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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 (WSe

Reverse engineering the brain by mimicking the structure and function of neuronal networks on a silicon integrated circuit was the original goal of neuromorphic engineering, but remains a distant prospect. The focus of neuromorphic engineering has thus been relaxed from rigorous brain mimicry to designs inspired by qualitative features of the brain, including event-driven signalling and in-memory information processing. Here we examine current approaches to neuromorphic engineering and provide a vision that returns neuromorphic electronics to its original goal of reverse engineering the brain. The essence of this vision is to ‘copy’ the functional synaptic connectivity map of a mammalian neuronal network using advanced neuroscience tools and then ‘paste’ this map onto a high-density three-dimensional network of solid-state memories. Our copy-and-paste approach could potentially lead to silicon integrated circuits that better approximate computing traits of the brain, including low power, facile learning, adaptation, and even autonomy and cognition. This Perspective explores the potential of an approach to neuromorphic electronics in which the functional synaptic connectivity map of a mammalian neuronal network is copied using a silicon neuro-electronic interface and then pasted onto a high-density three-dimensional network of solid-state memories.

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.

Moire 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 moire 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 moire patterns in twisted WSe2/WSe2 bilayers and directly correlate the increasing moire 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. Scanning electron microscopy is used to image stacking domains in few-layer graphene, as well as moire patterns in twisted van der Waals heterostructures, allowing for the correlation of the local structure with their excitonic properties.

Transition metal dichalcogenide (TMD) semiconductor heterostructures are actively explored as a new platform for quantum optoelectronic systems. Most state of the art devices make use of insulating hexagonal boron nitride (hBN) that acts as a wide-bandgap dielectric encapsulating layer that also provides an atomically smooth and clean interface that is paramount for proper device operation. We report the observation of large, through-hBN photocurrents that are generated upon optical excitation of hBN encapsulated MoSe2 and WSe2 monolayer devices. We attribute these effects to Auger recombination in the TMDs, in combination with an asymmetric band offset between the TMD and the hBN. We present experimental investigation of these effects and compare our observations with detailed, ab-initio modeling. Our observations have important implications for the design of optoelectronic devices based on encapsulated TMD devices. In systems where precise charge-state control is desired, the out-of-plane current path presents both a challenge and an opportunity for optical doping control. Since the current directly depends on Auger recombination, it can act as a local, direct probe of both the efficiency of the Auger process as well as its dependence on the local density of states in integrated devices.

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

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., Comment: 6 pages, 4 figures main text

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.

The growth of single crystals of MoS2 and WS2 by materials transport through a liquid salt flux made from a low-melting mixture of NaCl and CsCl is presented. The crystals are structurally characte...

We realize a new electroplasmonic switch based upon electrically tunable exciton–plasmon interactions. The device consists of a hexagonal boron nitride (hBN)-encapsulated tungsten diselenide (WSe2)...

High-resolution sensing of weak signals is implemented by means of an integrated diamond---nuclear-magnetic-resonance technique

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 moire 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 moire 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. Optical signatures reveal correlated insulating Wigner crystals—electron solids—in a bilayer of a two-dimensional transition metal dichalcogenide, MoSe2, with hexagonal boron nitride between the layers.

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.

CMOS microelectrode arrays (MEAs) can record electrophysiological activities of a large number of neurons in parallel but only extracellularly with a low signal-to-noise ratio. Patch-clamp electrodes can perform intracellular recording with a high signal-to-noise ratio but only from a few neurons in parallel. Recently, we have developed and reported a neuroelectronic interface that combines the parallelism of the CMOS MEA and the intracellular sensitivity of the patch clamp. Here, we report the design and characterization of the CMOS integrated circuit (IC), a critical component of the neuroelectronic interface. Fabricated in 0.18- $\mu \text{m}$ technology, the IC features an array of 4096 platinum black (PtB) nanoelectrodes spaced at a 20- $\mu \text{m}$ pitch on its surface and contains 4096 active pixel circuits. Each active pixel circuit, consisting of a new switched-capacitor current injector—-capable of injecting from ±15 pA to ±0.7 $\mu \text{A}$ with a 5-pA resolution—-and an operational amplifier, is highly configurable. When configured into the current-clamp mode, the pixel intracellularly records membrane potentials, including subthreshold activities with ~23- $\mu \text{V}_{\mathrm {rms}}$ input-referred noise while injecting a current for simultaneous stimulation. When configured into the voltage-clamp mode, the pixel becomes a switched-capacitor transimpedance amplifier with ~1-pArms input-referred noise and intracellularly records ion channel currents while applying a voltage for simultaneous stimulation. Such voltage-/current-clamp intracellular recording/stimulation is a feat only previously possible with the patch-clamp method. At the same time, as an array, the IC overcomes the lack of parallelism of the patch-clamp method, measuring thousands of mammalian neurons in parallel, with full-frame intracellular recording/stimulation at 9.4 kHz.

