Validating an algebraic approach to characterizing resonator networks.

Resonator networks are ubiquitous in natural and engineered systems, such as solid-state materials, electrical circuits, quantum processors, and even neural tissue. To understand and manipulate these networks it is essential to characterize their building blocks, which include the mechanical analogs of mass, elasticity, damping, and coupling of each resonator element. While these mechanical parameters are typically obtained from response spectra using least-squares fitting, this approach requires a priori knowledge of all parameters and is susceptible to large error due to convergence to local minima. Here we validate an alternative algebraic means to characterize resonator networks with no or minimal a priori knowledge. Our approach recasts the equations of motion of the network into a linear homogeneous algebraic equation and solves the equation with a set of discrete measured network response vectors. For validation, we employ our approach on noisy simulated data from a single resonator and a coupled resonator pair, and we characterize the accuracy of the recovered parameters using high-dimension factorial simulations. Generally, we find that the error is inversely proportional to the signal-to-noise ratio, that measurements at two frequencies are sufficient to recover all parameters, and that sampling near the resonant peaks is optimal. Our simple, powerful tool will enable future efforts to ascertain network properties and control resonator networks in diverse physical domains.

Coupled Nanomechanical Graphene Resonators: A Promising Platform for Scalable NEMS Networks.

Arrays of coupled nanoelectromechanical resonators are a promising foundation for implementing large-scale network applications, such as mechanical-based information processing and computing, but their practical realization remains an outstanding challenge. In this work, we demonstrate a scalable platform of suspended graphene resonators, such that neighboring resonators are persistently coupled mechanically. We provide evidence of strong coupling between neighboring resonators using two different tuning methods. Additionally, we provide evidence of inter-resonator coupling of higher-order modes, demonstrating the rich dynamics that can be accessed with this platform. Our results establish this platform as a viable option for realizing large-scale programmable networks, enabling applications such as phononic circuits, tunable waveguides, and reconfigurable metamaterials.

Comparison of fractal and grid electrodes for studying the effects of spatial confinement on dissociated retinal neuronal and glial behavior.

Understanding the impact of the geometry and material composition of electrodes on the survival and behavior of retinal cells is of importance for both fundamental cell studies and neuromodulation applications. We investigate how dissociated retinal cells from C57BL/6J mice interact with electrodes made of vertically-aligned carbon nanotubes grown on silicon dioxide substrates. We compare electrodes with different degrees of spatial confinement, specifically fractal and grid electrodes featuring connected and disconnected gaps between the electrodes, respectively. For both electrodes, we find that neuron processes predominantly accumulate on the electrode rather than the gap surfaces and that this behavior is strongest for the grid electrodes. However, the 'closed' character of the grid electrode gaps inhibits glia from covering the gap surfaces. This lack of glial coverage for the grids is expected to have long-term detrimental effects on neuronal survival and electrical activity. In contrast, the interconnected gaps within the fractal electrodes promote glial coverage. We describe the differing cell responses to the two electrodes and hypothesize that there is an optimal geometry that maximizes the positive response of both neurons and glia when interacting with electrodes.

Uncovering the morphological effects of high-energy Ga+ focused ion beam milling on hBN single-photon emitter fabrication.

Many techniques to fabricate complex nanostructures and quantum emitting defects in low dimensional materials for quantum information technologies rely on the patterning capabilities of focused ion beam (FIB) systems. In particular, the ability to pattern arrays of bright and stable room temperature single-photon emitters (SPEs) in 2D wide-bandgap insulator hexagonal boron nitride (hBN) via high-energy heavy-ion FIB allows for direct placement of SPEs without structured substrates or polymer-reliant lithography steps. However, the process parameters needed to create hBN SPEs with this technique are dependent on the growth method of the material chosen. Moreover, morphological damage induced by high-energy heavy-ion exposure may further influence the successful creation of SPEs. In this work, we perform atomic force microscopy to characterize the surface morphology of hBN regions patterned by Ga+ FIB to create SPEs at a range of ion doses and find that material swelling, and not milling as expected, is most strongly and positively correlated with the onset of non-zero SPE yields. Furthermore, we simulate vacancy concentration profiles at each of the tested doses and propose a qualitative model to elucidate how Ga+ FIB patterning creates isolated SPEs that is consistent with observed optical and morphological characteristics and is dependent on the consideration of void nucleation and growth from vacancy clusters. Our results provide novel insight into the formation of hBN SPEs created by high-energy heavy-ion milling that can be leveraged for monolithic hBN photonic devices and could be applied to a wide range of low-dimensional solid-state SPE hosts.

