William S. Whitney

Grains and grain boundaries in single-layer graphene atomic patchwork quilts

The properties of polycrystalline materials are often dominated by the size of their grains and by the atomic structure of their grain boundaries. These effects should be especially pronounced in two-dimensional materials, where even a line defect can divide and disrupt a crystal. These issues take on practical significance in graphene, which is a hexagonal, two-dimensional crystal of carbon atoms. Single-atom-thick graphene sheets can now be produced by chemical vapour deposition on scales of up to metres, making their polycrystallinity almost unavoidable. Theoretically, graphene grain boundaries are predicted to have distinct electronic, magnetic, chemical and mechanical properties that strongly depend on their atomic arrangement. Yet because of the five-order-of-magnitude size difference between grains and the atoms at grain boundaries, few experiments have fully explored the graphene grain structure. Here we use a combination of old and new transmission electron microscopy techniques to bridge these length scales. Using atomic-resolution imaging, we determine the location and identity of every atom at a grain boundary and find that different grains stitch together predominantly through pentagon–heptagon pairs. Rather than individually imaging the several billion atoms in each grain, we use diffraction-filtered imaging to rapidly map the location, orientation and shape of several hundred grains and boundaries, where only a handful have been previously reported. The resulting images reveal an unexpectedly small and intricate patchwork of grains connected by tilt boundaries. By correlating grain imaging with scanning probe and transport measurements, we show that these grain boundaries severely weaken the mechanical strength of graphene membranes but do not as drastically alter their electrical properties. These techniques open a new window for studies on the structure, properties and control of grains and grain boundaries in graphene and other two-dimensional materials.

Large-Scale Arrays of Single-Layer Graphene Resonators

We fabricated large arrays of suspended, single-layer graphene membrane resonators using chemical vapor deposition (CVD) growth followed by patterning and transfer. We measure the resonators using both optical and electrical actuation and detection techniques. We find that the resonators can be modeled as flat membranes under tension, and that clamping the membranes on all sides improves agreement with our model and reduces the variation in frequency between identical resonators. The resonance frequency is tunable with both electrostatic gate voltage and temperature, and quality factors improve dramatically with cooling, reaching values up to 9000 at 10 K. These measurements show that it is possible to produce large arrays of CVD-grown graphene resonators with reproducible properties and the same excellent electrical and mechanical properties previously reported for exfoliated graphene.

High, Size-Dependent Quality Factor in an Array of Graphene Mechanical Resonators

Graphenes unparalleled strength, stiffness, and low mass per unit area make it an ideal material for nanomechanical resonators, but its relatively low quality factor is an important drawback that has been difficult to overcome. Here, we use a simple procedure to fabricate circular mechanical resonators of various diameters from graphene grown by chemical vapor deposition. In addition to highly reproducible resonance frequencies and mode shapes, we observe a striking improvement of the membrane quality factor with increasing size. At room temperature, we observe quality factors as high as 2400 ± 300 for a resonator 22.5 μm in diameter, about an order of magnitude greater than previously observed quality factors for monolayer graphene. Measurements of quality factor as a function of modal frequency reveal little dependence of Q on frequency. These measurements shed light on the mechanisms behind dissipation in monolayer graphene resonators and demonstrate that the quality factor of graphene resonators relative to their thickness is among the highest of any mechanical resonator demonstrated to date.

Resonant absorption in semiconductor nanowires and nanowire arrays: Relating leaky waveguide modes to Bloch photonic crystal modes

We present a unified framework for resonant absorption in periodic arrays of high index semiconductor nanowires that combines a leaky waveguide theory perspective and that of photonic crystals supporting Bloch modes, as array density transitions from sparse to dense. Full dispersion relations are calculated for each mode at varying illumination angles using the eigenvalue equation for leaky waveguide modes of an infinite dielectric cylinder. The dispersion relations along with symmetry arguments explain the selectivity of mode excitation and spectral red-shifting of absorption for illumination parallel to the nanowire axis in comparison to perpendicular illumination. Analysis of photonic crystal band dispersion for varying array density illustrates that the modes responsible for resonant nanowire absorption emerge from the leaky waveguide modes.

