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Semiconductor nanostructures or thin films are vital components of modern optoelectronic devices, such as light-emitting diodes, sensors, or transistors. While single crystalline wafers are used as heteroepitaxial templates for them, increasing demands on flexibility or transferability require separation of the grown semiconductor structures on such substrates, which is technically challenging and expensive. Recent research suggests that large-scale 2D nanomaterials can serve as heteroepitaxial templates and provide additional functionalities such as transferability to foreign substrates or mechanical flexibility. In this paper, growth, structural properties, and optoelectronic device applications of semiconductor nanostructures or thin films which are heteroepitaxially grown on large-scale 2D nanomaterials are reviewed.

The Utah array powers cutting-edge projects for restoration of neurological function, such as BrainGate, but the underlying electrode technology has itself advanced little in the last three decades. Here, advanced dual-side lithographic microfabrication processes is exploited to demonstrate a 1024-channel penetrating silicon microneedle array (SiMNA) that is scalable in its recording capabilities and cortical coverage and is suitable for clinical translation. The SiMNA is the first penetrating microneedle array with a flexible backing that affords compliancy to brain movements. In addition, the SiMNA is optically transparent permitting simultaneous optical and electrophysiological interrogation of neuronal activity. The SiMNA is used to demonstrate reliable recordings of spontaneous and evoked field potentials and of single unit activity in chronically implanted mice for up to 196 days in response to optogenetic and to whisker air-puff stimuli. Significantly, the 1024-channel SiMNA establishes detailed spatiotemporal mapping of broadband brain activity in rats. This novel scalable and biocompatible SiMNA with its multimodal capability and sensitivity to broadband brain activity will accelerate the progress in fundamental neurophysiological investigations and establishes a new milestone for penetrating and large area coverage microelectrode arrays for brain–machine interfaces.

Prior studies have shown that neuronal spikes can be recorded with microelectrode arrays placed on the cortical surface. However, the etiology of these spikes remains unclear. Because the top cortical layer (layer 1) contains very few neuronal cell bodies, it has been proposed that these spikes originate from neurons with cell bodies in layer 2. To address this question, we combined two-photon calcium imaging with electrophysiological recordings from the cortical surface in awake mice using chronically implanted PEDOT:PSS electrode arrays on transparent parylene C substrate.Our electrode arrays (termed Windansee) were integrated with cortical windows offering see-through optical access while also providing measurements of local field potentials (LFP) and multiunit activity (MUA) from the cortical surface. To enable longitudinal data acquisition, we have developed a mechanical solution for installation, connectorization, and protection of Windansee devices aiming for an unhindered access for high numerical aperture microscope objectives and a lifetime of several months while worn by a mouse.Contrary to the common notion, our measurements revealed that only a small fraction of layer 2 neurons from the sampled pool (~13%) faithfully followed MUA recorded from the surface above the imaging field-of-view. Surprised by this result, we turned to computational modeling for an alternative explanation of the MUA signal. Using realistic modeling of neurons with back-propagating dendritic properties, we computed the extracellular action potential at the cortical surface due to firing of local cortical neurons and compared the result to that due to axonal inputs to layer 1. Assuming the literature values for the cell/axon density and firing rates, our modeling results show that surface MUA due to axonal inputs is over an order of magnitude larger than that due to firing of layer 2 pyramidal neurons.Thus, a combination of surface MUA recordings with two-photon calcium imaging can provide complementary information about the input to a cortical column and the local circuit response. Cortical layer I plays an important role in integration of a broad range of cortico-cortical, thalamocortical and neuromodulatory inputs. Therefore, detecting their activity as MUA while combining electrode recording with two-photon imaging using optically transparent surface electrode arrays would facilitate studies of the input/output relationship in cortical circuits, inform computational circuit models, and improve the accuracy of the next generation brain-machine interfaces.

We report the fabrication and characterization of indium gallium zinc oxide (IGZO) tunneling thin-film transistors. Both the IGZO channel and an Al2O3 tunneling barrier layer were deposited using the radio-frequency magnetron sputtering method. Compared with a conventional device, our device exhibited rapid saturation at a much smaller drain bias. Interestingly, we observed two different current saturation mechanisms within a single device, which can be explained as competition between the depletion envelope near the source electrode and channel depletion near the drain electrode. This work represents an industry-friendly method for implementing the tunnel-contact approach in the display industry.