Controlled assembly of retinal cells on fractal and Euclidean electrodes.

Controlled assembly of retinal cells on artificial surfaces is important for fundamental cell research and medical applications. We investigate fractal electrodes with branches of vertically-aligned carbon nanotubes and silicon dioxide gaps between the branches that form repeating patterns spanning from micro- to milli-meters, along with single-scaled Euclidean electrodes. Fluorescence and electron microscopy show neurons adhere in large numbers to branches while glial cells cover the gaps. This ensures neurons will be close to the electrodes' stimulating electric fields in applications. Furthermore, glia won't hinder neuron-branch interactions but will be sufficiently close for neurons to benefit from the glia's life-supporting functions. This cell 'herding' is adjusted using the fractal electrode's dimension and number of repeating levels. We explain how this tuning facilitates substantial glial coverage in the gaps which fuels neural networks with small-world structural characteristics. The large branch-gap interface then allows these networks to connect to the neuron-rich branches.

The Roles of an Aluminum Underlayer in the Biocompatibility and Mechanical Integrity of Vertically Aligned Carbon Nanotubes for Interfacing with Retinal Neurons.

Retinal implant devices are becoming an increasingly realizable way to improve the vision of patients blinded by photoreceptor degeneration. As an electrode material that can improve restored visual acuity, carbon nanotubes (CNTs) excel due to their nanoscale topography, flexibility, surface chemistry, and double-layer capacitance. If vertically aligned carbon nanotubes (VACNTs) are biocompatible with retinal neurons and mechanically robust, they can further improve visual acuity-most notably in subretinal implants-because they can be patterned into high-aspect-ratio, micrometer-size electrodes. We investigated the role of an aluminum (Al) underlayer beneath an iron (Fe) catalyst layer used in the growth of VACNTs by chemical vapor deposition (CVD). In particular, we cultured dissociated retinal cells for three days in vitro (DIV) on unfunctionalized and oxygen plasma functionalized VACNTs grown from a Fe catalyst (Fe and Fe + Pl preparations, where Pl signifies the plasma functionalization) and an Fe catalyst with an Al underlayer (Al/Fe and Al/Fe + Pl preparations). The addition of the Al layer increased the mechanical integrity of the VACNT interface and enhanced retinal neurite outgrowth over the Fe preparation. Unexpectedly, the extent of neurite outgrowth was significantly greater in the Al/Fe than in the Al/Fe+Pl preparation, suggesting plasma functionalization can negatively impact biocompatibility for some VACNT preparations. Additionally, we show our VACNT growth process for the Al/Fe preparation can support neurite outgrowth for up to 7 DIV. By demonstrating the retinal neuron biocompatibility, mechanical integrity, and pattern control of our VACNTs, this work offers VACNT electrodes as a solution for improving the restored visual acuity provided by modern retinal implants.

Nonvolatile Rewritable Frequency Tuning of a Nanoelectromechanical Resonator Using Photoinduced Doping.

Arrays of nanoelectromechanical resonators (NEMS) have shown promise for a suite of applications, from nanomechanical information processing technologies to mass spectrometry. A fundamental challenge toward broader adoption of NEMS arrays is a lack of viable frequency tuning methods, which must simultaneously allow for persistent and reversible control of single resonators while also being scalable to large arrays of devices. In this work, we demonstrate an electro-optic tuning method for graphene-based NEMS where locally photoionized charge tensions a suspended membrane and tunes its resonance frequency. The tuned frequency state persists unchanged for several days in the absence of any external power, and the state can be repeatedly written and erased with a high degree of precision. We show the scalability of this technique by aligning the frequencies of several NEMS devices on the same chip, and we discuss implications of this tuning method for both single devices and programmable NEMS networks.

A fast and sensitive room-temperature graphene nanomechanical bolometer.