Field Effect Optoelectronic Modulation of Quantum-Confined Carriers in Black Phosphorus

We report measurements of the infrared optical response of thin black phosphorus under field-effect modulation. We interpret the observed spectral changes as a combination of an ambipolar Burstein-Moss (BM) shift of the absorption edge due to band-filling under gate control, and a quantum confined Franz-Keldysh (QCFK) effect, phenomena that have been proposed theoretically to occur for black phosphorus under an applied electric field. Distinct optical responses are observed depending on the flake thickness and starting carrier concentration. Transmission extinction modulation amplitudes of more than two percent are observed, suggesting the potential for use of black phosphorus as an active material in mid-infrared optoelectronic modulator applications.

Imaging Grains and Grain Boundaries in Single-Layer Graphene: An Atomic Patchwork Quilt

1. School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA 2. Department of Physics, Cornell University, Ithaca, NY 14853, USA 3. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 14853, USA 4. Department of Physics and Astronomy, Brigham Young University, Provo, UT 84602, USA 5. Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY14853, USA * These authors contributed equally to this work.

Gate-Variable Mid-Infrared Optical Transitions in a (Bi1–xSbx)2Te3 Topological Insulator

We report mid-infrared spectroscopy measurements of ultrathin, electrostatically gated (Bi1-xSbx)2Te3 topological insulator films in which we observe several percent modulation of transmittance and reflectance as gating shifts the Fermi level. Infrared transmittance measurements of gated films were enabled by use of an epitaxial lift-off method for large-area transfer of topological insulator films from infrared-absorbing SrTiO3 growth substrates to thermal oxidized silicon substrates. We combine these optical experiments with transport measurements and angle-resolved photoemission spectroscopy to identify the observed spectral modulation as a gate-driven transfer of spectral weight between both bulk and 2D topological surface channels and interband and intraband channels. We develop a model for the complex permittivity of gated (Bi1-xSbx)2Te3 and find a good match to our experimental data. These results open the path for layered topological insulator materials as a new candidate for tunable, ultrathin infrared optics and highlight the possibility of switching topological optoelectronic phenomena between bulk and spin-polarized surface regimes.

Materials challenges for the Starshot lightsail

The Starshot Breakthrough Initiative established in 2016 sets an audacious goal of sending a spacecraft beyond our Solar System to a neighbouring star within the next half-century. Its vision for an ultralight spacecraft that can be accelerated by laser radiation pressure from an Earth-based source to ~20% of the speed of light demands the use of materials with extreme properties. Here we examine stringent criteria for the lightsail design and discuss fundamental materials challenges. We predict that major research advances in photonic design and materials science will enable us to define the pathways needed to realize laser-driven lightsails.This Perspective explores the optical, mechanical and thermal properties required to successfully design an ultralight spacecraft that can reach Proxima Centauri b, which is the goal of the Starshot Breakthrough Initiative.

Achieving near-unity broadband absorption in sparse arrays of GaAs NWs via a fundamental understanding of localized radial modes

We report a fundamental understanding of the mechanism for enhanced light absorption in sparse semiconductor nanowire arrays and design methods to achieve near-unity broadband absorption, demonstrated by GaAs nanowire arrays on a Si substrate. The sparse nanowire arrays absorb strongly into localized radial modes of individual nanowires, enabled by efficient scattering of incident light from neighboring nanowires. The radius-dependent localized modes led to two basic design approaches towards achieving near unity broadband absorption: (i) including multiple wire radii within an array for a 21% increase in absorbed current, and (ii) tapering the nanowires for a 23% increase in absorbed current.

Publisher Correction: Materials challenges for the Starshot lightsail

In the version of this Perspective originally published, the titles of the references were missing; all versions have now been amended to include them.