Electrophysiological devices are critical for mapping eloquent and diseased brain regions and for therapeutic neuromodulation in clinical settings and are extensively used for research in brain-machine interfaces. However, the existing clinical and experimental devices are often limited in either spatial resolution or cortical coverage. Here, we developed scalable manufacturing processes with a dense electrical connection scheme to achieve reconfigurable thin-film, multithousand-channel neurophysiological recording grids using platinum nanorods (PtNRGrids). With PtNRGrids, we have achieved a multithousand-channel array of small (30 μm) contacts with low impedance, providing high spatial and temporal resolution over a large cortical area. We demonstrated that PtNRGrids can resolve submillimeter functional organization of the barrel cortex in anesthetized rats that captured the tissue structure. In the clinical setting, PtNRGrids resolved fine, complex temporal dynamics from the cortical surface in an awake human patient performing grasping tasks. In addition, the PtNRGrids identified the spatial spread and dynamics of epileptic discharges in a patient undergoing epilepsy surgery at 1-mm spatial resolution, including activity induced by direct electrical stimulation. Collectively, these findings demonstrated the power of the PtNRGrids to transform clinical mapping and research with brain-machine interfaces.

The enhanced electrochemical activity of nanostructured materials is readily exploited in energy devices, but their utility in scalable and human-compatible implantable neural interfaces can significantly advance the performance of clinical and research electrodes. We utilize low-temperature selective dealloying to develop scalable and biocompatible one-dimensional platinum nanorod (PtNR) arrays that exhibit superb electrochemical properties at various length scales, stability, and biocompatibility for high performance neurotechnologies. PtNR arrays record brain activity with cellular resolution from the cortical surfaces in birds and nonhuman primates. Significantly, strong modulation of surface recorded single unit activity by auditory stimuli is demonstrated in European Starling birds as well as the modulation of local field potentials in the visual cortex by light stimuli in a nonhuman primate and responses to electrical stimulation in mice. PtNRs record behaviorally and physiologically relevant neuronal dynamics from the surface of the brain with high spatiotemporal resolution, which paves the way for less invasive brain−machine interfaces.

We report on the selective-area growth of GaN microstructures on tungsten (W)-metal electrodes using a micro-patterned graphene intermediate layer between GaN and W, and demonstrate their use as light-emitting diodes (LEDs). Prior to the GaN growths, the cm-scale graphene layer was transferred on W and then further patterned into a regular array of few-μm-sized graphene microdots using conventional lithography. The graphene microdots served as a seed layer for selectively growing crack-free GaN microstructures with regular diameter and spacing. Each microstructure displayed a microdisk morphology, exhibiting a single crystalline phase from epitaxial lateral overgrowth (ELOG). We observed ohmic behavior between the as-grown GaN microdisks and underlying W film, facilitating the fabrication of LED microarrays. Using the underlying W layer as an ohmic contact, we fabricated p-n junction GaN microdisk LEDs, consisting of three periods of InxGa1–xN/GaN multiple quantum wells. Uniform electroluminescence was observed across the microdisks. These results open up novel strategies for streamlined fabrication of high-performance and high-resolution LEDs.