Bolometers are a powerful means of detecting light. Emerging applications demand that bolometers work at room temperature, while maintaining high speed and sensitivity, properties which are inherently limited by the heat capacity of the detector. To this end, graphene has generated interest, because it has the lowest mass per unit area of any material, while also possessing extreme thermal stability and an unmatched spectral absorbance. Yet, due to its weakly temperature-dependent electrical resistivity, graphene has failed to challenge the state-of-the-art at room temperature. Here, in a departure from conventional bolometry, we use a graphene nanoelectromechanical system to detect light via resonant sensing. In our approach, absorbed light heats and thermally tensions a suspended graphene resonator, thereby shifting its resonant frequency. Using the resonant frequency as a readout for photodetection, we achieve a room-temperature noise-equivalent power (2 pW Hz-1/2) and bandwidth (from 10 kHz up to 1.3 MHz), challenging the state-of-the-art.

Deterministic Quantum Emitter Formation in Hexagonal Boron Nitride via Controlled Edge Creation.

Quantum emitters (QEs) in 2D hexagonal boron nitride (hBN) are extremely bright and are stable at high temperature and under harsh chemical conditions. Because they reside within an atomically thin 2D material, these QEs have a unique potential to couple strongly to hybrid optoelectromechanical and quantum devices. However, this potential for coupling has been underexplored because of challenges in nanofabrication and patterning of hBN QEs. Motivated by recent studies showing that QEs in hBN tend to form at edges, we use a focused ion beam (FIB) to mill an array of patterned holes into hBN. Using optical confocal microscopy, we find arrays of bright, localized photoluminescence that match the geometry of the patterned holes. Furthermore, second-order photon correlation measurements on these bright spots reveal that they contain single and multiple QEs. By optimizing the FIB parameters, we create patterned single QEs with a yield of 31%, a value close to Poissonian limit. Using atomic force microscopy to study the morphology near emission sites, we find that single QE yield is highest with smoothly milled holes on unwrinkled hBN. This technique dramatically broadens the utility and convenience of hBN QEs and achieves a vital step toward the facile integration of the QEs into large-scale photonic, plasmonic, nanomechanical, or optoelectronic devices.

A Bottom-Up Approach to Solution-Processed, Atomically Precise Graphitic Cylinders on Graphite.

Extended carbon nanostructures, such as carbon nanotubes (CNTs), exhibit remarkable properties but are difficult to synthesize uniformly. Herein, we present a new class of carbon nanomaterials constructed via the bottom-up self-assembly of cylindrical, atomically precise small molecules. Guided by supramolecular design principles and circle packing theory, we have designed and synthesized a fluorinated nanohoop that, in the solid state, self-assembles into nanotube-like arrays with channel diameters of precisely 1.63 nm. A mild solution-casting technique is then used to construct vertical "forests" of these arrays on a highly ordered pyrolytic graphite (HOPG) surface through epitaxial growth. Furthermore, we show that a basic property of nanohoops, fluorescence, is readily transferred to the bulk phase, implying that the properties of these materials can be directly altered via precise functionalization of their nanohoop building blocks. The strategy presented is expected to have broader applications in the development of new graphitic nanomaterials with π-rich cavities reminiscent of CNTs.

Single-Photon Emitters in Boron Nitride Nanococoons.

Quantum emitters in two-dimensional hexagonal boron nitride (hBN) are attractive for a variety of quantum and photonic technologies because they combine ultra-bright, room-temperature single-photon emission with an atomically thin crystal. However, the emitter's prominence is hindered by large, strain-induced wavelength shifts. We report the discovery of a visible-wavelength, single-photon emitter (SPE) in a zero-dimensional boron nitride allotrope (the boron nitride nanococoon, BNNC) that retains the excellent optical characteristics of few-layer hBN while possessing an emission line variation that is lower by a factor of 5 than the hBN emitter. We determined the emission source to be the nanometer-size BNNC through the cross-correlation of optical confocal microscopy with high-resolution scanning and transmission electron microscopy. Altogether, this discovery enlivens color centers in BN materials and, because of the BN nanococoon's size, opens new and exciting opportunities in nanophotonics, quantum information, biological imaging, and nanoscale sensing.

Engineered micro- and nanoscale diamonds as mobile probes for high-resolution sensing in fluid.

