technique for probing the dynamics of free excitons in nanoscale strain landscapes in such monolayers. A nanosculpted tapered optical fiber is used to simultaneously generate strain and probe the near-field optical response of WSe2 monolayers at 5 K. When the monolayer is pushed by the fiber, its lowest energy states shift by as much as 390 meV (>20% of the bandgap of a WSe2 monolayer). Polarization and lifetime measurements of these red-shifting peaks indicate they originate from dark excitons. We conclude free dark excitons are funneled to high-strain regions during their long lifetime and are the principal participants in drift and diffusion at cryogenic temperatures. This insight supports proposals on the origin of single-photon sources in WSe2 and demonstrates a route towards exciton traps for exciton condensation.

Bilayer Wigner crystals in a transition metal dichalcogenide heterostructure.

One of the first theoretically predicted manifestations of strong interactions in many-electron systems was the Wigner crystal1-3, in which electrons crystallize into a regular lattice. The crystal can melt via either thermal or quantum fluctuations4. Quantum melting of the Wigner crystal is predicted to produce exotic intermediate phases5,6 and quantum magnetism7,8 because of the intricate interplay of Coulomb interactions and kinetic energy. However, studying two-dimensional Wigner crystals in the quantum regime has often required a strong magnetic field9-11 or a moiré superlattice potential12-15, thus limiting access to the full phase diagram of the interacting electron liquid. Here we report the observation of bilayer Wigner crystals without magnetic fields or moiré potentials in an atomically thin transition metal dichalcogenide heterostructure, which consists of two MoSe2 monolayers separated by hexagonal boron nitride. We observe optical signatures of robust correlated insulating states at symmetric (1:1) and asymmetric (3:1, 4:1 and 7:1) electron doping of the two MoSe2 layers at cryogenic temperatures. We attribute these features to bilayer Wigner crystals composed of two interlocked commensurate triangular electron lattices, stabilized by inter-layer interaction16. The Wigner crystal phases are remarkably stable, and undergo quantum and thermal melting transitions at electron densities of up to 6 × 1012 per square centimetre and at temperatures of up to about 40 kelvin. Our results demonstrate that an atomically thin heterostructure is a highly tunable platform for realizing many-body electronic states and probing their liquid-solid and magnetic quantum phase transitions4-8,17.

Excitons in a reconstructed moiré potential in twisted WSe2/WSe2 homobilayers.

Moiré superlattices in twisted van der Waals materials have recently emerged as a promising platform for engineering electronic and optical properties. A major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate direct imaging of the moiré structure with optical and electronic properties. Here we develop a secondary electron microscope technique to directly image stacking domains in fully functional van der Waals heterostructure devices. After demonstrating the imaging of AB/BA and ABA/ABC domains in multilayer graphene, we employ this technique to investigate reconstructed moiré patterns in twisted WSe2/WSe2 bilayers and directly correlate the increasing moiré periodicity with the emergence of two distinct exciton species in photoluminescence measurements. These states can be tuned individually through electrostatic gating and feature different valley coherence properties. We attribute our observations to the formation of an array of two intralayer exciton species that reside in alternating locations in the superlattice, and open up new avenues to realize tunable exciton arrays in twisted van der Waals heterostructures, with applications in quantum optoelectronics and explorations of novel many-body systems.

Extracellular recording of direct synaptic signals with a CMOS-nanoelectrode array.

The synaptic connections between neurons are traditionally determined by correlating the action potentials (APs) of a pre-synaptic neuron and small-amplitude subthreshold potentials of a post-synaptic neuron using invasive intracellular techniques, such as patch clamping. Extracellular recording by a microelectrode array can non-invasively monitor network activities of a large number of neurons, but its reduced sensitivity usually prevents direct measurements of synaptic signals. Here, we demonstrate that a newly developed complementary metal-oxide-semiconductor (CMOS) nanoelectrode array (CNEA) is capable of extracellularly determining direct synaptic connections in dense, multi-layer cultures of dissociated rat neurons. We spatiotemporally correlate action potential signals of hundreds of active neurons, detect small (∼1 pA after averaging) extracellular synaptic signals at the region where pre-synaptic axons and post-synaptic dendrites/somas overlap, and use those signals to map synaptic connections. We use controlled stimulation to assess stimulation-dependent synaptic strengths and to titrate a synaptic blocker (CNQX: IC50 ∼ 1 µM). The new capabilities demonstrated here significantly enhance the utilities of CNEAs in connectome mapping and drug screening applications.

Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe2/MoSe2 bilayers.

Van der Waals heterostructures obtained via stacking and twisting have been used to create moiré superlattices1, enabling new optical and electronic properties in solid-state systems. Moiré lattices in twisted bilayers of transition metal dichalcogenides (TMDs) result in exciton trapping2-5, host Mott insulating and superconducting states6 and act as unique Hubbard systems7-9 whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures feature atomic reconstruction and domain formation10-14. However, due to the nanoscale size of moiré domains, the effects of atomic reconstruction on the electronic and excitonic properties have not been systematically investigated. Here we use near-0°-twist-angle MoSe2/MoSe2 bilayers with large rhombohedral AB/BA domains15 to directly probe the excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane electric dipole moments in opposite directions. The dipole orientation of ground-state Γ-K interlayer excitons can be flipped with electric fields, while higher-energy K-K interlayer excitons undergo field-asymmetric hybridization with intralayer K-K excitons. Our study reveals the impact of crystal symmetry on TMD excitons and points to new avenues for realizing topologically non-trivial systems16,17, exotic metasurfaces18, collective excitonic phases19 and quantum emitter arrays20,21 via domain-pattern engineering.