A facile and novel technique for the fabrication of pressure sensors is reported based on the hybridization of one-dimensional nanomaterials and two-dimensional graphene film. In particular, piezoelectric pressure sensors are fabricated by using vertically aligned and position- and dimension-controlled ZnO nanotube arrays grown on graphene layers. Graphene layers act not only as substrates for catalyst-free growth of high-quality ZnO nanotubes but also as flexible conduction channels connecting ZnO nanotubes and metal electrodes. Freestanding and flexible sensors have been efficiently obtained via mechanical lift-off of hybrid ZnO nanotube/graphene film structures and by exploiting the weak van der Waals forces existing between the graphene film and the original substrates. A prototype of such devices shows a high pressure sensitivity (−4.4 kPa−1), which would enable the detection of weak flows of inert gas. The relatively low wall thickness and large length of the ZnO nanotubes suggest a relatively high sensitivity to external pressures. The obtained nanotube sensors are attached to the philtrum and wrist of a volunteer and used to monitor his breath and heart rate. Overall, the prototype hybrid sensing device has great potential as wearable technology, especially in the sector of advanced healthcare devices. A novel technique is demonstrated for the fabrication of flexible and highly sensitive 1D piezoelectric pressure sensors containing ZnO nanotube arrays grown on 2D graphene layers. Due to the morphology-controlled tunable sensitivity, ultra-small size, and capability of detecting extremely low pressures, the sensors are able to efficiently detect human breath and pulse.

We report flexible and monolithically integrated multicolor light-emitting diode (LED) arrays using morphology-controlled growth of GaN microstructures on chemical-vapor-deposited (CVD) graphene films. As the morphology-controlled growth template of GaN microstructures, we used position-controlled ZnO nanostructure arrays with different spacings grown on graphene substrates. In particular, we investigated the effect of the growth parameters, including micropattern spacings and growth time and temperature, on the morphology of the GaN microstructures when they were coated on ZnO nanostructures on graphene substrates. By optimizing the growth parameters, both GaN microrods and micropyramids formed simultaneously on the graphene substrates. Subsequent depositions of InGaN/GaN quantum well and p-GaN layers and n- and p-type metallization yielded monolithic integration of microstructural LED arrays on the same substrate, which enabled multicolor emission depending on the shape of the microstructures. Furthermore, the CVD graphene substrates beneath the microstructure LEDs facilitated transfer of the LED arrays onto any foreign substrate. In this study, Cu foil was used for flexible LEDs. The flexible devices exhibited stable electroluminescence, even under severe bending conditions. Cyclic bending tests demonstrated the excellent mechanical stability and reliability of the devices.

Despite ongoing advances in our understanding of local single-cellular and network-level activity of neuronal populations in the human brain, extraordinarily little is known about their “intermediate” microscale local circuit dynamics. Here, we utilized ultra-high-density microelectrode arrays and a rare opportunity to perform intracranial recordings across multiple cortical areas in human participants to discover three distinct classes of cortical activity that are not locked to ongoing natural brain rhythmic activity. The first included fast waveforms similar to extracellular single-unit activity. The other two types were discrete events with slower waveform dynamics and were found preferentially in upper cortical layers. These second and third types were also observed in rodents, nonhuman primates, and semi-chronic recordings from humans via laminar and Utah array microelectrodes. The rates of all three events were selectively modulated by auditory and electrical stimuli, pharmacological manipulation, and cold saline application and had small causal co-occurrences. These results suggest that the proper combination of high-resolution microelectrodes and analytic techniques can capture neuronal dynamics that lay between somatic action potentials and aggregate population activity. Understanding intermediate microscale dynamics in relation to single-cell and network dynamics may reveal important details about activity in the full cortical circuit.

We report the fabrication and characterization of indium gallium zinc oxide (IGZO)-based synaptic thin-film transistors. Radio-frequency magnetron-sputtered AlO x thin films are embedded in the IGZO channel as charge-trapping layers to provide synaptic behavior. The voltage pulse introduced at the gate electrodes traps or de-traps charges in the embedded AlO x layer thus modulates the channel current, which in turn leads to the ability to mimic biological synaptic behaviors such as excitonic postsynaptic current, paired-pulse facilitation, and potentiation and depression. Simulation results suggest that the device can perform properly as a synaptic unit in an artificial neural network.