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted ${\mathrm{WSe}}_{2}/{\mathrm{WSe}}_{2}$ bilayers exhibit a high ($g60%$) degree of circular polarization (DOCP) and long valley lifetimes ($g40\text{ }\text{ }\mathrm{ns}$) at zero electric and magnetic fields. The valley lifetime can be tuned by more than 3 orders of magnitude via electrostatic doping, enabling switching of the DOCP from $\ensuremath{\sim}80%$ in the $n$-doped regime to $l5%$ in the $p$-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom.

Developing a new tool capable of high-precision electrophysiological recording of a large network of electrogenic cells has long been an outstanding challenge in neurobiology and cardiology. Here, we combine nanoscale intracellular electrodes with complementary metal-oxide-semiconductor (CMOS) integrated circuits to realize a high-fidelity all-electrical electrophysiological imager for parallel intracellular recording at the network level. Our CMOS nanoelectrode array has 1,024 recording/stimulation 'pixels' equipped with vertical nanoelectrodes, and can simultaneously record intracellular membrane potentials from hundreds of connected in vitro neonatal rat ventricular cardiomyocytes. We demonstrate that this network-level intracellular recording capability can be used to examine the effect of pharmaceuticals on the delicate dynamics of a cardiomyocyte network, thus opening up new opportunities in tissue-based pharmacological screening for cardiac and neuronal diseases as well as fundamental studies of electrogenic cells and their networks.

Getting a sense of atomically thin materials Two-dimensional materials such as graphene and transition metal dichalcogenides provide a powerful platform for optoelectronic applications. As the materials get thinner, however, characterizing the electronic properties can present an experimental challenge. Lovchinsky et al. demonstrate that atomic-like impurities in diamond can be used to probe the properties of 2D materials by nanometer-scale nuclear quadrupole resonance spectroscopy. Coherent manipulation of shallow nitrogen-vacancy color centers enabled probing of nanoscale ensembles down to several tens of nuclear spins in atomically thin hexagonal boron nitride. Science , this issue p. 503

Understanding the coordination of cell division timing is one of the outstanding questions in the field of developmental biology. One active control parameter of the cell cycle duration is temperature, as it can accelerate or decelerate the rate of biochemical reactions. However, controlled experiments at the cellular-scale are challenging due to the limited availability of biocompatible temperature sensors as well as the lack of practical methods to systematically control local temperatures and cellular dynamics. Here, we demonstrate a method to probe and control the cell division timing in Caenorhabditis elegans embryos using a combination of local laser heating and nanoscale thermometry. Local infrared laser illumination produces a temperature gradient across the embryo, which is precisely measured by in-vivo nanoscale thermometry using quantum defects in nanodiamonds. These techniques enable selective, controlled acceleration of the cell divisions, even enabling an inversion of division order at the two cell stage. Our data suggest that the cell cycle timing asynchrony of the early embryonic development in C. elegans is determined independently by individual cells rather than via cell-to-cell communication. Our method can be used to control the development of multicellular organisms and to provide insights into the regulation of cell division timings as a consequence of local perturbations., 6+6 pages, 4+9 figures

Quantum metrology is a powerful tool for explorations of fundamental physical phenomena and applications in material science and biochemical analysis. While in principle the sensitivity can be improved by increasing the density of sensing particles, in practice this improvement is severely hindered by interactions between them. Here, using a dense ensemble of interacting electronic spins in diamond, we demonstrate a novel approach to quantum metrology to surpass such limitations. It is based on a new method of robust quantum control, which allows us to simultaneously suppress the undesired effects associated with spin-spin interactions, disorder, and control imperfections, enabling a fivefold enhancement in coherence time compared to state-of-the-art control sequences. Combined with optimal spin state initialization and readout directions, this allows us to achieve an ac magnetic field sensitivity well beyond the previous limit imposed by interactions, opening a new regime of high-sensitivity solid-state ensemble magnetometers., publishedVersion

Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Transition metal dichalcogenides (TMDs), with their large spin-orbit coupling, have been of special interest for valleytronic applications for their coupling of circularly polarized light to excitons with selective valley and spin$^{1-4}$. In atomically thin MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructures, the unique atomic registry of vdW layers provides a quasi-angular momentum to interlayer excitons$^{5,6}$, enabling emission from otherwise dark spin triplet excitons. Here, we report electrically tunable spin singlet and triplet exciton emission from atomically aligned TMD heterostructures. We confirm the spin configurations of the light-emitting excitons employing magnetic fields to measure effective exciton g-factors. The interlayer tunneling current across the TMD vdW heterostructure enables the electrical generation of singlet and triplet exciton emission in this atomically thin PN junction. We demonstrate electrically tunability between the singlet and triplet excitons that are generated by charge injection. Atomically thin TMD heterostructure light emitting diodes thus enables a route for optoelectronic devices that can configure spin and valley quantum states independently by controlling the atomic stacking registry., Comment: Extended work of previous study: arXiv:1912.07678

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe_{2}/WSe_{2} bilayers exhibit a high (60%) degree of circular polarization (DOCP) and long valley lifetimes (40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than 3 orders of magnitude via electrostatic doping, enabling switching of the DOCP from ∼80% in the n-doped regime to5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom.