The nitrogen-vacancy (NV) center in diamond is an attractive platform for quantum information and sensing applications because of its room temperature operation and optical addressability. A major research effort focuses on improving the quantum coherence of this defect in engineered micro- and nanoscale diamond particles (DPs), which could prove useful for high-resolution sensing in fluidic environments. In this work we fabricate cylindrical diamonds particles with finely tuned and highly reproducible sizes (diameter and height ranging from 100 to 700 and 500 nm to 2 µm, respectively) using high-purity, single-crystal diamond membranes with shallow-doped NV centers. We show that the spin coherence time of the NV centers in these particles exceeds 700 µs, opening the possibility for the creation of ultrahigh sensitivity micro- and nanoscale sensors. Moreover, these particles can be efficiently transferred into a water suspension and delivered to the region to probe. In particular, we introduce a DP suspension inside a microfluidic circuit and control position and orientation of the particles using an optical trapping apparatus. We demonstrate a DC magnetic sensitivity of 9 µT/√Hz in fluid as well as long-term trapping stability (>30 h), which paves the way toward the use of high-sensitivity pulse techniques on contactless probes manipulated within biological settings.

Electron spin resonance of nitrogen-vacancy centers in optically trapped nanodiamonds.

Using an optical tweezers apparatus, we demonstrate three-dimensional control of nanodiamonds in solution with simultaneous readout of ground-state electron-spin resonance (ESR) transitions in an ensemble of diamond nitrogen-vacancy color centers. Despite the motion and random orientation of nitrogen-vacancy centers suspended in the optical trap, we observe distinct peaks in the measured ESR spectra qualitatively similar to the same measurement in bulk. Accounting for the random dynamics, we model the ESR spectra observed in an externally applied magnetic field to enable dc magnetometry in solution. We estimate the dc magnetic field sensitivity based on variations in ESR line shapes to be approximately 50 µT/√Hz. This technique may provide a pathway for spin-based magnetic, electric, and thermal sensing in fluidic environments and biophysical systems inaccessible to existing scanning probe techniques.

Graphene veils and sandwiches.

We report a new and highly versatile approach to artificial layered materials synthesis which borrows concepts of molecular beam epitaxy, self-assembly, and graphite intercalation compounds. It readily yields stacks of graphene (or other two-dimensional sheets) separated by virtually any kind of "guest" species. The new material can be "sandwich like", for which the guest species are relatively closely spaced and form a near-continuous inner layer of the sandwich, or "veil like", where the guest species are widely separated, with each guest individually draped within a close-fitting, protective yet atomically thin graphene net or veil. The veils and sandwiches can be intermixed and used as a two-dimensional platform to control the movements and chemical interactions of guest species.

Transfer-free batch fabrication of large-area suspended graphene membranes.

We demonstrate a process for batch production of large-area (100-3000 microm(2)) patterned free-standing graphene membranes on Cu scaffolds using chemical vapor deposition (CVD)-grown graphene. This technique avoids the use of silicon and transfers of graphene. As one application of this technique, we fabricate transmission electron microscopy (TEM) sample supports. TEM characterization of the graphene membranes reveals relatively clean, highly TEM-transparent, single-layer graphene regions ( approximately 50% by area) and, despite the polycrystalline nature of CVD graphene, membrane yields as high as 75-100%. This high yield verifies that the intrinsic strength and integrity of CVD-grown graphene films is sufficient for sub-100 microm width membrane applications. Elemental analysis (electron energy loss spectroscopy (EELS) and X-ray energy-dispersive spectroscopy (EDS)) of the graphene membranes reveals some nanoscaled contamination left over from the etching process, and we suggest several ways to reduce this contamination and improve the quality of the graphene for electronic device applications. This large-scale production of suspended graphene membranes facilitates access to the two-dimensional physics of graphene that are suppressed by substrate interactions and enables the widespread use of graphene-based sample supports for electron and optical microscopy.

Sustained mechanical self-oscillations in carbon nanotubes.

The potential size and power benefits of resonant NEMS devices are frequently mitigated by the need for relatively large, high-frequency, high-power electronics. Here we demonstrate controllable, sustained self-oscillations in singly clamped carbon nanotubes operating with a single dc voltage supply, and we develop a model that predicts the required voltage on the basis of the material properties and device geometry. Using this model, we demonstrate for the first time top-down, self-oscillating NEMS devices suitable for large-scale integration.

Biomimetic nanowire coatings for next generation adhesive drug delivery systems.

Without bioadhesive delivery devices, complex compounds are typically degraded or cleared from mucosal tissues by the mucous layer.While some chemically modified, microstructured surfaces have been studied in aqueous environments,adhesion due to geometry alone has not been investigated. Silicon nanowire-coated beads show significantly better adhesion than those with targeting agents under shear, and can increase the lift-off force 100-fold. We have shown that nanowire coatings, paired with epithelial physiology, significantly increase adhesion in mucosal conditions.