We report the experimental realization of piezoelectric ZnO dual-gate thin film transistors (TFTs) as highly sensitive force sensors and discuss the physical origins of its electrically tunable piezoelectric response using a simple analytical model. A dual gate TFT is fabricated on a polyimide substrate using radio-frequency (RF) magnetron sputtering of piezoelectric ZnO thin film as a channel. The ZnO TFTs exhibited a field effect mobility of ~ 5 cm(2)/Vs, I(max) to I(min) ratio of 10(7), and a subthreshold slope of 700 mV/dec. Notably, the TFT exhibited static and transient current changes under external force stimuli, with varying amplitude and polarity for different gate bias regimes. To understand the current modulation of the dual-gate TFT with independently biased top and bottom gates, an analytical model is developed. The model includes accumulation channels at both surfaces and a bulk channel within the film and accounts for the force-induced piezoelectric charge density. The microscopic piezoelectric response that modulates the energy-band edges and correspondent current-voltage characteristics are accurately portrayed by our model. Finally, the field-tunable force response in single TFT is demonstrated as a function of independent bias for the top and bottom gates with a force response range from −0.29 nA/mN to 22.7 nA/mN. This work utilizes intuitive analytical models to shed light on the correlation between the material properties with the force response in piezoelectric TFTs.

We report on the fabrication of individually addressable, high-density vertical zinc oxide (ZnO) nanotube Schottky diode arrays. The individually addressable nanotube Schottky diode arrays were fabricated by arranging the top and bottom electrodes in a crossbar configuration on a free-standing layer consisting of position-controlled ZnO nanotubes on graphene films. The electrical characteristics of each Schottky diode in the arrays were investigated by measuring current–voltage characteristics. We also investigated the variation in device characteristics within an array by spatially mapping the barrier height of individual devices. Additionally, we further confirmed the excellent flexibility and electrical robustness of the free-standing and thin Schottky diode arrays under extreme bending conditions and over multiple cycles. Moreover, the photoresponses of the nanotube Schottky diode arrays were investigated by measuring their spectral responses and current–voltage characteristics under light illuminations, yielding a maximum photocurrent to dark current ratio of 1400 and responsivity of 106 A/W. We believe that this work provides a general and rational route for developing many other two-terminal one-dimensional nanostructure device arrays for ultra-high density electronic and optoelectronic devices.

We report UV emission from a ZnO nanorod (NR) highly enhanced by coupling of excitons to cavity-enhanced second harmonic generation (SHG). A Ag cavity concentrates the exciting field into the center of the NR, producing an enhanced second harmonic (SH) response through the nonlinearity of ZnO, that spatially overlaps with an ensemble of excitons. Strong coupling to the excitons at room temperature is achieved when the SH response is spectrally tuned to the exciton transition through the NR diameter, yielding total SHG enhancements of 2 orders of magnitude. Our approach highlights a unique and simple platform for enhancing coherent, nonlinear light–matter interactions in a size regime that is challenging for plasmonic architectures, yet important for optoelectronics.

In this paper, we describe a new method for the selective extraction and quantification of glutathione (GSH) using matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) and maleimide-presenting gold nanoparticles (Mal-AuNPs). Our strategy utilizes the Michael addition to selectively extract GSH, from chosen samples, onto the maleimide of Mal-AuNPs. After the extraction step, the GSH bound to the AuNPs was analyzed by MALDI-TOF MS in the presence of an internal standard which was prepared by reacting Mal-AuNPs with isotope-labeled GSH (GSH*). The GSH* has the same structure as GSH but a higher molecular weight, and therefore, enables absolute quantification of GSH by comparing the mass signal intensities of the GSH- and GSH*-conjugated alkanethiols. Our strategy was verified by analyzing GSHspiked fetal bovine serum and NIH 3T3 cells.

Zinc blende ZnSe longitudinal twinning nanowires and a sandwich structure with the wurtzite ZnSe inserting into the zinc blende ZnSe longitudinal twinning nanowires are fabricated via a simple thermal evaporation method. The high-resolution transmission electron microscope images of the two types of nanowires match well with simulated atomic models of them. The growth of them might be caused by the crystal plane slip during the phase transformation process between the wurtzite and the zinc blende ZnSe nanowire. The vibrating and luminescence properties of the as-grown longitudinal twinning nanowire are investigated by room-temperature Raman and low-temperature (10 K) photoluminescence spectroscopy, respectively. The electrical transport properties of the two types of longitudinal twinning ZnSe nanowires and the monocrystal ZnSe nanowires were compared using in situ measurement in transmission electron microscope.