Van der Waals heterostructures obtained via stacking and twisting have been used to create moiré superlattices

The nitrogen vacancy (NV) center in diamond exhibits spin-dependent fluorescence and long spin coherence times under ambient conditions, enabling applications in quantum information processing and sensing. NV centers near the surface can have strong interactions with external materials and spins, enabling new forms of nanoscale spectroscopy. However, NV spin coherence degrades within 100 nanometers of the surface, suggesting that diamond surfaces are plagued with ubiquitous defects. Prior work on characterizing near-surface noise has primarily relied on using NV centers themselves as probes; while this has the advantage of exquisite sensitivity, it provides only indirect information about the origin of the noise. Here we demonstrate that surface spectroscopy methods and single spin measurements can be used as complementary diagnostics to understand sources of noise. We find that surface morphology is crucial for realizing reproducible chemical termination, and use these insights to achieve a highly ordered, oxygen-terminated surface with suppressed noise. We observe NV centers within 10 nm of the surface with coherence times extended by an order of magnitude.

Atomically thin van der Waals semiconductor films were synthesized in a three-dimensional membrane form with monolayer precision., We report wafer-scale growth of atomically thin, three-dimensional (3D) van der Waals (vdW) semiconductor membranes. By controlling the growth kinetics in the near-equilibrium limit during metal-organic chemical vapor depositions of MoS2 and WS2 monolayer (ML) crystals, we have achieved conformal ML coverage on diverse 3D texture substrates, such as periodic arrays of nanoscale needles and trenches on quartz and SiO2/Si substrates. The ML semiconductor properties, such as channel resistivity and photoluminescence, are verified to be seamlessly uniform over the 3D textures and are scalable to wafer scale. In addition, we demonstrated that these 3D films can be easily delaminated from the growth substrates to form suspended 3D semiconductor membranes. Our work suggests that vdW ML semiconductor films can be useful platforms for patchable membrane electronics with atomic precision, yet large areas, on arbitrary substrates.

We realize a new electroplasmonic switch based upon electrically tunable exciton-plasmon interactions. The device consists of a hexagonal boron nitride (hBN)-encapsulated tungsten diselenide (WSe

Nanodiamond-gold nanoparticle (ND-AuNP) dimers constitute a potent tool for controlled thermal heating of biological systems on the nanoscale, by combining a local light-induced heat source with a sensitive local thermometer. Unfortunately, previous solution-based strategies to build ND-AuNP conjugates resulted in large nanoclusters or a broad population of multimers with limited separation efficiency. Here, we describe a new strategy to synthesize discrete ND-AuNP dimers via the synthesis of biotin-labeled DNA-AuNPs through thiol chemistry and its immobilization onto the magnetic bead (MB) surface, followed by reacting with streptavidin-labeled NDs. The dimers can be easily released from MB via a strand displacement reaction and separated magnetically. Our method is facile, convenient, and scalable, ensuring high-throughput formation of very stable dimer structures. This ligand-induced self-assembly approach enables the preparation of a wide variety of dimers of designated sizes and compositions, thus opening up the possibility that they can be deployed in many biological actuation and sensing applications.

Sensing single proteins with diamonds Nuclear magnetic resonance is a powerful technique for medical imaging and the structural analysis of materials, but is usually associated with large-volume samples. Lovchinsky et al. exploited the magnetic properties of a single spin associated with a defect in diamond and manipulated it with a quantum-logic protocol. They demonstrated the magnetic resonance detection and spectroscopy of multiple nuclear species within individual ubiquitin proteins attached to a specially treated diamond surface at room temperature. Science , this issue p. 836

We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photonic density of states in a controllable and reversible fashion, we show that both the absorption and emission properties of the excitons can be dynamically modulated. This electromechanical control over exciton dynamics in a mechanically flexible, atomically thin semiconductor opens up new avenues in cavity quantum optomechanics, nonlinear quantum optics, and topological photonics., accepted version

The ability to communicate quantum information over long distances is of central importance in quantum science and engineering. For example, it enables secure quantum key distribution (QKD) relying on fundamental principles that prohibit the "cloning" of unknown quantum states. While QKD is being successfully deployed, its range is currently limited by photon losses and cannot be extended using straightforward measure-and-repeat strategies without compromising its unconditional security. Alternatively, quantum repeaters, which utilize intermediate quantum memory nodes and error correction techniques, can extend the range of quantum channels. However, their implementation remains an outstanding challenge, requiring a combination of efficient and high-fidelity quantum memories, gate operations, and measurements. Here we report the experimental realization of memory-enhanced quantum communication. We use a single solid-state spin memory integrated in a nanophotonic diamond resonator to implement asynchronous Bell-state measurements. This enables a four-fold increase in the secret key rate of measurement device independent (MDI)-QKD over the loss-equivalent direct-transmission method while operating megahertz clock rates. Our results represent a significant step towards practical quantum repeaters and large-scale quantum networks., Comment: 6 pages and 4 figures. Supplementary material, 9 pages and 5 figures, is available at the end of the manuscript